PhDthesis YapingCai

Research Collection
Doctoral Thesis
Microplastics and the Textile Sector: Experimental Studies

Concerning the Release from Fabrics and Environmental Risk
Assessment in Laundry Care Products
Author(s):
Cai, Yaping
Publication Date:
2021
Permanent Link:
https://doi.org/10.3929/ethz-b-000499754
Rights / License:
In Copyright - Non-Commercial Use Permitted
This page was generated automatically upon download from the ETH Zurich Research Collection. For more
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ETH Library
Diss. ETH no. 27529
MICROPLASTICS AND THE TEXTILE SECTOR:

EXPERIMENTAL STUDIES CONCERNING THE RELEASE
FROM FABRICS AND ENVIRONMENTAL RISK
ASSESSMENT IN LAUNDRY CARE PRODUCTS
A dissertation submitted to attain the degree of
DOCTOR OF SCIENCES OF ETH ZURICH

(Dr. sc. ETH Zurich)
presented by
YAPING CAI
M.Sc., ETH Zurich
born on 27 September 1990
citizen of China
accepted on the recommendation of
Prof. Dr. Bernd Nowack, examiner
Prof. Dr. Denise M. Mitrano, co-examiner

Prof. Dr. Manfred Heuberger, co-examiner
Prof. Dr. Jing Wang, co-examiner
2021
2
TABLE OF CONTENTS
Abstract..................................................................................................................... 6
Zusammenfassung................................................................................................... 9
Acknowledgements................................................................................................ 12
1. Introduction ...................................................................................................... 14
1.1. Plastics in the environment ................................................................................ 14
1.2. Polymers in the textile sector ............................................................................. 15
1.3. Occurrence of and source microplastic fibers in the environment ...................... 15
1.4. Origin of microplastic fibers in textiles ................................................................ 16
1.5. Release of microplastic fibers from synthetic textiles during washing and wearing
17
1.6. Microplastics in laundry care products ............................................................... 21
1.7. Environmental risk assessment ......................................................................... 21
1.8. Motivation .......................................................................................................... 23
1.9. Objectives ......................................................................................................... 24
1.10. Publications included in this thesis .................................................................... 25
1.11. References ....................................................................................................... 26
2. The Origin of Microplastic Fiber in Polyester Textiles: the Textile Production
Process Matters ..................................................................................................... 34
2.1. Abstract ............................................................................................................. 34
2.2. Introduction ....................................................................................................... 35
2.3. Materials and methods ...................................................................................... 37
2.3.1. Sliver, yarns and textiles ......................................................................... 37
2.3.2. Sample preparation ................................................................................ 39
2.3.3. Extraction experiments and filtration processes ...................................... 40
2.3.4. Filter imaging and analysis...................................................................... 41
2.3.5. Influence of edge processing methods on MPF extraction ...................... 41
2.3.6. Statistics ................................................................................................. 42
2.4. Results .............................................................................................................. 42
2.4.1. Assessment of experimental procedures ................................................ 42
2.4.2. Extraction dynamics of MPFs.................................................................. 43
2.4.3. Cumulative number of MPFs extracted from sliver, yarns and textiles ..... 45
2.4.4. Length distribution of extracted MPFs ..................................................... 47
3
2.4.5. Investigating the edge effect ................................................................... 51
2.5. Discussion ......................................................................................................... 52
2.5.1. Ultrasound as a method to extract embedded MPFs .............................. 52
2.5.2. The origin of MPFs in textile products ..................................................... 53
2.5.3. Comparison with previous studies on the MPF release from textiles ....... 57
2.5.4. Implications for the textile industry .......................................................... 58
2.6. Conclusions ....................................................................................................... 58
2.7. Acknowledgements ........................................................................................... 59
2.8. References ........................................................................................................ 60
3. A Systematic Study of Microplastic Fiber Release from 12 Different Polyester
Textiles during Washing ........................................................................................ 64
3.1. Abstract ............................................................................................................. 64
3.2. Introduction ....................................................................................................... 65
3.3. Materials and methods ...................................................................................... 66
3.3.1. Textiles ................................................................................................... 66
3.3.3. Washing experiments ............................................................................. 68
3.3.4. Water collection and filtration .................................................................. 69
3.3.5. Filter imaging and analysis...................................................................... 70
3.3.6. Statistics ................................................................................................. 70
3.4. Results .............................................................................................................. 71
3.4.1. MPF release from 12 polyester textiles ................................................... 71
3.4.2. MPF release during repeated wash cycles.............................................. 72
3.4.3. MPF release with different mechanical stress and cutting/sewing methods
75
3.5. Discussion ......................................................................................................... 77
3.6. Acknowledgements ........................................................................................... 80
3.7. References ........................................................................................................ 81
4. Formation of Fiber Fragments during Abrasion of Polyester Textiles ........ 85
4.1. Abstract ............................................................................................................. 85
4.2. Introduction ....................................................................................................... 86
4.3. Material and method .......................................................................................... 87
4.3.2. Abrasion experiments ............................................................................. 88
4.3.3. MPF and fibril extraction ......................................................................... 89
4
4.3.4. Image analysis ........................................................................................ 91
4.3.5. Statistics ................................................................................................. 92
4.4. Results .............................................................................................................. 92
4.4.1. Assessment of the methodology ............................................................. 92
4.4.2. Characterization of abraded textiles and fiber fragments ........................ 94
4.5. Discussion ......................................................................................................... 98
4.6. Acknowledgements ......................................................................................... 101
4.7. References ...................................................................................................... 102
5. Country-Specific Environmental Risks of Fragrance Encapsulates Used in
Laundry Care Products........................................................................................ 108
5.1. Abstract ........................................................................................................... 108
5.2. Introduction ..................................................................................................... 109
5.3. Methods ........................................................................................................... 111
5.3.1. Material flow model description .............................................................. 111
5.3.2. Input parameters................................................................................... 113
5.3.3. Hazard assessment .............................................................................. 115
5.4. Results ............................................................................................................ 118
5.4.1. Exposure assessment .......................................................................... 118
5.4.2. Hazard assessment ............................................................................. 124
5.4.3. Risk characterization ............................................................................ 125
5.5. Discussion ....................................................................................................... 126
5.6. Acknowledgements ......................................................................................... 129
5.7. References ...................................................................................................... 130
6. Conclusions and outlook .............................................................................. 136
6.1. Conclusions ..................................................................................................... 136
6.2. Outlook ............................................................................................................ 138
6.3. References ...................................................................................................... 140
Annex 1. Supporting Information for Chapter 2 ................................................ 141
Curriculum Vitae................................................................................................... 232
5
Abstract
The occurrence of microplastics is reported to be ubiquitous throughout the world. Among the
different types of microplastics found in environmental samples, microplastic fibers (MPF) are
often detected in high abundance and their composition is often consistent with the polymers
used in synthetic textiles. Therefore, a pathway of MPF release from synthetic textiles to the
environment likely exists. MPFs can be emitted into the environment during washing and
wearing of textiles. Although a number of studies have been carried out to investigate the
release of MPFs during the laundering process, the origin of the MPFs in the textile products
is unclear. Understanding the source of MPFs is important, since different origins will lead to
different mitigation strategies. Besides, a systematic study to investigate the influence of textile
properties on MPF release is still missing. Compared to the number of washing studies, much
less is known about the MPF release during wearing of textiles and the MPF formation as a
consequence of abrasion. In addition to synthetic textiles, the use of laundry care products
containing fragrance encapsulates (FEs) made of thermoset polymers is another pathway of
releasing microplastics from the textile sector and their environmental risk has not been
assessed yet. Therefore, the aim of this thesis was to contribute to a better understanding of
MPF formation and release from textile products and the environmental risk associated with
the use of FEs used in laundry care products.
To track the origin of MPFs from textile products, the presence of MPFs in 18 intermediate
and finished polyester textiles products along the textile production line was investigated. A
sonication extraction method was developed to extract the MPFs in the textile products. The
presence of MPFs has been confirmed in all textile samples, with a number of extracted MPFs
ranging from 15 MPF/g for a filament to 45’400 MPF/g for a scissor-cut microfiber textile. Some
yarn spinning process may be responsible for the MPF formation, as a rotor spinning yarn
exhibited much higher number (4’310 MPF/g) of extracted MPFs compared to the air-jet and
ring spinning yarns (160-230 MPFs/g). MPFs may be also formed during the surface treatment
step, since the textiles with processed surfaces and microfiber fabrics had five times more
extractable MPFs than those with unprocessed surfaces. Furthermore, 3 to 31 times higher
numbers of MPFs could be extracted from scissor-cut textiles than laser-cut textiles,
suggesting that the majority the extracted MPFs may originate from the cut edges. Most of the
extracted MPFs were found to be between 100 to 800 µm in length, which was in accordance
with the findings in previous washing studies.
6
Next a series of experiments was carried out to investigate the factors controlling the MPF
release from synthetic textiles during washing. A panel of 12 representative textiles were
tailored using five different cutting/sewing methods and washed up to 10 times with Gyrowash
lab washing machine. The MPF release ranged from 210 to 72’000 MPF/g textile per wash
with a median length between 165 µm and 841 µm. A decrease of the MPF release over
repeated wash cycles was found for all tested textiles, suggesting the washing process is likely
a process of depleting the production-inherited MPFs. Similar to the findings from the
ultrasonic extraction experiments, the textiles with processed surfaces demonstrated higher
release than the textiles with unprocessed surfaces. The adoption of laser-cutting method
resulted in a great reduction of MPF release compared to the other four commonly used
cutting/sewing methods.
In addition to the release during washing, MPFs can be released into the environment during
wearing of textiles. To simulate the abrasion of textiles after a period of use, fleece and
interlock textiles were abraded using a Martindale tester. The fiber fragments formed during
abrasion were extracted and characterized in terms of number, length and diameter. Fiber
fragments in two distinct morphologies were extracted from the abraded samples: MPFs with
a similar diameter to the textile fibers (fleece: 12.3 µm; interlock: 12.7 µm) and fibrils with much
smaller diameter (2 - 5 µm). MPFs also demonstrated a longer length profile (200 - 800 µm)
than fibrils (30 - 150 µm). Abrasion of textiles resulted in a strong increase of the extracted
amount of MPFs and fibrils, where 5 to 30 times more MPFs and approximately 200 times
more fibrils were extracted from abraded samples than from non-abraded ones.
Besides, the use of laundry care products containing microplastics such as fragrance
encapsulates (FEs) makes up another release pathway of microplastics from the textile sector.
Therefore, the work was conducted to assess the environmental risks associated with the
application of FEs in laundry care products. For the exposure assessment, a worst-case
predicted environmental concentration (PEC) was modelled for 34 countries using a
probabilistic material flow analysis (PMFA) model. The freshwater PEC was calculated for the
year 2019, and the concentrations for sediment and sludge-treated soil were predicted by
considering the accumulation between 2010 and 2019. For freshwater and sediment, Finland
(freshwater: 0.00011 µg/L; sediment: 3.0 µg/kg) and Belgium (freshwater: 0.13 µg/L;
sediment: 3400 µg/kg) had the lowest and the highest PECs, respectively. Two countries had
zero concentrations for sludge-treated soil (Malta and Switzerland), while the highest PEC
value was predicted for Vietnam (3600 µg/kg). In the hazard assessment, no toxicological
effects were observed for FE shells at the highest tested concentration, thus a predicted no
7
effect concentration (PNEC) could not be derived and a standard environmental risk
assessment could not be performed. The risk characterization was conducted by comparing
the Highest Observed-No-Effect Concentrations (HONECs) with the PEC values. The PEC
values for surface waters, sediments and soils were 107’000, 8 and 25 times lower than the
HONEC values, suggesting that based on current data there is no environmental risk of FE
shells.
In conclusion, the findings from this thesis confirmed the presence of production-inherited
MPFs in textile products and identified some manufacturing stages that may be responsible
for the MPF formation such as the yarn spinning process and surface treatment. These results
can provide a scientific basis for optimizing the production line. The majority of MPFs released
during washing is found to originate from cut edges, highlighting the importance of the
adoption of the cleaner cutting methods. Moreover, fibrils possessing much a smaller size than
MPFs were discovered in textile samples after abrasion, which raises the concern of human
exposure issues. Future research needs to be conducted to investigate the potential adverse
effect by these fibrils which fall into the inhalable size of airborne particles. Lastly, the thesis
provides a first assessment of the environmental risks of FEs shells used in laundry care
products. The accuracy of the assessment can be advanced in the future if more data such
as WWTP removal efficiency of FEs and actual PNEC values are available.
8
Zusammenfassung
Mikroplastik wird heute überall in der Umwelt gefunden. Unter den verschiedenen Arten von
Mikroplastik, die in Umweltproben gefunden werden, werden Mikroplastikfasern (MPF) oft in
großer Menge gefunden und ihre Zusammensetzung stimmt häufig mit den in synthetischen
Textilien verwendeten Polymeren überein. Daher ist es wahrscheinlich, dass MPF aus
synthetischen Textilien beim Waschen und Tragen in die Umwelt freigesetzt werden. Obwohl
eine Reihe von Studien durchgeführt wurde, um die Freisetzung von MPF während des
Waschvorgangs zu untersuchen, ist die Quelle der MPF - also bei welchen Prozessen sie
entstehen und an welchem Ort im Textil - unklar. Das Verständnis der Quellen der MPF ist
wichtig, da unterschiedliche Ursachen zu unterschiedlichen Minderungsstrategien führen
können. Ausserdem fehlt bisher eine systematische Studie, die den Einfluss der
Textileigenschaften auf die MPF-Freisetzung untersucht. Verglichen mit der Anzahl der
Waschstudien ist über die Freisetzung von MPF während des Tragens von Textilien und die
MPF-Bildung als Folge von Abrieb viel weniger bekannt. Nach unserem Kenntnisstand gibt es
keine Studie, welche die MPF-Bildung als Folge von Abrieb untersucht. Neben synthetischen
Textilien ist die Verwendung von Waschmitteln, welche Duftstoffkapseln aus duroplastischen
Polymeren enthalten, ein weiterer Freisetzungspfad für Mikroplastik aus dem Textilbereich,
der untersucht werden müsste. Das Ziel dieser Arbeit ist es daher, zu einem besseren
Verständnis der Bildung und Freisetzung von MPF aus Textilprodukten beizutragen und das
mit der Verwendung von Duftstoffkapseln in Wäschepflegeprodukten verbundene
Umweltrisiko zu bewerten.
Um die Herkunft von MPF in Textilprodukten zu verfolgen, wurde das Vorhandensein von
MPFs in 18 Zwischen- und Fertigprodukten aus Polyestertextilien entlang der Textilproduktion
untersucht. Es wurde eine Ultraschallextraktionsmethode entwickelt, um die MPF aus den
Textilprodukten zu extrahieren. Das Vorhandensein von MPF wurde in allen Textilprodukten
bestätigt, wobei die Anzahl der extrahierten MPF von 15 MPF/g Filament bis zu 45'400 MPF/g
in einem mit einer Schere geschnittenen Mikrofasertextil variierte. Die Art des
Garnspinnprozess kann die MPF-Bildung beeinflussen, da ein Rotorspinngarn eine viel
höhere Anzahl (4'310 MPF/g) an extrahierten MPF im Vergleich zu den Air-Jet- und
Ringspinngarnen (160-230 MPF/g) aufwies. MPF können auch während der
Oberflächenbehandlung gebildet werden, da die Textilien mit bearbeiteten Oberflächen und
Mikrofasergewebe fünfmal mehr extrahierbare MPF aufwiesen als solche mit unbearbeiteten
Oberflächen. Darüber hinaus konnten aus scherengeschnittenen Textilien 3- bis 31-mal mehr
MPF extrahiert werden als aus lasergeschnittenen Textilien, was darauf hindeutet, dass der
9
Großteil der extrahierten MPF von den Schnittkanten stammen könnte. Die meisten der
extrahierten MPF hatten eine Länge zwischen 100 und 800 µm, was mit den Ergebnissen
früherer Waschstudien übereinstimmte.
Als nächstes wurde eine Reihe von Experimenten durchgeführt, um die Faktoren zu
untersuchen, welche die MPF-Freisetzung aus synthetischen Textilien während des
Waschens beeinflussen. Eine Auswahl von 12 repräsentativen Textilien wurde mit fünf
verschiedenen Schnitt- und Nähmethoden konfektioniert und bis zu 10 Mal mit einer
Gyrowash-Laborwaschmaschine gewaschen. Die MPF-Freisetzung reichte von 210 bis
72'000 MPF/g Textil pro Waschgang. Die mittlere Faserlänge betrug zwischen 165 µm und
841 µm. Eine Abnahme der MPF-Freisetzung über wiederholte Waschzyklen wurde ebenfalls
für alle getesteten Textilien festgestellt, was darauf hindeutet, dass der Waschprozess
wahrscheinlich die produktionsbedingten MPF freisetzt. Ähnlich wie bei den Ergebnissen der
Ultraschallextraktionsversuche zeigten die Textilien mit bearbeiteten Oberflächen eine
anzahlmässig höhere Freisetzung von MPF als die Textilien mit unbearbeiteten Oberflächen.
Die Anwendung der Laserschneidmethode führte zu einer starken Reduzierung der MPF-
Freisetzung im Vergleich zu den anderen vier gängigen Schneid- und Nähmethoden.
Neben der Freisetzung beim Waschen können MPF auch beim Tragen von Textilien an die
Umgebung abgegeben werden. Um den Abrieb von Textilien nach einer gewissen Tragedauer
zu simulieren, wurden Vlies- und Interlock-Textilien mit einem Martin-Dale-Tester abgerieben.
Die beim Abrieb entstandenen Faserfragmente wurden extrahiert und hinsichtlich ihrer Anzahl,
ihrer Länge und ihrem Durchmesser charakterisiert. Aus den abgeriebenen Proben wurden
Faserfragmente mit zwei unterschiedlichen Morphologien extrahiert: MPF mit einem ähnlichen
Durchmesser wie die Textilfasern (Vlies: 12,3 µm; Interlock: 12,7 µm) und Fibrillen mit deutlich
kleinerem Durchmesser (2 - 5 µm). MPF zeigten auch ein längeres Längenprofil (200 - 800
µm) als die Fibrillen (30 - 150 µm). Der Abrieb von Textilien führte zu einem starken Anstieg
der extrahierten Menge an MPF und Fibrillen, wobei aus abgeriebenen Proben 5 bis 30 Mal
mehr MPF und etwa 200 Mal mehr Fibrillen extrahiert wurden als aus nicht abgeriebenen
Proben.
Daneben stellt die Verwendung von Textilpflegemitteln welche Mikroplastik wie z. B.

Duftstoffkapseln enthalten, einen weiteren Freisetzungspfad von Mikroplastik aus dem
Textilbereich dar. Daher wurden die Umweltrisiken der Anwendung von Duftstoffkapseln in
Textilpflegemitteln untersucht. Für die Expositionsabschätzung wurde mit Hilfe eines
probabilistischen Materialflussanalysemodells (PMFA) eine "Worst-Case"-Vorhersage der
10
Umweltkonzentration (PEC) für 34 Länder modelliert. Die Süsswasser-PECs wurde für das
Jahr 2019 berechnet, und die Konzentrationen für das Sediment und den mit Klärschlamm
behandelten Boden wurden, unter Berücksichtigung der Anreicherung der MPF zwischen
2010 und 2019 vorhergesagt. Für Süsswasser und Sediment hatten Finnland (Süsswasser:
0,00011 µg/L; Sediment: 3,0 µg/kg) und Belgien (Süsswasser: 0,13 µg/L; Sediment: 3400
µg/kg) die niedrigsten bzw. die höchsten PECs. Zwei Länder wiesen Nullkonzentrationen für
den mit Klärschlamm behandelten Boden auf (Malta und Schweiz), während der höchste PEC-
Wert für Vietnam (3600 µg/kg) vorhergesagt wurde. Bei der Gefährdungsbeurteilung wurden
für Duftstoffkapseln bei der höchsten getesteten Konzentration keine toxikologischen
Wirkungen beobachtet, so dass eine vorhergesagte Nicht-Effekt-Konzentration (PNEC) nicht
abgeleitet und eine Standard-Umweltrisikobewertung nicht durchgeführt werden konnte. Die
Risikocharakterisierung wurde durch den Vergleich der höchsten beobachteten Nicht-Effekt-
Konzentrationen (HONECs) mit den PEC-Werten durchgeführt. Die PEC-Werte für
Oberflächengewässer, Sedimente und Böden waren 107'000, 8 und 25 mal niedriger als die
HONEC-Werte, was darauf hindeutet, dass basierend auf den aktuellen Daten kein
Umweltrisiko durch die Anwendung von Duftstoffkapseln besteht.
Zusammenfassend lässt sich sagen, dass diese Arbeit das Vorhandensein von
produktionsbedingten MPF in Textilprodukten bestätigen und einige Herstellungsschritte
identifizieren konnte, welche für die MPF-Bildung verantwortlich sein können, wie z. B. der
Garnspinnprozess und die Oberflächenbehandlung. Die Ergebnisse dieser Arbeit können eine
wissenschaftliche Grundlage für die Optimierung der Produktionsprozesse liefern. Es wurde
festgestellt, dass der Grossteil der MPF, die beim Waschen freigesetzt werden, von den
Schnittkanten stammen, was die Bedeutung der Anwendung von saubereren
Schnittmethoden unterstreicht. Darüber hinaus wurden in Textilproben nach dem Abrieb
Fibrillen entdeckt, die eine viel geringere Größe als MPFs besitzen, was die Frage nach der
Exposition und deren Gefährdungspotential für die Menschen aufwirft. In Zukunft müssen die
möglicherweise schädliche Wirkung dieser Fibrillen untersucht werden, da diese Fibrillen in
die Grössenordnung von Feinstaub fallen und sind somit potentiell lungengängig sind,
Schliesslich liefert die Arbeit eine erste Bewertung der Umweltrisiken von Duftstoffkapseln,
die in Wäschepflegeprodukten verwendet werden. Die Genauigkeit der Bewertung kann in
Zukunft verbessert werden, wenn mehr Daten, wie z. B. die Menge der Elimination von
Duftstoffkapseln in Kläranlagen und PNEC-Werte basierend auf ökotoxikologischen Studien
verfügbar sind.
11
Acknowledgements
I would have never achieved this without the support of many people. Here I would like to
thank all of them who have contributed to this thesis.
First of all, I would like to express my deep gratitude to Bernd, who supervised my work and
guided me through my PhD with his knowledge, enthusiasm and patience. I am so grateful
that I was given the opportunity to work on this exciting project. He is an excellent researcher
and supervisor, whose door is always open for discussion and ideas. Whenever I run into
difficulties, he is always available to help. Without his guidance and support, the completion
of this thesis would have never been possible.
Furthermore, I would like to thank my co-supervisors, Denise, Manfred and Rudolf, for the
inspiration, discussion and feedback. Denise is always there for helping me with the
experiments, data analysis and the manuscript writing. Her critical inputs always make the
discussion productive. She is willing to share her knowledge on both science and life, and help
me with my language skills. Many thanks also go to Manfred, for the countless discussion
regarding the experimental design and the manuscript writing. As a physicist, his feedback is
always inspiring and highly appreciated. I would also like to express my gratitude to Rudolf,
who helped me with the textile samples and the experimental equipment as well as the
manuscript writing. He brings his tremendous knowledge of the textile sector to the project
and his comments are always highly valuable.
I would also like to thank Prof. Jing Wang for being the co-examiner for my defense. Thank
you for spending time in reviewing the thesis and giving me feedback. My thanks also go to
Prof. Heini Wernli for chairing the defense.
Moreover, I would like to thank the scientists from our industrial partner, Dr. Jianming Lin, Dr.
Sylvia Gimeno, and Dr. Frédéric Begnaud for the meetings, discussion and valuable inputs. I
feel really grateful to have the opportunity to work with you.
Many thanks also go to my warm, friendly and supportive colleagues from the whole lab. It is
a great pleasure to work with you and I really enjoyed my time at Empa. Especially I would
like to thank Claudia for the help and the support on both of my work and life. This year is quite
special. As a foreign student living abroad, you really make me feel at home. I would also like
to thank Tong, who joined in the project as a master thesis student and conducted an amazing
job. My thanks also go to Veronique for explaining the models, so I can start the work quickly.
12
Besides, I would also like thank Yan, for the encouragement during my PhD and the advice
regarding the career development.
Lastly, I would like to thank my friends and family for backing me up. Especially, I would like
to express my thanks to my parents. I am so lucky to grow up in a family with so much love.
You are always there for me. I would have never had the opportunity to study in Switzerland
without your encouragement and support.
13
1. Introduction
1.1. Plastics in the environment
The word "plastic" stems from the Greek word ''plastikos'', which means "capable of being
molded"1. Plastics are made from a wide range of polymers such as polyester, polyethylene,
and polycarbonate1. The first synthesis of plastics such as Bakelite can be traced back to the
beginning of 1900s2, but mass production was only initialized in the 1950s3. The beneficial
characteristics such as durability and lightweightness of this low-cost synthetic material results
in the use of plastics in almost every consumer product and has made plastics indispensable
in our daily lives4. The global production of plastics has experienced an enormous increase
during the last 60 years, from 1.7 million tonnes in 1950s to 368 million tonnes in 20195. Most
of the monomers used to produce plastics are derived from crude oil, and the majority of the
plastics is not biodegradable2. Therefore, the accumulation of plastics in the environment has
raised great concerns regarding their potential in altering ecosystems.
The research about the environmental pollution by larger pieces of plastics started as early as
19706, 7, but it was not until the beginning of the century when microplastics have drawn more
attention8. Microplastics are often defined as plastic debris with a size between 0.1 µm and 5
mm9. A pioneering study by Thompson, et al.10 reported the occurrence of microplastics in
marine sediment, highlighting the potential of accumulation of plastic fragments in the
environment. Since then, a number of studies have confirmed the presence of microplastics
in various environmental compartments throughout the world, from the water column11 to
sediments12, from the air13 to soils14, from populated coastlines15 to remote polar regions16.
The ubiquitous occurrence of microplastics in the environment emphasizes the need of

mitigating the microplastic emission at the source. Depending on the origin, microplastics are
usually split into primary and secondary microplastics17. Primary microplastics are defined as
those which are manufactured in that size, such as microbeads in consumer products 17.
Secondary microplastics are the result of the breakdown of larger items, such as fibers from
synthetic textiles and fragments from weathering processes of plastic products17. Since efforts
have been already made by regulators to reduce the release of microplastics as primary
particles, e.g. a ban on the use of microbeads in cosmetics18, the emission of microplastics
from secondary sources is becoming more predominant. As an important source of secondary
microplastics, microplastic fibers (MPFs) released from synthetic textiles are catching more
and more attention.
14
1.2. Polymers in the textile sector
The polymers used to produce textile fibers can be derived from several sources. Depending
on the way of production, the fibers in textile sectors are usually classified into natural and
chemical fibers19 (Table 1-1). Natural fibers are those that can be directly obtained from plants,
animals, and minerals, such as cotton, wool, and asbestos19. On the contrary, chemical fibers
refer to the fibers produced industrially, which can be further divided into three categories
depending on the origin of the polymers19. Cellulosic and glass fibers are the two
representatives of chemical fibers originating from natural and inorganic polymers
respectively19. The most important type of chemical fibers in textile industry is synthetic fibers,
which are made of synthetic polymers such as polyester, polyamide and polypropylene19. The
production of synthetic fibers was about 67 million tons in 2018, accounting for 62% of the
global fiber production (107 million tons)20. The synthetic fiber market is dominated by
polyester and the annual production of this material is 55 million tons alone, making up more
than 80% of the synthetic fiber production and more than half of the global fiber production20,
21
. The global fiber market has doubled in the last 20 years and is expected to grow by another
third in the next ten years20. Therefore, the emissions of microplastics from the textile sector
are also expected to increase if no further mitigations are adopted.
Table 1-1. Polymers in the textile sector19.
Type Source of polymers Examples
Natural fiber Plant, animal, and mineral Cotton, wool, and asbestos
Natural polymers Cellulosic fiber
Chemical fiber Inorganic polymers Glass fiber
Synthetic polymers Polyester, polyamide, polypropylene
1.3. Occurrence of and source microplastic fibers in the environment
MPFs are frequently detected as one of the dominant types of microplastics in wastewater
treatment plants (WWTPs) and in environmental samples22-32. A recent study reviewed 21
research papers analyzing the fate of microplastics in WWTPs, where MPFs were commonly
detected in high abundance in wastewater33. Although in average about 90% (35 – 99%) of
15
the microplastics are removed with the sludge33, 34, the uncaptured microplastics can still enter
the environment, resulting in elevated microplastic concentrations downstream of WWTPs 31,
35, 36
. Besides, the captured MPFs in sludge can re-enter into the environment due to the
common application of sewage sludge on agricultural soils37.
In addition to the occurrence of MPFs in WWTPs, the ubiquitous presence of MPFs in

environmental samples has been reported by many studies32, from the water column to
sediments38, 39, from atmospheric fallout to soils40, 41
. Since the composition of the MPFs
detected in the environment is often consistent with the polymers used in textile products42, 43,
it raises the suspicion that synthetic textiles are one of the important sources of MPFs in the
environment. A report estimated that about one third of the microplastics release into the
ocean can be attributed to synthetic textiles44. Clothing also ranked as the second largest
source of all microplastics to Swiss freshwaters in a recent modeling study45.
1.4. Origin of microplastic fibers in textiles
Since synthetic textiles may be one of the potential sources of MPFs in the environment and
the use of textile is suspected to release MPFs, a question is emerging: what is the origin of
those MPFs in textiles? Are they formed during manufacturing or generated during use or
washing? To track the origin of MPFs in textiles, we first need to gain an insight on how ready-
to-wear clothes are manufactured from raw materials. Crude oil provides the base for
synthesizing polymers. Then the polymer chips are melted and spun into endless filaments.
To make synthetic fibers similar to natural fibers, the endless filaments are often cut into short
staple fibers with a length of approximately 35 - 40 mm and then carded into slivers19. In the
next step, slivers are spun into yarns by different spinning methods (e.g. rotor spinning, air-jet
spinning, and ring spinning). Depending on the types of fibers spun into yarns, either "spun
yarns" (made of short staple fibers) or "filament yarns" (made of endless filaments) are
produced. Then these yarns can be further woven or knitted into fabrics. The difference
between the woven and knit textile is geometry (Figure 1-1). The woven textile has two
perpendicularly interlacing threads, while the knit textile has only one thread to produce
symmetric loops. The produced textiles can further go through finishing steps to enhance the
performance, look and feel. For example, fleece is produced by mechanically modifying the
surface fibers at this stage to obtain a fuzzy texture. Finally, the finished textiles are tailored
into garments and delivered to customers.
16
Figure 1-1. Examples of woven (A) and knit (B) textiles. The images were taken from Adanur46.
Since mechanical stress is required throughout the manufacturing of textiles, such as the
conversion of filaments into staple fibers, spinning fibers into yarns, weaving or knitting yarns
into fabrics and tailoring fabrics into garments, it is possible that the stress applied during the
production of textile products may results in the breakage of fibers and subsequently the
formation of MPFs. Therefore, a considerable amount of MPFs may be already present in
textile products prior to the delivery to customers.
1.5. Release of microplastic fibers from synthetic textiles during washing and wearing
Washing of textiles is commonly recognized as an important pathway of releasing MPFs from

synthetic textiles into the environment. Understanding the mechanism controlling the MPF
release during washing is a prerequisite to mitigate the emissions from this pathway. Bishop47
has reviewed the possible factors that might influence the laundering process of textiles. Firstly,
he has pointed out that the performance of textiles during laundering is strongly influenced by
the previous history of fabrics, especially during the first few washes. The manufacturing
process of textiles is important, since it determines the textile geometry as well as the stress
built into textile products. In terms of MPF release, tailoring of fabrics may also play an
important role, since the fibers sitting on the unfinished seam are more likely to migrate from
textiles into wash water during washing. Secondly, Bishop has suggested that the mechanical
stress during washing may induce changes in textiles. The relative movement between yarns,
the migration of fibers from yarns, and the abrasion of fabrics can potentially contribute to the
change of textile geometry, fiber shedding, and fiber breakage. Thirdly, the study also
17
mentions that the addition of washing products can physically modify the mechanical action
during the laundering process. This is because the application of surfactant can generate foam
and cause adsorption of surfactant onto the fiber, which mitigates the friction and further
reduce the fabric damage. Additionally, Bishop has pointed out that washing textiles at a
temperature higher than the glass transition temperature (Tg) may result in swelling at a higher
degree, which subsequently increases the abrasion. However, this may not apply for polyester.
Because polyester fabrics are commonly washed below the wet Tg of polyester (85 °C), the
swelling and hydrolysis of polyester fibers at normal washing temperature is almost
negligible47, 48.
Those factors hypothesized to control the release of MPFs during washing of synthetic textiles
have been continuously investigated by previous studies (Table 1-2). The influence by textile
geometry on MPF release was explored in the past49-51, but the conclusions from those studies
were inconsistent, and shedding of MPFs was observed to be either affected50 or not affected
by the textile structure49, 51. Another commonly investigated factor is the number of wash cycles.
The majority of studies reported a decrease of MPF release with increasing number of wash
cycles50, 52-59, sometimes with a plateau between the 4th and 5th wash55, 56. However, there are
also a few studies reporting a relative stable release over time49, 60. Moreover, the influence
by the addition of laundry care products was widely addressed as well49, 52, 54, 57, 58, 61, 62. The
results again varied between studies, where a number of studies reported the addition of
detergents resulted in an increased MPF release compared to pure water49, 54, 61, 62, while the
others observed no influence52, 57 or a decrease of MPF release60. Only one study investigated
the influence by textile softeners on MPF release and a reduction of the MPF release was
61
reported . Additionally, an increase of MPF release during washing was observed as a
consequence of the increase of water volume because of the higher hydrodynamic pressure
on fibers57. Other factors such as temperature, duration of washing, and mechanical stress
induced by steel balls were reported to have no significant impact on the MPF release49, 57, 61.
18
Table 1-2. An overview of the studies investigating the MPF release from synthetic textiles during washing.
Material Set-up
Author Temperature Wash Steel
Composition Sample Model Detergent
(°C) cycles balls
Front-load washing
Browne, et al.63 Polyester Blanket, shirt, fleece 1 -
machine 40 None
Top-load, front-load
Hartline, et al.64 Nylon, polyester Jacket
washing machine 29 - 41 1 - None
Front-load washing
Pirc, et al.52 Polyester Blanket None, liquid detergent, liquid
machine 30 10 -
detergent plus softener
Napper and Polyester, acrylic, Front-load washing

Jumper None, liquid detergent,
Thompson54 polyester/cotton machine 30, 40 5 -
conditioner
Sillanpaa and Front-load washing
Polyester, cotton Fleece, turquoise, shirt
Sainio53 machine 40 5 - Liquid detergent
Hernandez, et Interlock, jersey fabric swatch

Polyester Gyrowash 25, 40, 60, None, powder detergent, liquid
al.49 (scissor-cut, edge sewn) 5 10
80 detergent, surfactant
Knit, microfleece, fleece fabric
Polyester, nylon,
swatch (laser-cutter, edge Gyrowash
Almroth, et al.50 acrylic 60 10 25 None, liquid detergent
sewn)
Polyester, Plain and jersey fabric (edge
De Falco, et al.61 Linitest 40 None, liquid detergent
polypropylene sewn) 5 0,10,20
Tricot, fleece (scissor-cut,
Jonsson, et al.51 Polyester Gyrowash
ultrasonic-cut, edge sewn) 40 - 25 None
19
McIlwraith, et Top-load washing
Polyester Fleece blanket
al.65 machine 16 1 - None
polyester, polyester-
Front-load washing
Belzagui, et al.55 elastane, Shirt, pant, jacket, cap ambient
machine 5, 10 - Liquid detergent
polyamide-elastane temperature
Polyester, polyester Front-load washing
De Falco, et al.56
-cotton Shirt, blouse machine 40 10 - Liquid detergent
Tergotometer, front-
Kelly, et al.57 Polyester Shirt, knit fabric (laser-cut) load washing 15, 30 4 -
None, liquid detergent
machine
Polyester,
Zambrano, et Interlock fabric (cut, edge Top-load washing
polyester-cotton, 25, 44 None, liquid detergent
al.62 sewn) machine 3 25
cotton, rayon
cotton, acrylic,
Cesa, et al.58 polyester, Shirt, sweater Top-load washing
24 10 0 None, liquid detergent
polyamide machine
Dalla Fontana, et Knit fabric (edge sewn with a

Polyester Front-load washing
al.60 double heat-sealing) 30, 40 5 - Liquid detergent
machine
Polyester,
De Falco, et al.66 Blouse, shirt, dress, sweatshirt Front-load washing
polyester-cotton 40 1 - Liquid detergent
machine
polyester, polyester-
Karkkainen and
elastane, Shirt, jumper, softshell Front-load washing
Sillanpaa59 40 5 - Liquid detergent
polyamide, acryl machine
20
Compared to the number of washing studies, much less research has been carried out to
address the MPF release from synthetic textiles during wearing66, 67. A recent study by De
Falco, et al.66 quantified the MPFs released into air from the garments worn by volunteers.
The number of released MPFs ranged from 1 to 403 MPF per g textile depending on the types
of textiles. The MPF length was between 494 and 1034 µm66, which is in accordance of the
MPFs released from textiles in the previous washing studies49. Much smaller fluorescent
aerosol particles (FAP) with a mode size between 3 - 5 μm were emitted from volunteers
wearing different garments in a chamber study67. Because more FAPs were detected from
volunteers wearing long clothing (i.e. long-sleeve shirts and pants) than those wearing short
clothing (i.e. t-shirts and shorts)67, clothing might be a source of FAPs.
1.6. Microplastics in laundry care products
Despite of the release of MPFs from synthetic textiles, the application of laundry care products
during washing is another potential release pathway of microplastics into the environment from
the textile sector. That is because intentionally added microplastics are present in many
consumer products to achieve certain functions. Fragrance encapsulates (FEs) made of
thermoset polymers are one of the primary microplastics commonly used in laundry care
products, especially in liquid fabric softeners68, 69. The FEs are spheres filled with fragrance
oil, which have a diameter between 5 to 50 µm and a wall thickness below 1 µm68. As it known
that many fragrance components are volatile and prone to degradation70, 71
, FEs were
designed to prevent fragrance components from losses due to evaporation and degradation70,
71
and to deliver long-lasting fragrance experiences68. A considerable amount of FEs are
consumed every year and ECHA69 estimates an annual release of about 200 t (130 - 275 t)
FE shells in Europe. Since the major application of FEs is in laundry care products, they will
most likely enter into the environment with wash water after use and pass through WWTPs.
1.7. Environmental risk assessment
Exposure and hazard assessments are the two facets of environmental risk assessment,
where the traditional environmental risk assessment is conducted by comparing exposure
level and hazard effect72. The environmental exposure of substances is represented by
predicted environmental concentration (PEC), which can be either derived from field
measurements or predicted by exposure models73. However, the application of field
measurements in exposure assessment is often limited by the availability of data. In terms of
21
microplastics, although the environmental concentrations have been determined worldwide,
the measurements are often spatially inhomogeneous and the information for certain
environmental compartments (e.g. soil) is still scarce. Moreover, the source of microplastics
detected in the environmental monitoring studies cannot be determined with current analytical
techniques, so it is impossible to obtain the environmental concentration of FEs from current
data.
Therefore, modeling is a valuable alternative approach to estimate the exposure level of

substances in different environmental compartments. The use of exposure models is
recommended by ECHA74 to derive PECs. The EUSES system has long been applied to
perform the exposure assessment for chemicals for regulatory purpose74. But the tools for
evaluating the exposure of microplastics are still missing at the moment. Recently, probabilistic
material flow analysis (PMFA) has been applied in quantify the emission of macro- and
microplastics released from a variety of products to different environmental compartments in
Switzerland75. The emission of microplastics from clothing was estimated to be 3.1 t/y 75.
Although the PMFA was only used to model the emission of microplatics at the moment, it is
possible to derive PNECs from extended PMFA models as it did for nanomaterials76, 77.
Hazard assessment is another facet of risk assessment, where the predicted no-effect
concentration (PNEC) is determined72. The PNEC describes the threshold of a substance
below which no adverse effect is expected. Depending on the availability of the data, the
PNEC can be derived by applying assessment factors or from species sensitivity distributions
(SSD). Currently, only a very limited number of peer-reviewed studies report the PNEC of
microplastics for a few environment compartments78-81. Adam, et al.78 used the SSD approach
to derive a PNEC of 4.2 x 10-2 µg/L for freshwater by considering all types of microplastics in
toxicological experiments such as spheres, fragments, and fibers. A similar approach was
applied to obtain the PNEC (3.84 x 106 part/m3) for marine habitats81.
The environmental risk of a substance is characterized with the risk characterization ratio
(RCR) (Equation 1-1). Until now, the risk of microplastics was only characterized for a few
environmental compartments. The RCR for freshwater was determined by comparing the
measured environmental concentrations (MECs) with PNECs derived from SSDs and the
results showed that the risk is under control in North America and Europe, since the RCR was
several orders of magnitude below 178. However, 0.4% of the probability distribution of the
RCR values exceeded 1 in Asia, suggesting that the ecological risks associated with
microplastics in this region cannot be completely excluded78. For the marine habitats, the
average RCR was 4 x 10-4, suggesting the risk is unlikely to occur based on current data81.
22
𝑃𝐸𝐶
𝑅𝐶𝑅 = 𝐸𝑞𝑢𝑎𝑡𝑖𝑜𝑛 (1 − 1)
𝑃𝑁𝐸𝐶
Where:
RCR: risk characterization ratio
PEC: predicted environmental concentration
PNEC: predicted no effect concentration
1.8. Motivation
While efforts have been made to investigate the MPF release during washing of synthetic
textiles, the mechanism controlling the release is still not fully understood. Firstly, it is unclear
whether the released MPFs are formed during the washing process or during the
manufacturing process. There are a number of studies reporting a decrease of MPF release
from textile samples over repeated wash cycles50, 52-59
. Therefore, it is possible that the
washing process may not be responsible for the formation of MPFs. But if this hypothesis is
correct, where do those MPFs come from? Understanding the origin of MPFs is important,
since if the washing process is the major process resulting in the MPF formation, future
measures should emphasize on the improvement of washing methods. Otherwise, if the
majority of MPFs are generated during the manufacturing of textiles, efforts should be made
to optimize the production process. Secondly, due to the limited types of textile samples in
each study, it is still difficult to gain an integrated insight on how textile properties can affect
the MPF release during washing. Although there are many types of textiles tested in different
studies, the comparison of results between studies is also not easy because of the variability
experimental protocols. Furthermore, although the edge treatment of textiles has been
revealed to significantly influence the MPF release from textiles51, less is known that how the
commonly adopted cutting (e.g. mechanical cutting, thermal cutting)19 and sewing approach
can influence the MPF release.
Moreover, almost nothing is known about MPF formation associated with textile abrasion after
a period of use, since only new garments were investigated in the previous research. The
application of repetitive shear stress may induce fiber fatigue and subsequent fiber failure82.
Fiber fibrillation can happen to both synthetic and natural fibers as a result of yarn-on-yarn
23
abrasion under gentle conditions82. The fibrillation of fibers can lead to the occurrence of axial
splitting and the release of much finer fibrils. Therefore, it is reasonable to suspect that new
types of fiber fragments may be formed as a consequence of textile abrasion.
Last but not the least, although regulators have initialized some legislative process to restrict
the use of intentionally added microplastics in the consumer products83, there is no viable
alternative to replace FEs in consumer goods at the moment68. Since laundry care products
containing FEs are used by households for more than a decade and the release of
microplastics from this pathway is overlooked by current studies, it is crucial to evaluate the
current exposure level and to understand the environmental risks.
1.9. Objectives
The goal of this thesis is to provide a better understanding of the microplastic release from the
textile sector. Novel experimental methods were designed to investigate the release and
formation mechanism of MPFs from the production stages through the use stages of synthetic
textiles. Moreover, a modeling approach was developed to offer a first estimation of
environmental exposure of FEs used in laundry products and the assessment of the
associated environment risks.
The research questions of the thesis are:
I. What is the origin of MPFs in textile products?

II. What is the mechanism controlling the MPF release from textiles during washing?
III. How does abrasion of textiles affect the formation of MPFs?
IV. What is the current environmental risk of FEs used in laundry care products?
To answer the above research questions, the goals of the thesis are to:
I. Identify the important stages responsible for the formation of MPFs during the
manufacturing of synthetic textiles.
II. Identify the factors affecting MPF release from textiles during washing.
III. Quantify and characterize the MPFs generated during abrasion to reveal the MPF
formation mechanism.
IV. Estimate the exposure of FEs in different environmental compartments and
characterize the risks for selected countries.
24
1.10. Publications included in this thesis
The following papers are included in the chapters 2, 3, 4 and 5 of this thesis.
I. Cai, Y., Mitrano, D. M., Heuberger, M., Hufenus, R., & Nowack, B. (2020). The origin
of microplastic fiber in polyester textiles: The textile production process
matters. Journal of Cleaner Production, 267, 121970.
Yaping Cai conducted all experiments, evaluated the data and wrote the manuscript.
II. Cai, Y., Yang, T., Mitrano, D. M., Heuberger, M., Hufenus, R., & Nowack, B. (2020).
Systematic study of microplastic fiber release from 12 different polyester textiles
during washing. Environmental Science & Technology, 54(8), 4847-4855.
Yaping Cai performed the sample characterization, evaluated the data and wrote the
final version of manuscript.
III. Cai, Y., Mitrano, D. M., Hufenus, R., & Nowack, B. (2021). Formation of fiber
fragments during abrasion of polyester textiles. Environmental Science &
Technology, 55(12), 8001–8009.
Yaping Cai conducted all the experiments, evaluated the data and wrote the
manuscript.
IV. Cai, Y., Lin, J., Gimeno, S., Begnaud, F., & Nowack, B (2021). Country-specific
environmental risks of fragrance encapsulates used in laundry care products.
Accepted by Environmental Toxicology and Chemistry.
Yaping Cai collected all the data, performed the calculation and wrote the
manuscript.
25
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33
2. The Origin of Microplastic Fiber in Polyester Textiles: the
Textile Production Process Matters
Reprinted from the accepted article: Cai, Y., Mitrano, D. M., Heuberger, M., Hufenus, R., &
Nowack, B. (2020). The origin of microplastic fiber in polyester textiles: The textile production
process matters. Journal of Cleaner Production, 267, 121970. Copyright 2020 Elsevier.
2.1. Abstract
Microplastic fibers (MPF) are often detected in wastewater treatment plants and environmental
samples, which implies a pathway of MPF release from domestic washing of textiles into the
environment. Although there are many textile washing/release studies, it is still unclear to what
extent the liberated MPFs originate from processes during washing (e.g. abrasion) or rather
from processes earlier in the textile supply chain. Understanding the origin of MPFs is
important since different MPF formation mechanisms would lead to different mitigation
strategies. Therefore, the aim of our study was to investigate the presence of MPFs in various
intermediate and finished polyester textiles products. In this study, we developed a sonication
extraction method to quantify and characterize extractable MPFs already present in the textiles
(i.e. manufacturing related MPFs). To identify the manufacturing process responsible for the
MPF formation, this study included 18 representative products along the textile production line.
The extraction dynamics of MPFs for all materials were investigated by ultrasonication. The
extracted MPFs ranged from 15 MPF/g for a filament to 45’400 MPF/g for a scissor-cut
microfiber textile. We found that a rotor yarn exhibited an elevated number (4’310 MPF/g) of
extracted MPFs compared to other types of yarns (160-230 MPFs/g), suggesting that the rotor
spinning may be a critical step responsible for MPF formation. On average, five times more
MPFs could be extracted from textiles with processed surfaces (such as Fleece, Plain brushed
and Microfiber) compared to those with unprocessed surfaces. This suggests that abrasive
friction during production may be another critical factor for MPF formation. Furthermore,
scissor-cut textiles demonstrated three to 31 times higher number of extracted MPFs than
laser-cut textiles, enabling us to quantitatively discriminate between the contribution of MPFs
from the textile surface opposed to those originating from the textile edges. The majority of
the extracted MPFs were found to be between 100 to 800 µm in length. The results of this
study may help to reduce the MPF release from textiles by modifications throughout the
production and finishing process.
34
2.2. Introduction
The increasing global production of synthetic fibers raises the concern that microplastics
released from synthetic textiles are likely to continue contaminating our environment in the
future1. Fibers are often detected as the dominant constituent of microplastics found in waste
water treatment plants (WWTP)2-4 as well as in many environmental samples5, 6. A recent
modeling study has reported that fibers from textiles significantly contributes to microplastic
releases into freshwater7. These findings imply that a pathway of microplastic fibers (MPF)
from domestic washing of textiles into the environment likely exists8. Although WWTPs exhibit
a high removal efficiency (above 98%) for microplastics9, 10
, elevated microplastic
concentrations were still observed downstream of WWTPs compared to control sites4, 11, 12.
Moreover, approximately 50% of the sewage sludge is estimated to be used on agricultural
soils in Europe and North America13, constituting a direct release pathway of the fibers
removed during wastewater treatment to the environment. One also needs to keep in mind
the disparity of wastewater connectivity ratio to WWTPs, which ranges from about 70% in
high-income countries to only 8% in low income countries14. This results in the (direct) release
of unprocessed wastewater. Therefore, MPFs can be released into the environment
regardless of the fact that the MPFs are in the effluent or captured by the sludge.
Several studies have been performed to quantify MPF release from textiles during laundering.
Browne, et al.8 were the first to quantify the number of MPF from polyester garments. Later,
additional experiments were conducted to investigate factors which may influence MPF
release during washing, such as the addition of detergents, temperature, washing duration
and types of textiles1, 15-21. A decrease of the MPF release with repeated wash cycles has been
observed in several studies17, 18, 21. These findings spurred us to question if there were any
MPFs present in textiles before washing.
The manufacturing of synthetic textiles usually begins with polymer chips which are melted
and spun into endless filaments. These filaments are cut into short staple fibers and then
carded into slivers (Figure 2-1). In the next step, different yarn spinning methods are applied
to spin slivers into yarn. The yarn made from short staple fibers are called “spun yarns”.
Correspondingly, there are yarns made from endless filaments which are called “filament
yarns”. These yarns can then be further woven or knit into textiles. The woven textile is made
by interlacing two threads perpendicularly and the knit textile has only one thread following a
course to produce symmetric loops on both sides of the mean path. In the finishing step,
various techniques can be applied to enhance the performance, look and feel of the final
product. Some surface treatments can be applied at this stage to produce textiles with special
35
textures, such as fleece. Finally, the finished textiles are cut and tailored into garments and
delivered to customers.
Figure 2-1. A simplified flow chart of the important stages for the manufacturing of polyester
textiles. Blue blocks represent processes and white blocks represent the corresponding
products.
Understanding the source of MPFs is relevant since different origins would advocate different
mitigation strategies. If the majority of MPFs are formed during the washing process, then
changes in washing methods, such as improvements of washing detergents, or entrapments
of released MPFs during washing may be needed in the future. However, if MPFs are already
generated in the textile throughout the manufacturing process, then efforts should be made to
localize and improve the culprit process(es) in the production line or submit textiles and
garments to additional washing/cleaning steps before they are shipped to the consumer.
Since mechanical stress affects yarns and textiles at different textile processing steps, a
systematic study with the products along the production line can help in identifying the crucial
steps in MPF formation. Therefore, the aim of our study was to investigate the presence of
MPFs in various intermediate fiber products and for a number of different finished polyester
textiles. We first developed a method to quantify the extractable MPFs which were already
present in textiles and applied it to 18 samples at different stages along the production line.
The extracted MPFs were characterized (length and diameter) and counted to identify which
stages along the production line were most relevant for MPF formation. The results from this
work enable comparisons of the presence of MPFs from different textile products leading to
the understanding of the origin of MPFs, and may provide the basis for engineering options to
produce textiles with reduced MPF release.
36
2.3. Materials and methods
2.3.1. Sliver, yarns and textiles
A representative set of 18 products along the polyester textile production line was obtained
directly from manufactures and suppliers located in China and Switzerland (Table 2-1). One
sliver, one filament yarn and four spun yarns were selected to investigate the influence of
sliver production and different yarn spinning methods. To further determine the existence of
MPFs in textiles, we selected 12 textiles with different textile structures, types of yarn and post
processing finishing steps. In the manuscript, a suffix is given to distinguish the textiles made
of spun yarns “S” or filament yarns “F”, respectively. Additionally, the suffix “B” was given to
the plain textile with a brushed surface. Most of the samples were dark-colored, except for one
sliver and three spun yarns which were white. This allowed us to more easily and accurately
quantify the MPF extracted from the sample using our detection methods (see below). The
density of the textiles ranged from 75 g/m2 to 294 g/m2, which was determined by weighing
three pieces of 36 cm2 swatches. The chemical composition (polyester) of the textiles was
further confirmed by FTIR analysis (Varian 640-IR).
All samples were characterized by scanning electron microscopy (SEM) (Hitachi S6200) to
obtain structures of the textiles and yarns as well as fiber diameters (Figure 2-2, Table A1-1).
To enhance SEM contrast, the samples were sputtered with a layer of Au/Pd (nominally 7 nm
thick) in a high vacuum sputter coater (LEICA EM ACE600). Fiber diameters were
characterized by randomly measuring 10 fibers from the SEM images.
37
Table 2-1: Sliver, yarns and sliver used in the study
Density Fiber diameter

Product Surface Structure Type Yarn Color
[g/m2] [µm]
Sliver - - - - White - 12.0±1.3
- - Rotor* Spun White - 12.5±0.7
- - Air-jet* Spun White - 11.9±0.7
Yarn - - Ring* Spun White - 12.3±0.6
- - Ring* Spun Black - 12.8±1.5
- - - Filament Black - 10.8±0.4
Interlock Spun Black 209±1 12.2±0.8
Jersey Spun Black 226±1 12.8±0.8
Knit Rib Spun Black 294±2 12.7±1.1
Rib Filament Black 199±1 15.9±2.2
Unprocessed Terry Spun Black 208±2 13.0±1.3
Plain Spun Black 100±0 12.7±0.5/13.4±0.9**
Plain Filament Black 149±1 7.5±0.6/7.9±0.5**

Textile
Woven
Twill Filament Black 154±1 12.4±1.8/19.9±1.7**
Satin Filament Black 75±0 13.0±0.7/16.4±1.7**
Knit Fleece Filament Black 185±1 11.7±1.3
Plain
Woven Filament Black 131±0 9.0±1.2/10.1±1.5**
brushed
Processed
19.9x8.9/7.7x2.2***
Woven - Filament Grey 191±3
(microfiber)
* Spinning methods of spun yarns
**The diameters of the weft and the warp yarns of the woven textiles
***The width and length of the weft yarn (19.9±1.1 x 8.9±1.2 µm) and the warp yarn (7.7±0.9
x 2.2±0.5 µm) with a rectangular cross section for the microfiber sample
38
Figure 2-2. SEM images for three textile samples: A) Interlock S; B) Twill F; C) Plain B: front
side (brushed); D) Plain B: back side (unbrushed)). For the textiles made of spun yarns (Figure
2-2A), there are many fibers protruding from the textile surface. In contrast, the filament textiles
(Figure 2-2B) have a surface with few protruding fibers. Figure 2-2C and 2-2D display the front
and the back side of Plain B, where one can observe how the abrasion (brushing”) process
affects the surface of the textile. The details for the other products can be found in Table A1-
1.
2.3.2. Sample preparation
Textile scissors or a laser cutter (tt-1300, Times technology) were used to cut the textile into
swatches with a dimension of 6 cm x 6 cm. Depending on the textile sample, the weight of the
sample ranged between 0.16 g to 1.05 g. The sliver and yarns were cut by a laser cutter into
pieces of approximately 1.50 g.
The white-colored fibers were dyed using a blue-colored pigment (BEMACRON E-RD, CHT,
Switzerland) in order to provide increased contrast when imaging the fibers in subsequent
analysis steps. In brief, the dyeing process compromised of two steps, where the first step
was to dye the polyester and the second step was to fix the color and remove the extra dye
on the surface. See the supplementary information (SI) for additional details on the dyeing
procedure. The solution from the two dyeing steps was also analyzed to determine if fibers
were released through this process as well. The dyed samples were then used in extraction
experiments.
39
2.3.3. Extraction experiments and filtration processes
Extraction of MPFs was carried out in a 0.75 g/L linear alkylbenzene sulfonic acid (LAS)
solution (Alfa Aesar) that was used in previous washing experiments to mimic domestic
laundry detergent16. LAS is the main surfactant ingredient in many commercial laundry
detergents. A 1 mol/L solution of sodium hydroxide (Sigma-Aldrich) was used to adjust the pH
of the LAS solution to approximately 9.0-9.5.
For the extractions, a sample was placed into a 600 ml beaker filled with 200 ml LAS solution.
No prewashing step was performed for any of the samples. The solution, together with the
sample, was sonicated for 10 min with an ultrasonic probe with an output power of 70 W and
a frequency of 20 kHz (Sonopuls HD 2070, with probe VS 70T). The tip of the probe was
submerged in the solution 1 cm under the air-water interface. Preliminary experiments were
conducted suggesting that the majority of the extractable MPFs could be extracted from
textiles within 90 minutes. Therefore, for each sample, the experiment was stopped at either
90 min (9 sequential extraction steps) or when there were less than 20 MPFs per cycle
extracted, whichever was reached first. The temperature of the solution was between 23 to
27 °C during extraction. For all experiments, three independent replicates were performed for
each product. Between each extraction step, the beaker was rinsed with DI H2O three times
to avoid any contamination between extractions.
After each extraction, the sample was taken out of the beaker with tweezers and allowed to
drip for 15 s to remove excess liquid. The remaining solution was continuously stirred and a
10 mL pipet was used to transfer the solution to a vacuum filtration system. A vacuum pump
with a filtration unit was used to filter the liquid through a cellulose nitrate membrane (GE
Whatman, diameter 4.7 cm, pore size 0.45 µm). We attempted to avoid too many fibers on the
filters, which would result in extensive overlapping of fibers and lead to difficulties in analyzing
the number and the length of fibers in the extraction solution. Therefore, the volume of water
filtered was between 10 ml to 200 mL, depending on the expected concentration of MPFs in
the solution. The filters were put into separate petri dishes (VWR, diameter 90 mm, height 16
mm), covered, and left to dry overnight at room temperature. Moreover, to determine the
reliability of the sample collection and filtration method, triplicate aliquots from the same
extraction solution for two randomly selected textiles (Interlock S, Microfiber) were filtered
through separate filters and dried overnight as described above.
Blanks were measured three times for each experimental day, before the daily analysis, mid-
way through the analysis, and after the last extraction. This involved sonicating 200 ml of the
LAS solution for 10 min without the textile sample.
40
2.3.4. Filter imaging and analysis
A single-lens reflex camera (Nikon D850) with a macro lens (Nikon 105 mm/2.8) was used to
image all filters. A ruler was added to each filter as a scale and images (8256 x 5504 pixels)
were edited in the software Adobe Ligthroom CC (version: 2015.14) to enhance contrast. Most
of the filters were analyzed for fiber number and length with the software FiberApp (version:
1.51)22. By manually selecting the starting point and the end point of each fiber, the software
automatically calculated the fiber length and recorded the fiber number. One exception was
the sliver samples, which were analyzed using ImageJ. This is because the sliver sample shed
many long fibers which were difficult to be tracked with FiberApp. Both methods had a lower
length detection limit approximately 3-4 pixels, corresponding to about 40 µm fiber length.
Only dark-colored fibers were counted. The number of MPFs on each filter was between 4 to
1’320, with an average of 186 MPFs per filter. In total, 615 filters were analyzed and the length
of approximately 120’000 MPFs were collected individually. Additionally, the mass of extracted
fibers was also calculated for knit textiles, but not for woven textiles. This is because woven
textiles have two threads, which made it difficult to determine the diameter of fibers and
subsequently which of the two fibers were shed from the textile. The mass calculation was
done by using the measured length and the known diameter of the fiber (see Table 2-1) and
multiplying by the polyester density of 1.38 g/cm3 23.
In addition, for seven selected scissor-cut samples, the diameters of the extracted MPFs on
the filters were determined by SEM, which were then compared with the fiber diameter in the
unused textile. A high vacuum sputter coater (LEICA EM ACE600) was applied to sputter the
filter with a layer of 7 nm Au/Pd. The fibers were observed by SEM (Hitachi S6200) at a voltage
of 2.0 kV and a magnification of 400. Ten SEM images were randomly captured from each
filter and one fiber was randomly chosen from each image to obtain the fiber diameter.
2.3.5. Influence of edge processing methods on MPF extraction
Additional experiments were performed to investigate if the number of fibers extracted from
the textiles scaled linearly with the total length of the edge of the textile samples. Interlock S
samples with a constant area of 36 cm2 were cut into smaller pieces with different perimeters
of 24, 36, 48, 60 and 72 cm either by a scissor or by a laser cutter. All pieces from one 36 cm2
textile were then sonicated together for a 10-minute extraction step. For each length of the
perimeter, three replicates were performed. The filtration process and image analysis was
done according to the previous experiments.
41
2.3.6. Statistics
A linear mixed model (package “lmerTest”) in R (version 3.4.3) was used to determine the
influence by factors on the number of extracted MPFs from textiles. The four factors included
the surface treatment (unprocessed, processed), the textile structure (knit, woven), the yarn
type (spun, knit) and the cutting method (scissors, laser). Each factor was taken as a fixed
effect. The textile types (Interlock, Jersey and etc.) were considered as random effects. Since
there were several extraction steps throughout the experiment, the number used in the model
was the cumulative number of extracted MPFs. A similar model was established to determine
the influence on the length, in which the median length of extracted MPF only during the 1st
extraction step was considered. Additionally, a non-parametric Kruskal-Wallis (K-W) one way
ANOVA test in IBM SPSS statistics (version 25) was used to compare the length distribution
in the following groups: 1) the length distribution of MPFs extracted from the sliver and yarns;
2) the length distribution of MPFs extracted from the scissor-cut and laser-cut textile samples;
3) the length distribution of MPFs extracted from textile samples in sequential extraction steps.
A p-value below 0.05 was considered to constitute a significant difference for all the statistical
tests.
2.4. Results
2.4.1. Assessment of experimental procedures
We conducted several measurements to determine the reliability of the analytical workflow

and the potential for contamination throughout the experiments. First, to quantify the
contamination from dark-colored fibers, three blanks were investigated three times; before the
daily analysis, mid-way through the analysis and after the last extraction on each experimental
day. The average number of fibers was found to be 2 ± 2 MPFs per filter (n = 60), as monitored
over a period of four months. Light-colored fibers do not interfere with the measurements,
since we only counted dark-colored fibers through the entire experiment. An example of
extracted MPFs collected on the filters for four types of textiles is shown in Figure 2-3.
42
Figure 2-3. MPFs extracted from four types of textiles: A) Interlock S; B) Plain F; C) Fleece
and D) Microfiber.
By analyzing three aliquots from the same washing solution for two randomly selected
samples (Interlock S and Microfiber), we found a similar fiber number (relative standard
deviation < 4%) and MPF length distribution (Figure A1-1). These results confirm that the sub-
sampling method used was representative for quantification of MPFs in our system and that
the chosen workflow yielded reproducible results. Moreover, all experiments were carried out
in triplicate. The average relative standard deviation of MPF number for different samples was
29%, ranging from 1% to 83%. In previously published studies, the average relative standard
variation of fiber number ranged between 20% 24 to 36% 16.
2.4.2. Extraction dynamics of MPFs
To track the origin MPFs along the manufacturing process, we investigated one filament yarn,
one sliver, and four spun yarns. All the dyed products (Sliver, Rotor, Air-jet, Ring-white)
demonstrated an elevated initial MPF release during the dyeing steps, followed by a decrease
in subsequent extractions. The decreasing trend of MPF release during extractions was also
observed for the undyed black-colored ring yarn. For the sliver and the rotor yarn, the number
43
of extracted MPFs remained high after several extractions at approximately 50 and 220 MPF/g
respectively, compared to the air-jet yarn, the white-colored and the black-colored ring yarns
with less than 20 MPF/g (Figure 2-4). The number of extracted MPFs from the filament yarn
remained at low level (smaller than 20 MPF/g) during the extraction steps.
Figure 2-4. Number of extracted MPFs from slivers and yarns. All results are presented in
number of MPFs per gram of textile. Standard deviations were calculated from triplicate
experiments.
The number of MPFs extracted from 12 textiles after each extraction step was also determined
(Figure 2-5 and Figure A1-2). In general, we observed a strong decrease in the number of
extracted MPFs between the 1st and 2nd extraction steps, followed by a relatively slow
decrease in subsequent extractions. One exception was the scissor-cut Plain B, which
demonstrated a slight increase in the 8th and 9th extraction steps. Therefore, we continued the
extraction for this sample with three more extractions. The results showed that the number of
extracted MPFs from scissor-cut samples dropped to a mean level of 62 MPF/g, compared
with the ones extracted from the 9th step (689 MPF/g). Since there was no elevated number
of extracted MPFs for the laser-cut samples and the standard deviation of this 9th sample was
much higher than for the extractions before and after, this suggest that the peak at extraction
step 9th was an outlier.
44
Knit Scissor-cut Laser-cut Woven
A B
20000 Interlock S 3000 Plain S
2500
[MPF/g textile]
[MPF/g textile]
15000
2000
10000 1500
Unprocessed surface
1000
5000
500
0 0
1 2 3 4 5 6 7 8 9 1 2 3 4 5 6 7 8 9
Extraction steps Extraction steps
C 3000
D
3000 Rib F Twill F
[MPF/g textile]
2500 2500
[MPF/g textile]
2000 2000
1500 1500
1000 1000
500 500
0 0
1 2 3 4 5 6 7 8 9 1 2 3 4 5 6 7 8 9
E F
20000 Fleece 3000 Plain B
Processed surface
[MPF/g textile]
2500
[MPF/g textile]
15000
2000
10000 1500
1000
5000
500
0 0
1 2 3 4 5 6 7 8 9 1 2 3 4 5 6 7 8 9
Figure 2-5. The number of extracted MPFs from textiles as a function of the number of
extractions steps. Six textiles with different textile structures, yarn types and surface
treatments were selected to present here and the remaining six samples are shown in Figure
A1-2. All results are presented in number of MPFs per gram of textile. The black lines
represent the scissor-cut samples, the red lines show results for laser-cut samples. Error bars
represent the standard deviation for triplicate experiments.
2.4.3. Cumulative number of MPFs extracted from sliver, yarns and textiles
To estimate the total amount of MPFs present in the products, we summed the extracted fibers
from all extraction steps (Figure 2-6). A logarithmic scale was used to cope with the large
differences in the number of extracted MPFs from different samples. For the sliver and yarns,
45
the lowest number of extracted MPFs was found for the filament yarn with a cumulative
extraction of 15 MPF/g. That was about 40 times lower than the number of MPFs extracted
from the sliver (590 MPF/g), which suggested that MPFs may be formed during sliver
production. Moreover, the number of extracted MPFs from spun yarns was influenced by the
spinning method. The majority of the yarns (Air-jet, Ring-black, Ring-white) exhibited a lower
number of extracted MPFs than the sliver. On the other hand, the amount of MPFs extracted
from the rotor yarn (4’310 MPF/g) was approximately seven times higher than the MPFs
extracted from the sliver, suggesting that the rotor-spinning process may be responsible for
some MPF formation.
For the textiles, the cutting method was one of the most critical factors which significantly
influenced the number of extracted MPFs (p-value < 0.001). The ratio of the cumulative
number of MPFs extracted from scissor-cut (black symbols) to laser-cut (red symbols)
samples was determined (Figure 2-6), where this is a constant ratio between the two variants.
In practice, one can think of this difference between black and red symbols as an indication
for the “extra” MPFs extracted due to the cutting method alone. It is interesting to note that the
textiles with unprocessed surfaces exhibited a relatively high scissor-to-laser ratio with an
average of 19. Meanwhile, the surface-processed textiles demonstrated a much lower scissor-
to-laser ratio, averaging approximately 6. This suggested that there was a relatively higher
share of MPFs extracted from the entire surface area when the surface underwent additional
surface treatment.
Besides the cutting method, the number of extracted MPFs from textiles was influenced by
the surface treatment. The linear mixed-effect model showed that the number of extracted
MPFs from the textiles with processed surfaces was significantly higher than those from the
textiles without surface treatment (p-value < 0.001). The highest number of extracted MPFs
was found for the Microfiber textile, with 45’400 MPF/g and 11’300 MPF/g for the scissor-cut
and laser-cut samples respectively. That is approximately 60 times higher than the number of
MPF extracted from Twill F, which exhibited the lowest number of extracted MPFs (scissor-
cut: 760 MPF/g; 120 MPF/g laser-cut). On the other hand, there were no significant influences
observed by the yarn type (spun, filament) or the textile structure (woven, knit).
46
Figure 2-6. Cumulative number of MPFs extracted from the sliver, the yarns and the textiles
in number of MPFs per gram of material. The mean values for the scissor-cut and laser-cut
methods are represented by the black dots and red dots, respectively. Error bars indicate the
standard deviation from triplicate experiments.
Furthermore, we found that the number of extracted MPFs during the 1st extraction step
usually accounted for a high percentage of the total cumulative extraction (Figure A1-3). The
results show that for 9 out of 13 scissor-cut samples and 12 out of 13 laser-cut samples, more
than 50% of their cumulative MPFs were extracted during the first extraction. In comparison,
the number of the MPFs extracted in the last step only accounted for a few percent of the
cumulative extraction; only 3% for the scissor-cut samples and 8% for the laser-cut samples,
on average. For nine out of 13 laser-cut samples, the experiments were stopped in less than
90 minutes, meaning that there were fewer than 20 MPFs per cycle extracted.
2.4.4. Length distribution of extracted MPFs
Although the number of extracted MPFs varied significantly between samples, the length
distribution of released MPFs was relatively similar. The majority of the extracted MPFs were
found to be between 100 and 800 µm in the 1st extraction (Figure 2-7). Significantly longer
MPFs were extracted from the sliver (median: 405 µm) than those from the filament (median:
285 µm, p-value of 0.009). Another notable feature for the sliver was that there were some
47
much longer fibers, as indicated by the outliers in Figure 2-7, some of which were over 10’000
µm. The MPFs extracted from rotor yarns were significantly shorter (median: 226 µm, p-value
< 0.001) than those from other spun yarns (median: 393 µm).
The shortest MPFs extracted from textiles were found in laser-cut Plain B, with a median
length of approximately 184 µm, while the longest was found in scissor-cut Rib F (median:
595 µm). The length profile of extracted MPFs from textiles was affected by several factors.
In particular, the surface treatment was identified as one of the critical points influencing the
length of MPFs, with processed surfaces having shorter lengths than those from textiles with
unprocessed surfaces (p-value < 0.004). Moreover, we found that the knit textiles tended to
have significantly longer MPFs than the woven textiles (p-value of 0.04). No statistical
differences in the length of MPFs was observed between the textiles made from spun yarns
and the textiles made from filament yarns (p-value of 0.882).
Furthermore, we found that the length of fibers which were extracted was significantly affected
by the cutting method. The MPFs extracted from seven scissor-cut textiles (Interlock S, Jersey
S, Rib S Terry S, Rib F, Fleece and Microfiber) had longer lengths than those from the laser-
cut ones. In contrast, five textiles, including Plain S, Plain F, Plain F, Twill F and Plain B, had
longer MPFs extracted from laser-cut samples. It is notable that all of those that shed longer
MPFs from laser-cut samples have a woven structure.
48
Figure 2-7. Length distribution of MPFs extracted during the 1st extraction step. The MPFs
extracted from 1st extraction steps were present here, except for the dyed samples (Sliver, Air-
jet, Ring-white, Rotor) where the MPFs from the 1st dyeing solution were present here. 25th
and 75th percentiles were plotted in the boxes with a line indicating the median. Whiskers
represent 95% of length distribution and outliers were labelled dots representing 0.7% of total
distribution. The values presented here were a summation of three experimental replicates.
The number of MPFs plotted per sample was between 59 for Air-jet to 3’498 for Plain B, with
an average of 993.
Additionally, we analyzed the changes in length across all extraction steps (Figure 2-8, Figure
A1-4). In general, after a few extraction steps, the length of MPFs extracted from the same
textile was more or less constant. A pairwise K-W test was used to compare the length of
MPFs from the neighboring steps. For example, the extraction from 1st and 2nd, 2nd and 3rd
were compared in pairs, and so on. For the scissor-cut samples, the length of the extracted
MPFs often increased significantly between steps in the first few extractions. However, after
the 3rd or 4th extraction, there were no longer statistical differences between the steps. On the
other hand, no significant difference in length between steps was observed for most of the
laser-cut samples.
49
Knit Scissor-cut Laser-cut Woven
A Interlock S B Plain S
Length of MPFs [µm]

10000 10000
1000 1000
Unprocessed surface
100 100
1 2 3 4 5 6 7 8 9 1 2 3 4 5 6 7 8 9
Extraction step Extraction step
C Rib F D Twill F

10000 10000
1000 1000
100 100
1 2 3 4 5 6 7 8 9 1 2 3 4 5 6 7 8 9
E Fleece F Plain B
Processed surface
10000 10000
1000 1000
100 100
1 2 3 4 5 6 7 8 9 1 2 3 4 5 6 7 8 9
Figure 2-8. Length distribution of MPFs extracted during the sequential extraction steps. 25th
and 75th percentiles were plotted in the boxes with a line indicating the median. Whiskers
represent 95% of length distribution and outliers were labelled by dots representing 0.7% of
total distribution. The value present here was a summation of three experimental replicates.
The number of MPFs plotted per distribution was between 20 to 3’498 with an average of 663.
The diameter of extracted MPFs on the filters was compared with the fiber diameters within
the original textile swatches to gain further insight into the origins of the extracted MPFs
(Figure A1-5). The results show that most of the liberated MPFs shared a similar diameter as
50
the fibers in the parent textile. This is also true for the Plain F, which possesses the smallest
fiber diameter in our sample set.
2.4.5. Investigating the edge effect
Additional experiments were performed to further investigate if the number of fibers extracted
from the textiles scaled linearly with the total length of the edges. The Interlock S textile of
fixed surface area (36 cm2) was cut into a number of smaller pieces, resulting in additional
edges. For the laser-cut samples, an average extraction of 188 MPF/g was observed
regardless of the length of the edges (Figure 2-9), which corresponds to 5.2 MPF/g textile*cm2.
In contrast, for the scissor-cut samples, there is a linear correlation (Equation 2-1) between
the number of extracted MPFs and the total edge length (correlation coefficient of 0.984 with
a p-value < 0.001). The intercept of the regression line was set at 5.2 MPF/g*cm2, representing
the number of extracted MPFs from the textile surface of a 36 cm 2 swatch alone (i.e. the
number of fibers detected upon extracting fibers from the laser cut textile swatches). The slope
of the equation suggests that 346 MPFs can be extracted from one centimeter of cut textile
edge.
Equation (2-1)
51
Scissor-cut
Laser-cut
30000
y = 188 + 346*x, R2 = 0.984

[MPF/g textile]
20000
400
200
10000
0
24 48 72
0
24 36 48 60 72
Perimeter [cm]
Figure 2-9. Correlation between the number of extracted MPFs and the samples’ perimeter.
Black dots represent the extraction from the scissor-cut samples and the red dots represent
the extraction from the laser-cut samples. The black line indicates the linear regression
between the number of MPFs extracted and the length of the perimeter for scissor-cut samples.
The red line indicates the average extraction from the laser-cut samples. Error bars represent
the standard deviation from triplicate experiments.
2.5. Discussion
2.5.1. Ultrasound as a method to extract embedded MPFs
In this manuscript, the method we investigated to extract fibers from textiles was an ultrasound
extraction. A short-duration (2 to 5 minutes) ultrasonication has been found to cause little
damage to textiles in several previous experiments which assessed the removal of soil
contaminants from textiles25-30. That is not only true for polyester textiles26 but also for silk
textiles28. By forming and collapsing bubbles or cavities, ultrasound is considered as a gentler
way to remove surface contamination from textiles than methods using mechanical agitation,
which causes textile-textile friction.
Although the duration of the ultrasonication and the input energy is different between the
experiments in the literature and our present study, the results from our study suggest that
ultrasound itself does not produce a significant amount of MPFs. On one hand, we observed
that the number of extracted MPFs from the textiles dropped to 3-8% of the cumulative amount
after several extractions, suggesting that the sonication is not responsible for the major
amount of extracted MPFs. On other hand, we also have not observed any sign of damage or
52
pills on the fabric and the fiber structure itself remained intact after several extraction steps,
as verified by SEM images. However, since there was still a relatively small amount of MPFs
extracted from the samples at 90 minutes, we cannot exclude the possibility that the
ultrasound treatment generated a small amount of MPFs. Additionally, some MPFs in the
textiles may only be extracted after a longer period of time, and thus would not be accounted
for in our study.
2.5.2. The origin of MPFs in textile products
To track the origin of MPFs, we need to recall the manufacturing process of polyester textiles.
Our hypothesis was that fibers and fabric are subjected to strong forces during certain steps
in manufacturing and are responsible for the formation of MPF. Endless melt-spun fibers are
converted into filament yarns or cut into staple fibers of lengths between 25 to 150 mm, which
are further carded into slivers31, 32. As we can see in Figure 2-7, the extracted MPFs typically
had a length below 1’000 µm, which is 25 times shorter than the length of the shortest staple
fiber (25 mm). Therefore, neither the endless filaments nor the sliver is likely to be the origin
of MPFs found in our experiments. The number of MPFs extracted from the filament yarn was
below 15 MPF/g. That is in agreement with our hypothesis that there should not be any MPFs
originating from “endless filaments”, except for cross contamination from the production site,
which can be removed in the first few extractions. On other hand, we found a broad length
distribution of MPFs in the sliver ranging from 80 to 50’000 µm. There are many possibilities
of how these fibers may have formed during the sliver production. First, filaments are often
texturized before being cut and as a result they might not always be perfectly straight when
they are caught by the blade. Second, the machines usually work on a rotating-cutting principle
leading to unintentional cuts of protruding fiber ends. Moreover, staple fibers are processed
into a carding machine where very sharp edges are applied to merge and parallelize fibers.
Thus, it is also possible that these edges may cut fibers in a non-controlled way. The liberated
MPFs shared a similar diameter as the fibers in the parent textile, suggesting that the majority
of the shed MPFs we analyzed originated from the textile and that abrasion by cross-sectional
fibrillation (resulting in smaller fiber diameters) is a negligible mechanism of MPF production.
Although fibers underwent additional mechanical stress during spinning the sliver into yarn,
most of the spun yarns exhibited a lower number of extracted MPFs than the sliver. One
reason may be because yarn has a tighter structure and twisting the yarn creates tensile force,
which prevents the extraction of MPFs present in the yarn core. Moreover, the air-jet and ring
spinning processes often involve a stage where the fibers are drawn and parallelized and
53
where some of the ultrashort fibers may already be removed. However, there is one exception,
the rotor yarn, which shed substantially more MPFs than the sliver as well as the other yarns,
suggesting that the rotor spinning process might be the primary step responsible for the
formation of MPFs. In rotor spinning, opening rollers with very sharp edges are used to open
up the fiber bundle before twisting it together into a yarn. In addition, it is also known that the
accumulation of fiber dust (in other words: MPF) in the rotor groove can result in yarn defects
and end breakages (Lawrence, 2010), which may also contribute to the formation of ultrashort
fibers. However, we must consider that in the current experimental regime there are only a
limited number of fiber samples and they are sourced from different companies. Therefore,
they do not represent samples from one production line. Further research needs to be
performed to better quantify how much variability exists in the MPF content of fiber samples
from a larg(er) variety of machinery.
The next step along the production line is to weave or knit yarn into textiles. Although we found
a similar number of MPFs extracted between the spun yarns and the laser-cut textiles made
of spun yarns, we cannot draw a conclusion that the weaving or knitting of yarn into textiles
does not form MPFs. That is because textiles may be intensively washed during the finishing
process, which could remove some short fibers from the yarn. Therefore, future studies are
needed to investigate the influence of knitting or weaving from yarn to textile with more
controlled samples.
Some treatments can be applied to the textile surface to achieve a special texture. For
example, a screw-like shearing blade is commonly used to cut the surface fibers of fleece to
create a fuzzy feel. Additionally, several abrasion processes (e.g. sand blasting or rubbing
with sandpaper) can also be used to improve the look and feel of the textile. On one hand, a
large quantity of MPFs may be formed during this stage and remain in the textile. On the other
hand, with a looser surface structure, the MPFs present in the textiles may be more readily
extracted. Therefore, it is not surprising to find a statistical difference between the amount of
MPFs extracted from the textiles with processed and unprocessed surfaces.
One of the most important findings in our study is that the amount of MPF extracted from
textiles was significantly influenced by the cutting method. From the SEM images, we know
that the textile edges of laser-cut samples exhibited a seal of molten polymer and the scissor-
cut samples consisted of a large number of open ends near the edge (Figure A1-6). Therefore,
the major source of MPFs from laser-cut samples is the surface and for the scissor cut ones
the source is both the surface and the edges. We observed a much higher number of extracted
MPFs from all 12 scissor-cut samples compared to the laser-cut samples, suggesting that the
cutting method plays an important role in the number of MPF which can be extracted from
54
textiles. There is the possibility that the textile samples were contaminated by other fibers
during production or shipping. However, this contamination level should not be above the
amount of extraction from the laser-cut ones, which means the difference of extracted MPFs
between the scissor- and laser-cut samples was indeed due to the cutting method. Since
cutting textiles is normally undertaken when tailoring garments, as a consequence, tailoring
could be jointly responsible for the formation of MPFs present in garments.
There are two ways that scissor cutting can contribute to the MPFs extracted from textiles.
One is that cutting creates openings at the ends of the yarns by fraying, which enables the
extraction of MPFs present inside the yarn trapped during spinning. The other possibility is
that the fibers are formed during the cutting process itself. All knitted textiles share a basic
loop structure. Therefore, cutting through the loops may produce loose fiber fragments sitting
on the edge that can easily be removed by extraction. For woven textiles, the cutting line can
pass at random fiber positions leading to the formation of MPFs. We observed that the length
of extracted MPFs from scissor-cut knit textiles was longer than those from woven textiles.
However, there is no difference between the two kinds of structures in terms of the number of
extracted MPFs.
Based on the results, we propose to use a combination of extractions from laser- and scissor-
cut samples to develop an “extraction equation” for each textile (Equation 2-2):
Equation (2-2)
where “extractionlaser” is based on the laser-cut samples and “extractionscissor” on the scissor-
cut samples. With this equation, we can predict the number of extracted MPFs from a larger
piece of textile by considering both the surface area as well as the length of the edges (Table
2-2). The ratio of edge/surface release is between 3 for Fleece and 53 for Plain S. This
procedure could be used as a standardized test that would be suitable to estimate the number
of extractable MPFs present in textiles based on extraction of small textile swatches. For
example, upscaling from the scissor-cut sample of 36 cm2 to a fleece textile of 1 m2 (edge 4
m) would result in an extraction of approximately 2’234’000 MPFs. The influence of the
area/perimeter ratio decreases with increasing surface area. For a 1 m2 fleece textile, only 3%
of the MPFs originated from the edge, but the percentage increases 50 times for a 0.01 m2
textile. For Plain S, with the highest ratio of edge/surface, the corresponding release from a 1
m2 piece would result in an extraction of 180’000 MPF, with 56% of MPFs originating from the
edge.
55
Table 2-2. Estimated MPFs extracted per cm2 surface area and per cm perimeter. The
calculations were performed according to Equation 2-2 and based on the cumulative number
of extracted MPFs.
Ratio
Extraction from Surface Extraction from edge
edge/surface
Textile
[MPF/(g*cm2)] [MPF/(g*cm)] [cm]
Twill F 3 27 9
Plain F 7 69 10
Satin F 7 86 12
Rib F 4 98 25
Plain S 3 159 53
Jersey S 12 268 22
Terry S 10 328 33
Rib S 17 518 30
Interlock S 11 556 51
Plain B 21 312 15
Fleece 300 781 3
Microfiber 313 1422 5
In addition, it is interesting to note that although the length of extracted MPFs from different
textiles exhibited a degree of variation, the majority of extracted MPFs shared a similar length
range between 100 µm to 800 µm. The similarity in the length of extracted MPFs may be
explained by the origins of MPFs. We have identified that there are two plausible origins of
MPFs in textiles. The first is a “liberation” of existing MPFs which are produced during the
manufacturing process. Although there are many textile varieties for different purposes on the
market, the manufacturing processes of slivers, yarns and textiles are rather similar. Therefore,
it is not surprising that the length of MPFs produced during the manufacturing exhibit a high
degree of similarity. The second origin of MPFs is suspected to be “production” through the
textile cutting process. Apart from the fact that there are many different textile structures such
as interlock, jersey, plain, and twill, there were often variations derived from some basic
structures. For example, all knitted textiles are knitted by the yarn following a meandering path
to form symmetric loops and all the woven textiles are made by two or more threads interlaced
56
at a right angle. This might be another reason that the length of MPFs is limited to a relatively
narrow range.
2.5.3. Comparison with previous studies on the MPF release from textiles
Several studies have investigated the MPF release from synthetic textiles during washing,
using either real domestic washing machines8, 17, 18, 33-35 or lab washing machines to simulate
the domestic washing process16, 19, 20, 24. We cannot directly compare our numbers of extracted
fibers to these studies or estimated releases from different textiles during washing as the
release mechanism may not be the same. Further studies have to show how the extraction
used in our work relates to the number of MPF released during washing. Moreover, the MPFs
can be also formed in the use phase of textiles. Therefore, the number of the MPFs extracted
in our study do not correspond to the total release including the use phase. The MPFs
extracted from textiles products may correlate with the MPF release during the first few
washing cycles, which needs to be confirmed in future studies.
However, several conclusions regarding the release mechanisms can still be made. Because
the washing studies investigated different textiles with various experimental setups and
analytical methods, the amount of MPFs released per wash reported varied, ranging from
0.012 mg/g15 to 3.3 mg/g18, from 23 MPF/g15 to 1’273 MPF/g24. Our work has shown that the
type of textiles and the treatment of edges can also strongly influence the magnitude of release.
The material used in different studies varied from whole garments8, 34 to pieces of textiles24, to
double folded and sewn edges16 to scissor-cut edges20. These variables make it difficult to
directly compare the results amongst or between the studies with the data we have collected
here. For instance, we found that the MPF extracted from the scissor-cut Jersey S during the
first extraction was 0.4 mg/g, which is much higher than the 0.1 mg/g release for the jersey
textile per wash reported by Hernandez, et al.16, using doubled folded and sewn edges.
Because we demonstrated the importance of the cutting method and the ratio edge/surface is,
different studies cannot be compared without a fully standardized procedure.
While there are some studies quantifying the number or the mass of MPFs released during
textile washing, there is limited information regarding the length of MPFs released. A few
recently published studies provided more detailed length distributions of released MPFs by
characterizing a larger number of MPFs16, 24, 35. Sometimes the length profile was also provided
in the form of a “size range” with intervals usually above 200 µm 19, 34. Some previous studies
only suggested an average length of MPFs released by sampling a limited number of MPFs
57
on filters15, 17. The length of the released MPFs ranged from 100 µm16 to 25 mm15, depending
on the application of different filtering and analysis methods. The MPFs from our study fell into
a range between 100 to 800 µm which is in accordance with the findings by Hernandez, et
al.16 and De Falco, et al.24, using a similar filtration technique and analysis methods.
2.5.4. Implications for the textile industry
Our results confirm that a predominant fraction MPFs may already be present in textiles when
manufactured. The rotor yarn production method leads to the most important number of
extracted MPFs compared to the other yarns. This is a strong indication that the rotor spinning
process may be a critical stage responsible for the MPF formation during the yarn spinning. A
more representative study on rotor-processed yarns is now advised. Furthermore, a
comprehensive investigation is needed to compare different spinning methods, which requires
the collaboration between industry and academia. A precise location of the origin of MPFs in
the production process will guide any future efforts to minimize MPF release. Additionally, we
observed that textiles with processed surface treatments (fleece, brushed surface) exhibited
a significantly higher release than the other types of textiles.
Furthermore, for all textile variants, the laser-cut samples demonstrated on average 17 times
fewer extracted MPFs than the scissor-cut ones, suggesting that adopting cleaner cutting
methods (e.g. during tailoring) is another option for the industry to help reduce the MPF
release since the majority of the MPF originates from the edges of the textile and not from the
textile surface. Scrutinizing the cutting and seaming processes thus offers another means to
minimize MPF release from garments. Finally, our results revealed a sharp decrease in the
number of extracted MPF after the 1st extraction, which typically accounted for more than 50%
of the total number of fibers extracted. Therefore, prewashing cut textiles or garments once at
the factory and collecting the released MPFs before delivery to the customers may be an
efficient way to remove a large part of the present MPFs in the products, which was also
suggested by other researchers19.
2.6. Conclusions
Although there have been a number of textile washing/MPF release studies performed in the
recent years, the origins of MPFs released during the wash cycle has remained unclear. In
this study, we have developed an ultrasonic extraction method to extract and characterize
MPFs already present in the textiles, which was used to discern MPFs exclusively generated
in the production process. A representative set of 18 polyester products along the textile
58
production line was investigated. We found that the rotor spinning and surface treatment are
among the most critical steps responsible for the formation of MPFs during the yarn production
and textile production, respectively. Moreover, the cutting methods to create textile swatches
(and, to begin tailoring garments) had a significant influence on the number of extracted MPFs.
We used this insight to differentiate between surface- and edge- contributions of total MPF in
the extraction process.
Our results confirm the presence of MPFs in textiles throughout the manufacturing process.
Since the first extraction consistently released the majority of the total MPFs, we propose that
prewashing textiles may remove a significant portion of the production-initiated MPFs from a
textile product at a point source (i.e. the factory). However, it should be noted that MPF which
are intrinsically in the textiles from the manufacturing process do not necessarily influence the
formation of additional MPF during washing, wearing or the later use phase(s). Therefore, the
number of the MPFs extracted in our study does not correspond to the total release of MPFs
from textiles during the whole life cycle. Instead, our results confirm that it is analytically
possible to discern between production-inherited MPF and those which are produced as part
of the use phase of the life cycle, which opens up new avenues to systematically study release
scenarios that include abrasive washing and usage.
2.7. Acknowledgements
We would like to thank Leonie El Issawi-Frischknecht and Markus Hilber from Empa for their
assistance in textile sample preparation and for valuable discussions. Additionally, we would
like to thank Laura Knezevic for help in dyeing the samples. This research was partially
supported by funds from the Zürcher Stiftung für Textilforschung and the Swiss National
Science Foundation, Ambizione grant number PZP002_168105.
59
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23. Kallay, N.; Grancari, A.; Tomi, M., Kinetics of polyester fiber dissolution. Textile
Research Journal 1990, 60, (11), 663-668.
25. Hurren, C.; Cookson, P.; Wang, X., The effects of ultrasonic agitation in laundering on
the properties of wool fabrics. Ultrason Sonochem 2008, 15, (6), 1069-1074.
26. Gotoh, K.; Hirami, C., Soil removal from polyester fabric by laundering with frequency-
modulated ultrasound. Journal of Oleo Science 2012, 61, (5), 249-254.
27. Gotoh, K.; Harayama, K., Application of ultrasound to textiles washing in aqueous
solutions. Ultrason Sonochem 2013, 20, (2), 747-753.
28. Gotoh, K.; Harayama, K.; Handa, K., Combination effect of ultrasound and shake as a
mechanical action for textile cleaning. Ultrason Sonochem 2015, 22, 412-421.
29. Gotoh, K.; Nakatani, H.; Tsujisaka, T., Delicate laundering of textiles with application of
38 kHz ultrasonic waves. Textile Research Journal 2015, 85, (15), 1565-1578.
30. Ma, M.; You, L.; Chen, L.; Zhou, W., Effects of ultrasonic laundering on the properties
of silk fabrics. Textile Research Journal 2014, 84, (20), 2166-2174.
31. Krifa, M.; Ethridge, M. D., Compact spinning effect on cotton yarn quality: Interactions
with fiber characteristics. Textile Research Journal 2006, 76, (5), 388-399.
62
2), 290-293.
63
3. A Systematic Study of Microplastic Fiber Release from 12
Different Polyester Textiles during Washing
Reprinted with permission from the accepted article: Cai, Y., Yang, T., Mitrano, D. M.,
Heuberger, M., Hufenus, R., & Nowack, B. (2020). Systematic study of microplastic fiber
release from 12 different polyester textiles during washing. Environmental Science &
Technology, 54(8), 4847-4855. Copyright 2020 American Chemical Society.
3.1. Abstract
Microplastic fibers (MPF) have been found to be a major form of microplastic in freshwaters
and washing of synthetic textiles has been identified as one of their main sources. The aim of
this work was to use a panel of twelve different textiles of representative fiber and textile types
to investigate the source(s) of the MPF released during washing. Using standardized washing
tests, textile swatches tailored using five different cutting/sewing methods were washed up to
10 times. The MPF quantity and fiber length were determined using image analysis. The 12
textiles demonstrated a great variability in MPF release, ranging from 210 to 72’000 MPF/g
textile per wash. The median MPF length ranged from 165 µm to 841 µm. The number of
released MPF was influenced by the cutting method that scissor-cut samples released 3 - 21
times higher numbers of MPF the laser-cut samples. The textiles with mechanically processed
surfaces (i.e. fleece) released significantly more (p-value < 0.001) than the textiles with
unprocessed surfaces. For all textiles, the MPF release decreased with repeated wash cycles
and a small continuous fiber release was observed after 5-6 washings, accompanied by a
slight increase in fiber length. The decrease in the number of MPF released is likely caused
by depletion of the production-inherited MPFs trapped within the threads or the textile structure.
The comparison of MPF release from laser-cut samples, which had sealed edges, and the
other cutting methods allowed us to separate the contributions of the edge- and surface-
sourced fibers from the textiles to the total release. On average, 84% (range 49-95%) of the
MPF release originated from the edges, highlighting the importance of the edge-to-surface
ratio when comparing different release studies. The large contribution of the edges to the total
release offers options for technical solutions which have the possibility to control MPF
formation throughout the textile manufacturing chain by using cutting methods which minimize
MPF formation.
64
3.2. Introduction
The ubiquitous presence of microplastics in the environment1-6 as well as in biota7, 8 has been
reported by hundreds of studies. A mixture of fibers, beads, and fragments were usually found
in environmental samples, where microplastic fibers (MPF) were reported to account for a
large proportion of all microplastics9-11. A modeling study has shown that fibers released from
textiles are one of the most important sources of microplastics in freshwaters12. One pathway
is likely from synthetic clothing where domestic washing may release a high number of fibers13,
14
. Although the removal efficiency of microplastics in wastewater treatment plants can reach
98% or higher15, 16, the few percent of MPF which are not captured can make a contribution of
about 20% to the microplastic release to freshwaters12. Alternatively, MPF captured during
water treatment can enter the terrestrial environment when sewage sludge is applied on soil17-
20
.
Several studies have investigated the general release of MPF from textiles during washing,
addressing a few factors in isolation that were hypothesized to control the release13, 21-32. The
MPF release was mostly found to decrease with increasing number of wash cycles21, 27-32,
sometimes reaching a plateau between the 4th and 5th wash30, 31. However, a relative stable
release over time was also observed in one study, which proposed that MPF may have been
formed during textile manufacturing process prior to washing24. The addition of liquid or
powder detergents was reported to either increase22, 24, 27 or have no impact28, 32 the MPF
release compared to pure water, while textile softeners were found to significantly reduce the
MPF release22. A recent study revealed that a higher water volume can elevate the release of
MPF during washing because of the increasing hydrodynamic pressure on fibers32. In addition,
other factors including temperature, duration of the wash cycle and mechanical stress (number
of steel balls added to the container) were investigated, but there was no significant influence
of these factors on the MPF release22, 24, 32.
The textile samples tested in previous studies were either garments purchased on the market14,
23, 26, 27, 29
or consisted of only a limited types of textile samples21, 22, 24, 25. Although efforts have
been made to compare MPF release between different washing system33, considering the
variability of experimental protocols adopted by the different studies, it is still difficult to
comprehensively compare the results on MPF release from textiles with different properties
(e.g. surface treatment, textile structure and yarn type) and to gain an integrated insight on
how those properties influence the MPF release through the washing process. Furthermore,
the cutting method has been identified as being one of the most critical factors affecting the
number of MPF released from textiles during washing25. The most commonly used cutting
approach in industry is mechanical cutting where knives are vertically guided to cut multiple
65
layers of textiles34. Besides, thermal cutting is also applied during textile tailoring34. Then cut
edges are often sewn with stiches in the later step. Similar to the industry, many studies
adopted either mechanically cut swatches with sewn edges31 or thermally cut swatches21, 32 to
reduce MPF shedding from edges. However, it is still unclear whether those procedures can
really prevent MPF release from the edge and how the cutting/sewing method affects MPF
release.
Therefore, the aim of our study was to systematically investigate the influence of textile
properties and tailoring methods on the MPF release during washing. In particular, we place
special emphasis on studying the influence of industrially used cutting/edge sewing methods.
We suspect that: 1) MPFs are already present in the textile before washing and are only
released but not generated through the washing procedure; 2) MPF release from textiles
during washing will be affected by textile properties such as surface treatment, textile structure
and/or yarn type); 3) higher mechanical stress will lead to increased MPF release; 4) textiles
with tailored edges will release fewer MPFs than the textiles with scissor-cut edges without
any treatment. The results from this work will not only form a basis for the understanding of
the mechanisms which influence MPF release from textiles during washing, but also provide
evidence to help the industry to develop better mitigation strategies.
3.3. Materials and methods
3.3.1. Textiles
A set of 12 commercially available polyester textiles were obtained directly from different
manufacturers (Table 3-1). Seven of the textiles were made of filament yarns and five of spun
staple fiber yarns. The suffix “S” or “F” was used to distinguish textiles made from spun yarns
(staple-length fibers) or filament yarns (endless fibers), respectively. Six woven and six knitted
textiles were used. The production of some types of textiles can include a mechanical surface
treatment, where the surface fibers are cut to create a fuzzy or soft texture of the final product34,
35
. For the fleece, there is a shearing process where the surface fibers are cut by a blade. For
textiles with brushed surface, the break of surface fibers is usually carried out by a metal brush
in the brushing process. In our study, a fleece textile and a plain textile with brushed surface
was investigated and they were referred as textiles with processed surface. The suffix “B” was
given to the plain textile with a brushed surface. A microfiber cloth containing fibers with a
much smaller diameter than all the other textiles was also included. All samples were dark-
colored and ranged in density from 75 to 294 g/m2 (determined by weighing three pieces of
66
36 cm2 samples). FTIR analysis (Varian 640-IR) confirmed the chemical composition
(polyester) of all textile samples.
Scanning electron microscopy (SEM) (Hitachi S6200, 2.0kV, x40) was used to characterize
the textile structure and fiber diameter (Table 3-1, Table A2-1). Before observation under the
SEM, a layer of 7 nm Au/Pd was sputtered on the samples’ surface by a high vacuum sputter
coater (LEICA EM ACE600) to enhance the contrast. To determine the fiber diameter, ten
fibers from the textile were randomly measured on the SEM image.
Table 3-1. Characterization of textile physical properties.
Density Fiber diameter

Surface Structure Type Yarn Color
[g/m2] [µm]
Interlock Spun Black 209±1 12.2±0.8
Jersey Spun Black 226±1 12.8±0.8
Knit Rib Spun Black 294±2 12.7±1.1
Rib Filament Black 199±1 15.9±2.2
Unprocessed Terry Spun Black 208±2 13.0±1.3
Plain Spun Black 100±0 12.7±0.5/13.4±0.9*
Plain Filament Black 149±1 7.5±0.6/7.9±0.5*
Woven
Twill Filament Black 154±1 12.4±1.8/19.9±1.7*
Satin Filament Black 75±0 13.0±0.7/16.4±1.7*
Knit Fleece Filament Black 185±1 11.7±1.3
Plain
Woven Filament Black 131±0 9.0±1.2/10.1±1.5*
Processed brushed
19.9x8.9/7.7x2.2**(
Woven - Filament Grey 191±3
microfiber)
*The diameters of the weft and the warp yarns of the woven textiles
**The width and length of the weft yarn (19.9±1.1 x 8.9±1.2 µm) and the warp yarn (7.7±0.9 x
2.2±0.5 µm) with a rectangular cross section for the microfiber sample
Textiles were cut into small pieces with sizes depending on the requirement of the experiments
(Figure 3-1). For the first three sets of experiments, the swatches were cut either with textile
scissors or a laser cutter (tt-1300, Times technology) into pieces of 4 x 10 cm according to the
ISO standard 105-C0636. The weight of these samples ranged between 0.29 and 1.30 g. To
discriminate the influence of the cutting/sewing methods, an additional set of textile swatches
were cut to a larger size of 10 x 10 cm to have enough area available to sew the edges. Three
additional types of cutting/sewing methods commonly used in industry were investigated:
model cutting (MC) (SAMCO type SB 25 A), overlock sewing (OS) and double-folded sewing
(DS). An overlock sewing machine (BERNINA 2000D) was used to sew the edges with
overlock stiches (width: 5 mm; length: 2.5 mm; density: 10 stiches per inch), which is one of
67
the most commonly used stiches to tailor the edges in garment manufacturing. For the double-
sewn samples, the edges were folded twice and then sewn with simple stiches (length: 1.5
mm; density: 17 stiches per inch) as described in our previous study24. Both overlock- and
double-sewn samples were originally scissor-cut, and white cotton threads were used to sew
the samples so that it would not interfere with our MPF analysis later in the study. The
contribution of the sewing thread to the total weight of the finished sample was between 3%
and 6%. The size of a finished double-sewn swatch was approximately 5 x 5 cm with an
average weight of 1.47 and 2.29 g per piece for Plain F and Interlock S, respectively. Examples
of the finished samples can be found in Figure A2-1.
Figure 3-1. Flow chart of the study. 12 types: 12 types of textiles as shown in Table 3-1; 4
types: Fleece, Interlock S, Plain F, Plain S; 2 types: Plain F and Interlock S. SC: scissor cutting;
LC: laser cutting; DS: double-folded sewing; MC: model cutting; OS: overlock sewing.
3.3.3. Washing experiments
Domestic washing was simulated by a Gyrowash lab washing machine (James Heal,
GyroWash Model 1615). Before each wash cycle, the steel vessels were rinsed with deionized
water H2O three times and a five minute rinse cycle with linear alkylbenzene sulfonic acid
(LAS) solution (0.75g/L, pH 9.2 ±1) was performed. LAS solution was used to simply mimic
the liquid laundry detergent commonly containing a more complex composition used in
households, as was done in our previous study24. Two of the eight steel vessels were used as
68
blanks containing only LAS solution in each experimental round and the blank vessels were
always randomly chosen for the next round of experiments. No prewash step was performed
on the textile samples. All experiments were performed in triplicates. A schematic of the work
flow is shown in Figure 3-1. The washing experiments were conducted following a
standardized wash procedure from ISO (105‐C06, 1994) with a slight modification of the
washing solution (Table A2-3) and no adjacent textile was used. One piece of textile was
added to a steel vessel (500 ml) with 150 ml LAS solution together with ten steel balls
(diameter of 6 mm). Each wash cycle lasted for 45 min at a temperature of 40 °C. This
standardized washing condition was applied once to all 12 textiles in the experiment which
investigated the influence of textile properties on MPF release. To determine the influence of
repeated wash cycles on MPF release, four representative textile variants (Fleece, Interlock
S, Plain F, Plain S) with scissor-cut and laser-cut edges were washed for ten rounds following
the washing condition as described above. The wash liquid from 1st, 2nd, 3rd, 5th, 8th and 10th
round was filtered and analyzed. The influence of mechanical stress on the MPF release was
investigated by adding different number of steel balls (0, 10 and 20) for the four selected
samples (Fleece, Interlock S, Plain F, Plain S). To study how the edge treatment influenced
the MPF release, samples of two selected textiles (Plain F and Interlock S) were prepared with
five different cutting/sewing methods as described in the previous section. The experiments
followed the standardized conditions and three wash cycles were performed for each
treatment.
3.3.4. Water collection and filtration
After each wash cycle the textile sample was taken out of the vessel with tweezers and allowed
to drip for 15 seconds to drain excess liquid. The washing liquid remaining in the vessel was
continuously stirred to keep the suspension homogenous. Then the liquid was transferred by
a 10 ml pipet to a filtration system consisting of a filtration unit and a vacuum pump. The wash
water was filtered through a cellulose nitrate membrane (GE Whatman diameter 4.7 cm, pore
size 0.45 µm). To avoid too many overlapping fibers on the filters, the volume of the filtered
solution was adjusted to be between 1 and 50 mL depending on the MPF concentration,
aiming for 100 to 200 MPFs per filter. All filters were dried in separate petri dishes (VWR,
diameter 90 mm, height 16 mm) covered with corresponding caps at room temperature
overnight.
69
3.3.5. Filter imaging and analysis
The filters were imaged by a single-lens reflex camera (Nikon D850) with a macro lens (Nikon
105 mm/2.8) together with a calibration slide for microscope with a smallest scale of 100 µm
(VWR Catalog number: 630-1123). The images (8256 x 5504 pixels) were edited in the
software Adobe Lightroom CC (version: 2015.14) to enhance the contrast. All images were
analyzed with the software FiberApp (version: 1.51)37 for MPF number and length. The semi-
automatic software allowed manual selection of the starting and the end points of each fiber
and automatically recorded the fiber number and calculated the fiber length. In total, the
individual lengths of 52,800 MPF were recorded from 530 filters with a detection limit of 7-8
pixels, corresponding to about 90 µm in length. Examples of filter images can be found in
Figure A2-2 and A2-3. Additionally, to determine the mechanism of fiber breakage, fibers
released from Interlock S during the 1st and 10th washing cycle on the filter were sampled by
adhesive tape and nine fibers were randomly selected to image the fiber ends with SEM
(Hitachi S6200, 2.0kV, x1.80). The experimental procedure was assessed in terms of level of
contamination and reliability of a standardized workflow, which can be found in the
supplementary information.
The mass of released MPF from knit textiles was calculated by multiplying the density of
polyester (1.38 g/cm3)38 by the measured length and the known diameter of the fibers (Table
3-1). For woven textiles, the mass cannot be calculated because there are two types of yarns
with different diameters which we could not separate with the chosen image analysis method.
3.3.6. Statistics
For the experiment investigating textile properties, the influence of three factors including the
surface treatment (unprocessed, processed), the textile structure (knit, woven), and the yarn
type (spun, filament) on the number and length of MPF released from scissor- and laser-cut
textiles was determined by a linear mixed model (package “lmerTest”) in R (version 3.4.3.)
respectively. The three factors and the textile types (Interlock, Plain and etc.) were considered
as fixed and random effects, respectively. For the other experiments, a one-way ANOVA test
in IBM SPSS software (version 25) was used to determine the impact of different treatments
on the number of MPF released in the following groups: 1) mechanical stress: experiments
with different steel balls; 2) cutting/sewing methods: five different ways of cutting/sewing
technique. A non-parametric Kruskal-Wallis (K-W) one-way ANOVA test in IBM SPSS
software (version 25) was applied to compare the length distribution of the mentioned groups.
The p-value of any statistical test below 0.05 was considered to indicate statistical significance.
70
3.4. Results
3.4.1. MPF release from 12 polyester textiles
The number of released MPF per wash demonstrated a large variety ranging from 210 MPF/g
for laser-cut Twill F to 72,000 MPF/g for scissor-cut Microfiber (Figure 3-2A, Table A2-4). The
majority of the MPF exhibited a length between 100 to 1000 µm (Figure 3-2B, Table A2-5).
The shortest MPFs were released from laser-cut Microfiber (median: 165 µm), while the
longest MPF were found from scissor-cut Terry S (median: 841 µm).
Furthermore, the cutting method and the surface treatment of the textile were found to have
significant impact on the MPF release. The scissor-cut samples released 3 - 21 times higher
numbers of MPF than the laser-cut textiles (Figure 3-2A). The length distribution was displayed
in a notched box plots, where there is a strong evidence (95% confidence) of different medians
if two boxes' notches do not overlap39. For most of the samples, the MPF shed from the
scissor-cut samples exhibited longer length (Figure 3-2B). The textiles with mechanically
processed surfaces released significantly more MPF (p-value < 0.001) than textiles with
unprocessed surfaces for both scissor-cut and laser-cut samples. On the other hand, the linear
mix model shows that the textile structure and the yarn type were found to have no significant
influence on the number of MPF released. The MPF length seemed to be influenced by textile
structure and surface treatment depending on the cutting methods. The scissor-cut woven
textile and the laser-cut textile with processed surface shed significantly shorter MPFs than
the knit textile (p-value = 0.0297) and the textile with unprocessed surface (p-value < 0.001)
respectively.
71
Figure 3-2. A) Number of MPF released from 12 polyester textiles during the 1st wash cycle in
number of MPF per gram of textile. The mean values are represented by the black dots
(scissor-cut) and red dots (laser-cut). Error bars show the standard deviation for three
experimental replicates. The mean of the blanks for this set of experiments is displayed as a
horizontal line. S/L stands for the scissor to laser ratio, which was calculated number of
released MPF from SC sample divided by LC sample; B) Length distribution of MPF released
during the 1st wash cycle. The values presented here are a summation of triplicate experiments.
The number of MPF plotted per box was between 182 and 1498, with an average of 560. The
boxes represent 25th and 75th percentiles with the median indicated by a line. The notches
represent 95% confidence interval for the median. Whiskers and outliers are not shown on the
graph. The complete datasets can be found in Figure A2-5. Asterisks are given to those where
the median length was significantly different between laser-cut and scissors-cut samples.
3.4.2. MPF release during repeated wash cycles
To investigate the influence of repeated wash cycles on MPF release, four textiles were
washed for ten wash cycles and the wash liquid from selected rounds were filtered and
analyzed. A decrease in the number of MPF released in the first three wash cycles was
72
observed for all the samples (Figure 3-3, Table A2-6 and A2-7). Depending on the type of
textiles, six to 120 times higher numbers of MPF were released in the 1st wash cycle than the
10th wash cycle. After 3 to 5 wash cycles, the number of released MPF either stabilized at a
lower level or slightly increased. The number of MPF released after the 10th wash cycle was
still above the blank (4 MPF per filter) with an average between 10 and 1200 MPF/g. In terms
of length, most of the samples released significantly shorter MPFs in the 1st wash cycle
compared to the 10th cycle (Figure 3-4, Table A2-8), especially for Fleece. To determine the
mechanism of fiber breakage, MPFs were randomly selected to characterize the morphology
of fiber ends by SEM and the images suggest that the most MPFs released from the 1st (Figure
3-5A) and 10th (Figure 3-5B) wash cycles had ends similar to those caused by the scissor
cutting (Figure 3-5D). In addition, a comparison between the MPFs shed from scissor- and
laser-cut samples (Figure 3-5A and 3-5C) shows that both sample shed some MPFs with
distorted ends, but MPFs possessing molten ends were exclusively found for laser-cut
samples.
Number released [MPF/g textile]
A Scissor-cut textile swatches B Laser-cut textile swatches

100000 100000
Plain F Plain F
Plain S Plain S
10000 Interlock S 10000 Interlock S
Fleece Fleece
1000 1000
100 100
10 10
Blank: mean = 4 MPF Blank: mean = 4 MPF
1 1
1 2 3 4 5 6 7 8 9 10 1 2 3 4 5 6 7 8 9 10
Wash cycle Wash cycle
Figure 3-3. Number of MPF released per cycle, as a function of the number of wash cycles for
Plain F, Plain S, Interlock S and Fleece. A) and B) are for scissor-cut and laser-cut samples,
respectively. All values are presented in MPF per gram of textile. Error bars show the standard
deviation for three experimental replicates. The mean of blanks (n = 4 MPFs) for this set of
experiments is displayed as a horizontal line.
73
Scissor-cut Laser-cut
A Plain F B Plain S
2500 2500
2000 2000
MPF length [µm]
1500 1500
1000 1000
500 NA 500
0
1
*2 *3 *5 *8 *10 * 2 * *3 *5 * *10*
1 8
C Interlock S D Fleece
2500 2500
2000 2000
MPF length [µm]
1500 1500
1000 1000
500 500
0
1
* 2 * * 3 * * 5 * * 8 * *10 0
1
* 2 * * 3 * * 5 * * 8 * *10*
Figure 3-4. Length distribution of MPF released during the 1 , 2 , 3 , 5th, 8th and 10th wash
st nd rd
cycle. NA: less than five MPFs. The values here were a summation of triplicate experiments.
The number of MPF plotted per box was between 10 and 1277 with an average of 318. The
boxes represent 25th and 75th percentiles with the median indicated by a line. Whiskers and
outliers are not shown on the graph. The complete datasets can be found in Figure A2-6.
Asterisks are given to those samples where the median length was significantly different from
the 1st release.
74
Figure 3-5: Characterization of MPFs released from Interlock S A: scissor-cut, 1st wash cycle;
B: scissor-cut, 10th wash cycle; C: laser-cut, 1st wash cycle; D: Examples of scissor-cut and
molten fiber ends. SEM images were taken under 2 kV and the magnification was 1.80 k.
To calculate the cumulative release of MPF during the ten wash cycles, the number of MPF
released from 1st to 10th wash cycles was summed up. An interpolation was made for the
cycles were no analysis was performed (4th, 6th, 7th and 9th wash cycles). We assumed that the
number of released MPF in the wash cycles which were not analyzed was the mean number
of its neighboring cycles. For instance, to estimate the release during 4th wash cycle, we
averaged the number of MPF released from 3rd and 5th wash cycles. The resulting cumulative
release is shown in Table A2-9. The release during the first wash cycle accounted for 30%
(Plain S) to 90% (Plain F) of the cumulative release.
3.4.3. MPF release with different mechanical stress and cutting/sewing methods
The number of steel balls added (0, 10 and 20) did not show a statistically significant impact
on the number of MPF released for the majority of tested samples including Plain F, Interlock
S and Fleece (Figure A2-7, Table A2-10). On the other hand, a similar MPF length distribution
75
was found for most of the textiles regardless of the level of mechanical stress during the
experiments.
Five different cutting and sewing methods were tested to examine their influence on MPF
release. Only laser cutting significantly reduced the amount of the MPF release from textiles
during washing (Figure 3-6, Table A2-11). Laser-cut Interlock S released a cumulative number
of 1’300 MPF/g in the first three washes which was about 7 to 12 times lower than for the
other cutting/sewing methods. Similar results were found for Plain F, where the laser-cut
sample shed fewer MPFs (370 MPF/g) than the other treatments (3760 – 7’400 MPF/g). No
significant difference was found for the number of MPF released between the other four types
of cutting/sewing methods (scissor-cut, model-cut, double-sewn, overlock-sewn) for Interlock
S. However, for Plain F, the overlock-sewn sample released 1.5 to 20 times more MPF (7’400
MPF/g) than the other cutting/sewing methods. In addition, all treatments decreased the
number of MPF released through multiple wash cycles (Figure A2-9 and A2-10).
The length of MPF released from the textile with different cutting/sewing methods exhibited a
larger variability for Plain F than for Interlock S. Scissor-cut Plain F released approximately
two times longer MPF (median: 434 µm) than the double-sewn samples (median: 204 µm)
during the 1st wash cycle, while the Interlock S released MPFs with length ranged from 363
(double-sewn) to 528 µm (model-cut). For both textiles, the shortest MPF were found for
double-sewn samples.
Figure 3-6. A) Influence of the cutting/sewing method on the number of MPFs released from
two textiles during the 1st wash cycle. The mean values are represented by black (laser-cut),
red (double-sewn), blue (model-cut), green (scissor-cut) and purple (overlock-sewn) symbols.
Error bars indicate standard deviation for three experimental replicates; B) Length distribution
of MPF released during the 1st wash cycle. The boxes represent 25th and 75th percentiles with
the median indicated by a line. Whiskers and outliers are not shown on the graph. The
complete datasets can be found in Figure A2-8.
76
3.5. Discussion
Our work explored the hypothesis that a significant fraction of MPF released during washing
of textiles were already present in the textile during the manufacturing process and not
produced during the number of wash cycles investigated here. We found that the number of
MPF released was greatly influenced by the number of wash cycles, with fewer MPF observed
in the wash water after the first cycle, as has been observed in other studies21, 27-32. This
strongly indicates that MPF were present in textile products before washing and that the act
of washing released the MPF which were on/in the textile. The morphology of the fiber ends
can inform us about the processes responsible for fiber breakage40, 41
. For example, a
mushroom head indicates that the fracture was caused by a high tensile force (Figure A2-11).
For washing the most relevant scenario is breakage by fatigue failure, resulting in fiber ends
that have been split into finer fibers or fibrils41. Another form of fiber failure is surface wear and
peeling, which often leads to tapered ends or multiple splits41. In our experiments, the SEM
images showed no sign of fibrillation or splits at the fiber end. Most of the MPF released from
scissor-cut samples during the 1st and 10th wash cycles showed a solid end similar to the
scissor-cut ones. Some MPFs exhibited distorted ends seem to be originated during
manufacturing process where mechanical stress such as transverse pressure can happen
deliberately or accidentally.
The relatively steady release of MPF after a few washings suggests that a part of the fibers
have a slow release dynamics. The MPF released during the 10th wash cycle were significantly
longer compared to the MPF from the 1st wash cycle for most of the samples. Since longer
fibers are more entangled within the textile structure, they may require more time to work their
way out from textile. It may be possible that additional breakage and release of fibers could
be expected during laundering with older textiles as they experience more wear during use,
but this was not evaluated in this present study.
The textiles with mechanically processed surfaces exhibited higher MPF releases than those
with untreated surfaces, which was also observed in some other studies21, 30
. Processed
surfaces investigated by this study are produced by cutting surface fibers by blade or brush.
On one hand, it is possible that a number of loosely entangled MPF are generated during this
process. On the other hand, such processes can loosen both yarn and surface structure,
therefore making the release of MPF from within the textile structure easier. The statistical
analysis showed that the MPF released from the laser-cut processed textiles had shorter
lengths suggesting that shorter MPF may be generated during the surface treatment process.
Another point worth noting is that although textiles with processed surface sheds higher
77
amount of MPFs at the beginning, after ten rounds of washing, the MPF release decreased to
the same level than the unprocessed textiles.
We hypothesized that higher mechanical stress would lead to higher MPF release during
washing, since the steel balls may contribute to the abrasive friction on the fibers or to increase
textile bending and consequently loosening the structure to release more pre-existing MPF.
However, the mechanical stress enacted by adding different number of steel balls did not
influence the number and length of MPF released for most samples in our experiment. This
may be due to the timeframe of the experiment was too short to observe any significant impact
induced by adding steel balls.
Two aspects are suspected to contribute to the fact that the scissor-cut samples released
more MPFs than the laser-cut textiles. On one hand, the cutting process may open up the yarn
at the end which results in the release of MPF present inside. On the other hand, it is also
possible that some new MPFs are generated during the cutting processes. This can be derived
from the fact that some scissor-cut samples released significant longer MPFs than the laser-
cut ones, which is an indication that a new population of MPFs may be formed. For the laser-
cut samples, the yarns are melted together at the end which largely prevent the "opening up"
at the yarn end. Moreover, even though the laser cutting can generate some new MPF similar
to scissor cutting, most of those newly generated MPFs will be probably melted/bonded into
"solid" ends. Therefore, most of them cannot be released in the future washing process.
Most of the cutting/sewing methods (model cutting, double sewing and overlock sewing) did
not significantly reduce the MPF release from textile during washing, which is against our
hypothesis that textile with sewn edge release less MPF. The overlock-sewn sample even
released higher numbers of MPF than the samples with raw edges. The elevated level of
release may be due to additional damage by cutting or needling during the overlock sewing
process. Since overlock sewing is one of the most commonly used hemming/seaming
methods in the textile industry, this finding is highly relevant for those who want to identify the
stages responsible for the generation of MPF during the textile manufacturing.
The evaluation of the results using the different cutting/sewing method can be used to gain
additional insight on the origin of MPF released from within the textile. The SEM images show
that the edges of laser-cut samples were molten and sealed, while the scissor-cut edges were
loose and open (Table A2-2). Therefore, we can assume that all the MPF released from laser-
cut samples originate from the textile surface rather than the edges. For the scissor-cut textiles
it can then be expected that release from the textile surface should be equal to the laser-cut
78
samples and that the additional fibers measured are released from the edges. Therefore, a
“release equation” can be proposed for each textile (Equation 3-1):
Equation (3-1)
where “MPFSC” and “MPFLC” are the MPF releases from the scissor- and laser-cut samples
respectively, and “Releasetextile” is the mass-specific MPF release from a textile (in MPF/g).
With this equation, the number of MPF released from a larger piece of textile can be predicted
as shown in Table 3-2. For 10 out of 12 textiles, the MPFs shedding from edges contributed
to more than 80% to the total release. It is worth noting that the majority of MPF released from
textiles with processed surface still originated from the cut edge, especially for Plain B where
the edge was responsible for more than 90% of the MPF release. For the edge-to-surface
ratio, no statistically significant influence was found by the surface treatment, the textile
structure and the yarn type.
Table 3-2. Estimated mass-specific MPFs released per cm2 surface area and per cm perimeter
from the textile samples (4 x 10 cm2) during washing when fabric swatches have a scissor-cut
edge. Release from the fabric surface is measured from fabric swatches with laser-cut edges.
The ratio of the MPF release from the edges and surface was calculated for the sample that
has an area of 40 cm2 and a perimeter of 28 cm. Releasesurface and Releaseedge were calculated
based on Equation (3-1).
Releaseedge Releasesurface Releaseedge/Releasesurface
Textile
[MPF/(cm*g)] [MPF/(cm2*g)] [cm]
Satin F 26 19 1
Twill F 100 5 19
Rib F 193 7 30
Plain F 186 19 10
Terry S 221 9 23
Plain S 235 28 9
Rib S 249 31 8
Jersey S 291 23 12
Interlock S 391 15 26
Fleece 475 253 2
Plain B 1251 58 22
Microfiber 2001 408 5
79
The 12 textiles investigated in our work demonstrated a great variability in MPF release. The
upper limit observed in our study is much higher than found in other studies reporting a range
from 4 to 13’000 MPF (Figure A2-12). The length range of the fibers released in our study
(100-1000 µm) is in accordance with previous measurements22, 24, 27, 29. The MPF release from
the Microfiber (72’000 MPF/g), is the highest among all the published studies in terms of fiber
number. The generally higher number of MPF released in our study can be explained by the
higher edge-to-surface ratio (0.70 cm) of our samples compared to other Gyrowash studies
(with a ratio of 0.34 - 0.43 cm)21, 22, 25. Since we have found that the edge released much more
MPFs than the surface of textile, the higher edge-to-surface ratio will result in higher MPF
release when the result is normalized to the textile weight. Some previous studies reported
lower release in terms of number but higher mass release per wash compared to our study
(Table A2-12, Figure A2-12 and A2-13). That may because a few studies only measured the
weight of the released MPFs and estimated the fiber number based on the average length of
a few MPFs. The mean value is influenced by extremes which may not be accurate enough.
Therefore, we believe it is conceptually better to work with a number-based MPF release
method.
Since our study has shown that the majority of the released MPFs during washing likely
originate from edges instead of the surface of the textile, adopting the cleaner cutting
technique is important for industry to help reduce the MPF release from textile as a source of
microplastics. Furthermore, a prewash of tailored garments at the factory could effectively
collect a large portion of the production-inherited MPF. One thing to be kept in mind is that the
MPF release quantified here were only those released during the laundering process. That
may not accurately reflect a real world scenario, since other processes such as wearing
process are also involved and may account for additional MPF releases in subsequent washes
as the textile ages. In addition, when standardizing the quantification method of MPF release
from textiles, it is extremely important to be cautious about the cutting methods and edge-
surface ratio. Besides, although the image analysis method is time consuming, it is
conceptually better than the mass-based method if we want to gain a complete profile of the
MPF release (number, length).
We would like to thank Melanie Halter from Empa for the assistance in the preparation of
textile samples. This research was partially supported by funds from the Zürcher Stiftung für
Textilforschung.
80
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84
4. Formation of Fiber Fragments during Abrasion of
Polyester Textiles
Reprinted with permission from the accepted article: Cai, Y., Mitrano, D. M., Hufenus, R., &
Nowack, B. (2021). Formation of fiber fragments during abrasion of polyester textiles.
Environmental Science & Technology, 55(12), 8001–8009. Copyright 2021 American
Chemical Society. Copyright 2021 American Chemical Society.
4.1. Abstract
Fiber fragments are one of the dominant types of microplastics in environmental samples,
suggesting that synthetic textiles are a potential source of microplastics to the environment.
Whereas the release of microplastics during washing of textiles is already well studied, much
less is known about the release during abrasion processes. The abrasion of textiles may
induce fibrillation of fibers and therefore result in the formation of much finer fiber fragments.
The aim of this study was to investigate the influence of abrasion of synthetic textiles on the
formation of microplastic fibers and fibrils. Fleece and interlock textile swatches made of
polyester were abraded using abrasion tests with a Martindale tester. The microplastic fibers
and fibrils formed during abrasion were extracted from the textiles and characterized in terms
of number, length and diameter. The microplastic fibers demonstrated the same diameter than
the fibers found in the textiles (fleece: 12.3 µm; interlock: 12.7 µm), while fibrils with a much
smaller diameter (fleece: 2.4 µm; interlock: 4.9 µm) were also found. The number of fibrils
formed during abrasion in both textiles was higher than the number of microplastic fibers. The
majority of the extracted microplastic fibers had a length between 200 and 800 µm, while most
fibrils were between 30 and 150 µm, forming two distinct fiber fragment morphologies. The
number of microplastic fibers formed during abrasion was 5 to 30 times higher than the number
of microplastic fibers that could be extracted from non-abraded samples. The number of fibrils
increased after abrasion by more than a factor of 200 for both fabric types. The fibrils formed
during abrasion have diameters that fall within the inhalable size for airborne particles. The
potential release of fibrils into air during wear of textiles thus raises questions about the human
exposure to these materials. Since the Martindale tester can simulate a daily application
scenario of textiles over a prolonged period only in a limited way, future studies are needed to
establish the correlation between the test results with a real-world scenario.
85
4.2. Introduction
Microplastic fibers (MPFs) are one of the dominant types of microplastics found in
environmental samples1-6, suggesting that synthetic textiles may be an important source of
microplastics to the environment. For aquatic systems, one study estimated that about 35%
of the global releases of microplastics into the ocean originated from washing of synthetic
textiles7. Similar conclusions were drawn for freshwaters by a recent modeling study,
indicating that clothing ranked as the second largest source of all microplastics to Swiss
freshwaters8. It is estimated that about 0.17 to 0.28 million tons of MPFs reach the aquatic
system annually9, 10 and the emission is expected to continue to grow in the future10. The
occurrence of microplastics has been detected in atmospheric fallout3, rain11 and household
dust4, 12. The deposition rate of microplastics was estimated to range from 1586 to 11,130
particles/m2/day for the indoor environment4, 12, which is much higher than the rate obtained
for the outdoor environment from remote U.S. conservation areas (132 particles/m 2/day)11 or
a European metropolitan region (137 - 512 particles/m2/day)13. The size of the microplastics
reported in the studies is usually between 11 and 5,000 µm, while the majority of detected
MPFs had a size below 500 µm5, 14. A study investigated the occurrence of MPFs in urban air
in Beijing, where MPFs with a length below 20 µm were reported to be the dominant types of
airborne fibers15. Since MPFs are commonly detected in air samples and the composition is
consistent with those used in textiles, this raises the hypothesis that MPFs released from
synthetic textiles are an important source of airborne microplastics11, 16.
MPFs can be released from textiles to air during wearing clothes17. A recent study quantified
MPF release into air from textiles, where garments made of different types of textiles were
worn by volunteers and the MPFs released into air were collected on filter paper17. The results
showed that the MPF release ranged from 1 to 403 MPF per g textile with a length between
494 and 1034 µm, depending on textile properties, resembling the fibers released from textiles
during washing18. Besides, for most types of the textile samples, the release to air during
wearing was approximately 10 times higher than the release to water during washing,
highlighting the importance of wearing as a pathway of MPF release to the environment 18.
Another study focused on the emission of fluorescent aerosol particles from volunteers
wearing different garments made of polyester, cotton or a mixture during specified activities in
a closed chamber. The results showed that the mode size of the released fluorescent aerosol
particles was between 3−5 μm and volunteers wearing long clothing (i.e. long-sleeve shirts
and pants) emitted more fluorescent aerosol particles than those wearing short clothing (i.e.
t-shirts and shorts)19. Therefore, there is a possibility that microplastics with much smaller size
can be released from synthetic textiles to air during wearing.
86
It is still unknown how the abrasion of textiles after a period of use will affect the MPF formation.
The MPFs observed in washing studies have a similar diameter to the original fibers in the
textile18, 20. There is evidence that the application of repetitive shear stress on textile fibers can
cause fiber fatigue which subsequently leads to fiber failure21. The yarn-on-yarn abrasion of
polyester or nylon fibers under gentle conditions (leading to a long life in the test, e.g. failure
after 35 000 cycles) can result in fibrillation, where axial fiber splitting occurs and much finer
fibrils can be formed and worn away21. This fibrillation does not only happen to synthetic fibers,
but can be also observed for natural fibers, such as cotton21. The size of airborne fibers is
relevant, since it is generally acknowledged that particles with an aerodynamic diameter larger
than 30-70 µm can quickly deposit22. Particles with an aerodynamic diameter less than 10 µm
are often referred to as "inhalable particles"22.
The aim of this study was to investigate the influence of abrasion of synthetic textiles on MPF
and fibril formation (together designated as fiber fragments in the following). The abrasion
experiment was conducted by a Martindale tester which was originally designed to test the
abrasion resistance of upholstery textiles. The MPFs and fibrils formed during abrasion were
then extracted from the textile samples and deposited on a filter. A scanning electron
microscope (SEM) was applied to characterize the fiber fragments on filters and then the fiber
fragments were analyzed in terms of number, length and diameter. The results from this work
will not only lead to a better understanding of MPF and fibril formation during abrasion, but
provide a new method for investigating MPF and fibril release during abrasion.
4.3. Material and method
Black-colored interlock and fleece polyester textiles were obtained directly from manufactures
(Table A3-1 and Figure A3-1). The textiles were also used in the previous studies18, 20 to
investigate the formation of MPFs during manufacturing and the release of MPFs during
washing. The textile samples were cut by a laser cutter (tt-1300, Times technology) into circles
with diameters of either 38 mm (specimen) or 140 mm (abradant) following the ISO standard
12947-2:201623, where the specimen is rubbed against the abradant during the abrasion test.
The average weight for the fleece sample was 0.21g (specimen) and 2.84 g (abradant), and
for the interlock sample it was 0.23 g (specimen) and 3.23 g (abradant).
A prewash step was performed to remove the majority of extractable MPFs generated during
manufacturing20 as well as to reduce the interference by dusts and residues. All samples were
87
prewashed three times with 150 mL linear alkylbenzene sulfonic acid (LAS) solution (0.75 g/L
pH 9.2 ± 0.1) at 40 ºC with a Gyrowash lab washing machine (James Heal, GyroWash model
1615) as described in previous washing studies18, 24. No steel balls were used during washing,
since the use of steel ball may result in higher abrasion25. After prewashing, the textile samples
were dried under an aluminum foil at room temperature overnight. The change of sample
weight before and after prewashing and drying was below 0.5%.
4.3.2. Abrasion experiments
The textile wearing process was simulated by using a Martindale tester (4-station Martindale
tester. SN-103/06/1049, James Heal) (Figure A3-2). This instrument is designed to test the
abrasion resistance of the upholstery textile by rubbing textile samples against a standard
surface under a specific pressure23. The endpoint of the test is when the breakdown of textile
samples can be determined, where the criteria of breakdown refer to "thread breakage" or
"worn off area" as indicated in the ISO standard 12947-2:201623. The textile abrasion
resistance can be evaluated by recording the number of rubs needed until the endpoint. The
ISO standard aims at evaluating the quality of textile products and thus an extreme scenario
is considered. Since our study was designed to simulate the daily use of textiles, the abrasion
experiment was stopped after 5000 rubs. At this time, pilling was observed on the surface of
the fabrics. Compared with complete thread breakage, the pilling phenomenon is commonly
observed for polyester textiles under typical use conditions26. Some additional modifications
were made to the ISO standard to collect MPFs and fibrils from the apparatus. Firstly, the
standard abradant was replaced with the same material as the specimen, thereby simulating
a fabric-on-fabric rubbing situation. Secondly, the standard woven felt textile and the
polyetherurethane foam material were not used as underlays to back the abradant and
specimen, to avoid input of additional fibers unrelated to the test textile into the system. Instead,
rubber sheets (thickness of 1.5 mm) were cut into the size of the specimen and abradant by a
scissor and were used to replace the standard overlays. The rubber sheet had a smooth
surface from which fibers could be rinsed off more easily. Additionally, a metal ring made of
stainless steel (inner diameter of 13.3 cm, thickness of 1.3 cm, height of 4.8 cm) was mounted
on each station to avoid cross contamination between samples and to collect the MPFs/fibrils
deposit to the apparatus (see Figure A3-3).
Before the abrasion test, the equipment was cleaned with liquid soap, water and an air blower
to remove any contamination. During each round of abrasion experiments, 12 kPa pressure
was randomly placed on three stations and the fourth one served as a control (noted as
88
"control-abrasion" in Table 4-1). The setting for the control was the same as the abraded
samples, except that the specimen was lifted from the abradant to avoid any abrasion. A white
coat made of cotton and powderless nitrile gloves were worn throughout the experiment.
Since the system was not completely closed, we checked if MPFs or fibrils could escape from
the system by placing double-sided carbon tape (PLANO G3347, diameter of 12 mm) on the
top, middle and bottom of the three metal rings enclosing the abrasion samples as shown in
Figure A3-3. The tape was observed after the abrasion experiment under a SEM to assess if
MPFs deposited on the metal rings.
4.3.3. MPF and fibril extraction
MPFs and fibrils were collected from both the apparatus (steel sample holder, ring, and rubber
overlay) and extracted from the textile samples (abradant and specimen). 150 ml LAS solution
was used to rinse the apparatus and the liquid was collected. MPFs and fibrils in the textile
abradant and specimen were extracted separately with 150 ml LAS solution using a Gyrowash
lab washing machine (James Heal, GyroWash model 1615) for 45 min at a temperature of
40 °C. No steel balls were added during the washing. The samples were then squeezed to
remove excess water. To better disperse the MPFs in the extraction liquid, the solution was
sonicated for 3 minutes using an ultrasonic probe (Sonopuls HD, 2070; with probe VS 70T;
power 70 W; frequency 20 kHz; amplitude 25%; pulse 1s). The sonication is unlikely to cause
damage to the fibers and result in the generation of MPFs or fibrils as reported in a previous
study20. The solution was transferred by a pipette to a vacuum filtration system and the solution
was filtered onto a cellulose acetate membrane (diameter of 13 mm, pore size of 0.45 µm,
Sartorius GmbH). Depending on the concentration of MPFs and fibrils determined in pretests,
between 1 and 50 ml of extraction liquid was used as a subsample to avoid too much
overlapping of fibers on the filter. The filtered volume for each sample can be found in Table
A3-2. The filters were dried in a petri dish with a cap at room temperature overnight.
To determine the contamination level during extraction, two blanks containing only LAS
solution were randomly inserted into each extraction cycle (noted as "control-extraction" in
Table 4-1). To assess the baseline of extractable MPFs from non-abraded samples, fleece
and interlock textiles without abrasion were also extracted by the Gyrowash lab washing
machine. This set of experiments is indicated as "control-textile" in Table 4-1. Therefore,
together with "control-abrasion", controls at three different levels were conducted to assess
the whole experimental workflow.
89
An additional experiment (i.e. “water wash” in Table 4-1) was performed using the fleece textile
to investigate the extraction efficiency of MPFs and fibrils without surfactant. The experimental
procedure was the same as for the standard abrasion experiment, except that nanopure water
was used to replace LAS solution as the liquid during extraction in the Gyrowash lab washing
machine.
Table 4-1. Summary of the experimental conditions and the different control samples used.
The numbers of the samples for each experiment are summarized in Table A3-3.
Abrasion
Extraction
Experiment Aim Textile Put on the
Abrasion condition
Martindale
conditions
tester
Investigate
Abrasion Fleece, 12 kPa, 5000
MPFs/fibrils formation Yes
experiment Interlock rubs
during abrasion
Determine the
contamination (i.e. 5000 rubs,
Control- from the surroundings, Fleece, samples were
Yes
abrasion and the operation of Interlock lifted to avoid
the Martindale tester) abrasion
1 cycle (45
during abrasion
min) at
40 °C, no
Determine the
steel balls,
baseline of extractable Fleece,
Control-textile No N/A LAS solution
MPFs/fibrils in textile Interlock
samples
Determine the
contamination (i.e.
Control- from the LAS solution
None No N/A
extraction and the steel vessels
for washing) during
extraction
1 cycle (45
Investigate the min) at
influence of addition of 12 kPa, 5000 40 °C, no
Water wash Fleece Yes
surfactant on rubs steel balls,
MPFs/fibrils extraction nanopure
water
90
4.3.4. Image analysis
Filters were sputtered with a 7 nm layer of Au/Pd by a high vacuum sputter coater (LEICA EM
ACE600) before observation under SEM (7 kV, Quanta FEI 650). To determine the number
and length of MPFs and fibrils, the filters were imaged at a magnification of 200 with a
resolution of 1536 x 1024 pixels. A grid of 7 x 10 images (i.e. 70 photos total) were needed to
cover the entire area of each filter, which was achieved by the automatic "mapping" function
of the Quanta FEI 650. The 70 images were subsequently merged after manually checking
and adjusting the position of each image. The complete image had a width of 13.248 mm with
a resolution of 9669 x 9132 pixels (ca. 166 mm2). To determine the diameter of MPFs and
fibrils, a grid of 4 x 5 images (i.e. 20 photos total) were taken at a higher magnification of 500x.
The final image had a width of 3.0673 mm with a resolution of 5582 x 4601 pixels (ca. 8 mm2).
Examples of analyzed images are shown in Figures A3-4 and A3-5. The image analysis was
carried out with ImageJ27. The image captured all MPFs/fibrils in the sub-sample of the
extraction liquid and all MPFs and fibrils on the filters were labeled manually using a Microsoft
surface tablet and a stylus pen. In total, 104 composite images were analyzed, where 2365
MPFs and fibrils were measured to evaluate the number and length and 502 were used to
assess the diameter.
Only fiber fragments with an aspect ratio greater than 3 were counted as fibers, as defined by
the European Chemicals Agency28. Two fiber morphologies were identified. The first type had
a cylindrical shape and are referred to as "MPF" in the text. The second type of fibers had a
"tape-like" shape and had a much smaller diameter. They are referred to as "fibrils". The
detection limit for length was 9-10 pixels at the magnification of 200x, corresponding to 15 µm,
while at the magnification of 500x, the detection limit was 1 µm (4-5 pixels). For the tape-
shaped fibrils, the diameters were determined by measuring the widest part.
Additionally, SEM was used to characterize the surface of the textiles and the fibers protruding
from the textile surface. The same sputtering method was applied as described above. The
textile surface was imaged at a magnification of 100x, while the fiber ends were characterized
at a magnification of 2000x. Fifty fiber ends were randomly imaged to estimate the percentage
of truncated (i.e. solid ends) and fibrillated ends (i.e. fiber ends with axial fiber splitting at the
end). Images at different magnification (i.e. 500x, 2000x, 10,000x) were taken by SEM to
better characterize the fiber fragments. The percentage of truncated and fibrillated ends were
estimated by randomly imaging 50 fiber ends at a magnification of 500x.
91
4.3.5. Statistics
A one-way ANOVA test in IBM SPSS software (version 27) was used to determine the
influence of the textile type on the number of extracted MPFs and fibrils. A nonparametric
Kruskal−Wallis (K−W) one-way ANOVA test in IBM SPSS software (version 27) was used to
compare the distribution of length and diameter in the following groups: (1) with abrasion and
without abrasion; (2) different samples: apparatus, specimen and abradant; (3) with and
without addition of surfactant. A p-value of less than 0.05 was considered statistically
significant.
4.4. Results
4.4.1. Assessment of the methodology
The ISO standard was not designed to capture released fibers and therefore various tests
were performed to evaluate the suitability of our adapted methodology. The possibility that
MPFs and fibrils escaped the enclosure around the abrasion stand was evaluated by analyzing
double-sided carbon tape placed at different positions on the ring. On average 4 ± 4 MPFs
and 1 ± 1 fibrils were observed at the bottom of the ring, while 0 to 1 MPFs or fibrils were
observed at the upper side of the ring (Table A3-4). Therefore, it can be assumed that the
majority of MPF generated were contained and collected within this system and did not escape.
To optimize the extraction method, an experiment was carried out to assess the influence of
the surfactant on the extraction of MPF and fibrils after abrasion (Figure A3-6, Tables A3-5
and A3-6). The number of MPFs and fibrils extracted from abraded textile samples with pure
water was only 120 ± 32 MPF and 140 ± 40 fibrils per g textile, which was approximately 20
and 40 times lower than by extraction with LAS. There was no significant difference (p-value
of 0.52, Table A3-7) observed between the length distribution of MPFs extracted with LAS
(median: 290 µm) and water (median: 229 µm). LAS tended to extract significantly shorter and
thinner (p-value of 0.000, Table A3-7) fibrils (length: 56 µm; diameter: 2.4 µm) than water
(length: 99 µm; diameter: 3.0 µm). Therefore, LAS was chosen to extract the MPFs and fibrils
from textile samples.
MPFs and fibrils collected from the apparatus, specimen and abradant were first separately
analyzed for number, length and diameter. To better compare the number of fibers extracted
from different samples, the absolute values are shown in Figure A3-7, while the number
normalized to the mass of the textiles are shown in Table A3-8. The absolute number of MPFs
92
collected from the apparatus (fleece: 1700 ± 843; interlock: 2900 ± 910) was about more than
one thirds (fleece: 37%; interlock: 64%) compared to the one extracted from specimen and
abradant. These results show that it is important to include the fibers deposited on the
apparatus in the counting of fibers. In terms of the length distribution (Figure A3-7, Table A3-
9), the MPFs and fibrils collected from the apparatus usually demonstrated a significantly
longer length (p-value of 0.000, Table A3-11) than those extracted from specimen and
abradant (e.g. fibrils from fleece: 453 µm for apparatus, 57 µm for specimen and 53 µm for
abradant). There was no significant difference of the diameter between MPFs collected from
apparatus, specimen and abradant (Table A3-10, Table A3-11). The diameter of fibrils
collected from different samples was also similar, except for interlock where significantly
thicker fibrils (p-value of 0.000, Table A3-11) were found on the apparatus than in the textile
samples (Figure A3-7, Table A3-10). In the later analysis, the MPFs and fibrils collected from
apparatus, specimen and abradant were combined.
Several measurements were performed to assess the contamination and the reliability of the
extraction and analytical procedures. To quantify the contamination during the extraction step,
14 blanks were assessed and indicated as "control-extraction" in Table 4-1. The level of
contamination was 0 to 2 ± 1 MPFs per 150 ml and 0 to 8 ± 6 fibrils per 150 ml depending on
the set of experiments. The baseline of extractable MPFs or fibrils in textile samples was
determined by analyzing the number of MPFs and fibrils extracted from textile samples without
abrasion (“control-textile”), which was 410 ± 230 MPFs and 31 ± 16 fibrils per g textile for
fleece and 69 ± 36 MPFs and fibrils below the detection limit for interlock. The detection limit
considered here for fibrils was calculated as the mean of the blanks (“control-extraction”) plus
three times the standard deviation, which was 26 fibrils per g textile for interlock fabric. The
baseline value shows the amount of MPFs or fibrils present in textile samples before abrasion.
The MPFs and fibrils originated from this source accounted for about 20% and 0.51% for
fleece, and 3.1% and 0% for interlock. For "control-abrasion", the contamination of the
apparatus (steel sample holder, ring, and rubber overlay) was 0 MPFs and 5 ± 4 fibrils during
the whole abrasion period. The MPFs and fibrils found in the control-abrasion samples
(abradant and specimen) were 590 MPFs and 160 fibrils per g textile for fleece, and 87 MPFs
and 100 fibrils per g textile for interlock. The contamination during abrasion (the difference
between the number of extracted MPFs or fibrils from "control-textile" and "control-abrasion")
accounted for about 8% and 2% of those found in the abraded samples for fleece (2100 ± 930
MPF g per textile; 6000 ± 2700 fibril g per textile), and about 0.8% and 2% for interlock (2300
± 250 MPF g per textile; 5300 ± 640 fibril g per textile). Therefore, MPFs and fibrils analyzed
from the abraded samples were mainly formed during the abrasion process.
93
To determine the reliability of filtering to achieve precise number of MPF or fibrils measured,
three aliquots from the same extraction solution were analyzed as shown in Figure A3-8, Table
A3-12. The majority of the samples demonstrated a relative standard deviation below 15% (4
– 14%), except for the release to apparatus for the fleece samples (MPF: 26%; fibril: 44%).
Considering the small size of the filter required for SEM analysis which limited the number of
analyzed MPFs (average of 23 ± 15 MPFs and 43 ± 51 fibrils per filter), the results showed
that the subsamples were representative for the number of MPFs and fibrils and the results
obtained by the chosen workflow were reproducible. Moreover, all experiments were carried
out in three replicates. The relative standard deviation of MPF and fibril number ranged from
7 to 100% with an average of 38%.
4.4.2. Characterization of abraded textiles and fiber fragments
The change of the surfaces after abrasion of the fleece textile samples can be observed from
SEM images (Figure 4-1A and 4-1B). The surface of the textile without abrasion was fuzzy,
while aggregations of fibers were observed on the surface of the abraded textile. When
imaging the ends of fibers protruding from the surface of the textiles at a higher resolution, all
randomly selected fibers from the non-abraded sample had truncated ends (Figure 4-1C). For
the abraded samples (fleece, specimen), fibers with truncated ends also accounted for the
majority of fibers observed (about 90%), but approximately 10% of the fibers had fibrillated
ends (Figure 4-1D), where a number of tiny fibrils protruded from the end of the fiber. These
types of fiber ends were not observed in the non-abraded samples.
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Figure 4-1. Characterization of the fibers of the surface of fleece. The images on the left show
the non-abraded sample, on the right side the images show the abraded sample (12 kPa,
5000 rubs): (A) surface of fleece textile, non-abraded; (B) surface of fleece textile, abraded
specimen; (C) solid fiber ends of fleece textile, non-abraded specimen; (D) fibrillated fiber ends
of fleece textile, abraded specimen. SEM images were taken under 7 kV, the magnification for
(A) and (B) was 100x, for (C), (D), it was 2000x. The scale bars in figure (C) and (D) apply to
all the four small images. Similar images for the interlock sample are displayed in Figure A3-
9.
The MPFs and fibrils extracted from the samples were characterized by SEM (Figure 4-2). All
MPFs extracted from the non-abraded fleece textile demonstrated truncated ends, while fibrils
were rarely observed (Figure 4-2A). For abraded samples, the number of extracted fibrils was
much higher than the number of MPFs (Figure 4-2B), and both MPFs with solid ends and
fibrillated ends could be observed. The MPFs with solid ends were identical to those found in
non-abraded samples (Figure 4-2C) and accounted for the majority (>95%) of the fibers found
from abraded fleece. A small portion (<5%) of MPFs demonstrated fibrillated ends (Figure 4-
2C) and this feature was the same than the fibrillated fiber ends observed on the textile surface
(Figure 4-1D). Fibrils were further characterized at a higher magnification of 10,000x (Figure
4-2D). It can be seen that fibrils possessed a tape shape and had much smaller diameter
(about 2 µm) than the fibers (about 12 µm).
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Figure 4-2. Characterization of MPFs and fibrils extracted from fleece: (A) MPFs extracted
from non-abraded fleece textile at a magnification of 2000x; (B) MPFs and fibrils extracted
from abraded fleece textile at a magnification of 500x; (C) MPFs and fibrils extracted from
abraded fleece textile at a magnification of 2000x; (D) MPFs and fibrils extracted from abraded
fleece textile at a magnification of 10,000x. The scale bars in figure (A), (C) and (D) apply to
all the nine small images. Similar images for the interlock sample are displayed in Figure A3-
10.
The number of MPFs and fibrils contained in the textiles after abrasion was quantified in the
extraction solution. The number of MPFs extracted from fleece and interlock after abrasion
was 2100 ± 930 and 2200 ± 250 MPFs per g textile, which is 5 and 30 times higher than the
number of MPFs extracted without abrasion (Figure 4-3A and 4-3D). In non-abraded samples
almost no fibrils were detected. In particular for interlock, the number of fibrils was below the
detection limit of 26 fibrils/g for non-abraded samples and rose to 5300 ± 650 fibrils per g
textile after abrasion. For fleece, the number of fibrils increased approximately 200 times from
31 ± 16 fibrils per g textile before abrasion to 6000 ± 2700 fibrils per g textile after abrasion.
The number of total MPFs and fibrils extracted from the non-abraded interlock sample was
more than 5 times lower than the MPF extracted from the non-abraded fleece textile. However,
the number of MPF extracted from both types of textiles was not significantly different after
abrasion (p-value of 0.49 for MPF, and 0.68 for fibril, Table A3-13, A3-14, A3-15).
96
The length distribution of the MPFs is displayed in Figure 4-3B and 4-3E as notched box plots.
Overlapping notches of two boxes strongly indicate (95% confidence) that the median of two
distributions is not significantly different29. For fleece, significantly longer MPFs were extracted
from the abraded sample (p-value of 0.000, Table A3-20; median length of 290 µm) than MPFs
extracted from non-abraded samples (median length of 239 µm), which was opposite to the
trend observed for fibrils (abraded: 56 µm; non-abraded: 143 µm; p-value of 0.000, Table A3-
20). For interlock, significantly shorter MPFs (p-value of 0.000; median length of 332 µm) were
extracted from abraded samples than from non-abraded samples (median length of 632 µm).
For both fleece and interlock, fibrils had a length which was 2 to 4 times smaller than the one
of the MPFs.
The average diameter of the MPFs extracted from abraded samples was 11.8 and 12.9 µm
for fleece and interlock, respectively (Figure 4-3C and 4-3F) which were similar to the ones
observed within the textiles (12.3 ± 2.1 for fleece and 12.7 ± 1.5 for interlock) and there was
also no significant difference between the MPFs extracted from abraded and non-abraded
samples (p-value of 0.04 for fleece and 0.08 for interlock, Table A3-20). Compared to MPFs,
fibrils had much smaller diameters: 2.4 µm for fleece and 4.9 µm for interlock. Significantly
thinner fibrils were found to be extracted from the abraded fleece (diameter of 2.4 µm) than
from the non-abraded samples (diameter of 2.8 µm, p-value of 0.000).
97
Figure 4-3. Number and distribution of length and diameter of MPFs and fibrils extracted from
fleece and interlock textiles with and without abrasion. The length and diameter distribution
presented here are a summation of triplicate experiments. For length distribution, the number
of MPFs or fibrils counted per sample was between 13 and 835, with an average of 299. For
the diameter distribution, the number of MPFs or fibrils plotted per sample was between 9 and
156 (Table A3-21), with an average of 67. 25th and 75th percentiles are represented by the
boxes and the median is indicated by a line. The number of extracted MPF and fibrils is
normalized to the mass of the textiles. n.d. refers to "not detected". The numerical values
shown in the plots are given in Tables A3-16 to A3-19 in the supporting information (SI).
4.5. Discussion
Microplastic in air is ubiquitous and therefore a careful examination of possible cross-

contamination during sample handling is needed by carrying out various control experiments.
In our experiments, the contamination during abrasion contributed a very small amount of
MPFs and fibrils to those extracted from the abraded samples (MPF: 0.8-8%; fibril: 2%)
suggesting that the interference from this source was under control. The contamination during
extraction also contributed negligible amounts of fiber fragments (less than 0.1%) in the later
analysis. Although the interference from production-inherited MPF/fibrils in the textile samples
could not be fully eliminated, the assessment shows that the majority of the MPFs (fleece:
71%; interlock: 97%) and fibrils (fleece: 96%; interlock: 98%) extracted from the abraded
samples was formed during the abrasion process.
98
The abrasion process may affect the MPF extracted from synthetic textiles in two ways. Firstly,
previous work has shown that MPF can already be contained in some textiles and likely
originate from high-energy processes during textile manufacturing18, 20. MPFs are found to be
present in various textile products before the use phase20. Processes that induce fiber
breakage can be determined by characterizing the fiber end morphology, where high-energy
cuts usually result in solid fiber ends without splits21, 30. The production-inherited MPFs often
demonstrated solid ends similar to those generated by high-energy cut18. In this case, the
increase of MPF extracted from textiles after abrasion is likely due to the mobilization of MPF
from the textile structure. Most of the MPFs (>95%) extracted from abraded samples were
found to have similar ends to those found from non-abraded samples and they are
representative for fiber ends formed during high-energy cuts (e.g. scissors, knife). Therefore,
the fraction of the MPFs with solid ends collected from the abraded samples was unlikely
formed during the abrasion process but was liberated by the abrasion from within the yarns or
the textile structure.
Compared with MPFs formed by high-energy cuts, abrasion often leads to fiber fatigue and
fibrillation, resulting in the formation of much thinner fibrils21. MPFs with fibrillated ends and
fibrils with shorter length and smaller diameter were extracted from the abraded textile
samples, while the fibrillation of fibers was also observed at the textile surface after abrasion.
A small number of fibrils were found in the non-abraded fleece, but for the interlock textile, the
number of fibrils found for the non-abraded sample was below the detection limit. Therefore,
it is unlikely that the washing process is responsible for the generation of fibrils, because only
a very limited amount of fibrils was found in non-abraded samples which also went through
the washing process. It cannot be excluded that a small amount of fibrils may have been
formed during the textile manufacturing process and were already contained in the fabric
similar to the MPF. Fleece textiles are known for their fuzzy texture, which is usually generated
by a shearing process where surface fibers are cut31, 32 and this process may be responsible
for the small amount of fibrils already contained in the fabric before abrasion.
The number of MPFs extracted from the non-abraded interlock sample was higher than for
fleece, but after abrasion, the number of MPFs extracted from both types of textile was about
the same. Many studies investigated the factors affecting MPF release from different synthetic
textiles during washing18, 24, 26, 33-43
. MPF release from textiles has been reported to be
influenced by textile properties including the type of yarns, surface treatment and edge
treatment24, 26, 33-37, 40-42. A recent study also investigated the influence of finishing treatment
on fiber release from cotton textiles during washing44, where the results show that the
mechanical properties of fibers play an important role. Softer fabrics tended to form more fuzz
99
and release more fibers44. The application of softener to cotton textile can also reduce the fiber
brittleness and increase abrasion resistance, resulting in the release of longer fibers44. But the
influence by softener on polyester textiles still needs to be investigated, since polyester is
hydrophobic, which may absorb much less softener than cotton. Further systematic research
is also needed to understand how those textile properties can influence the MPF release after
abrasion because only two different fabric types were used in this work.
There are several limitations of this study that need to be considered. Firstly, the Martindale
tester can only simulate a very limited daily application scenario of textiles such as sitting and
moving with clothes on a chair and sofa over a prolonged period. Thus, the results obtained
from the experiment describe the potential of MPFs and fibrils to be generated during several
years of use. Further research needs to establish the influence of parameters such as the
number of rubs and the level of pressure on fibril formation during abrasion. Secondly, in our
abrasion tests, the specimen and the abradant were fixed on the sample holders and they
were always in close contact to each other, which may hamper the release of fibers to the
surrounding environment. To simulate a more realistic scenario, a chamber study needs to be
conducted by volunteers wearing aged garments and establishing if under these conditions
also a bimodal size distribution is obtained.
So far, the presence of fibrils and the bimodal size distribution of fiber fragments released from
textiles has not been reported in textile release studies or in monitoring studies in the
environment. The length of the fibrils formed during abrasion was shorter than the MPFs
detected in aquatic and terrestrial systems, where the length of detected MPFs ranged from
500 to 1000 µm45. Compared to microplastics in soil and water, the majority of MPFs found in
air demonstrate a size below 500 µm14. A study investigated the occurrence of MPFs in urban
air in Beijing, where MPFs with a size below 20 µm were reported to be the dominant types of
airborne fibers15. The size of MPFs in surface dust was found to be a bit longer than the
airborne fibers with a major size between 25 - 200 μm15, which is in accordance with the length
of fibrils reported in our study.
A fraction of the airborne MPFs with smaller size are believed to be inhalable46, 47 and may be
persistent in the lung and cause a biological response such as inflammation48-50. Compared
to the longer MPFs, the fibrils with smaller size may raise more human exposure issues. The
transport of particles in air is determined by their aerodynamic behavior which depends on the
aerodynamic diameter 51. For stiff fibers, the diameter or width of fibers plays the central role
controlling the aerodynamic diameter and subsequently the pulmonary deposition52, 53, while
the length was reported to have little impact on fiber deposition in lungs53. Although the fibrils
discovered in our study have an average diameter between 2 and 5 µm, it is difficult to estimate
100
the aerodynamic diameter of fibrils. The fibrils can demonstrate a high degree of curvature
and flexibility compared to (comparatively more) stiff MPF. Further studies are needed to
investigate the aerodynamic behavior and the penetration of fibrils to the lower respiratory tract
and the subsequent potential health hazards. It should be noted here that if the mechanism of
toxicity is merely a consequence of inhalation of fine particles, the fibrils generated from
synthetic textiles would not necessarily be more hazardous than those from natural fibers
which may be easier to be broken down to smaller pieces than those of synthetic origin. It is
therefore necessary to also include natural fibers such as cotton into further studies about the
release and hazard of fibrillated fibers.
In terms of the ecotoxicity of MPFs, a recent review by Bucci, et al.54 has analyzed the data
from 139 studies investigating the ecotoxicological effects by plastic debris, and the results
show that the shape of the particles is an important factor affecting the effects of microplastic.
The observed effects ranged from no effects55, effects at cellular level (e.g. mucosal damage,
inflammation, metabolism disruption)56 and effects at sub- and organism level (e.g. longer
egestion times, reduced growth, mortality)57-59. Some studies compared the toxicity of MPFs
with microplastics with other shapes, and MPFs were found to be more toxic to shrimp
(Palaemonetes pugio)58 and a crustacean (Hyalella azteca)57 than spheres and fragments,
respectively. Fibers were also found to cause higher degree of intestinal damage after
ingestion by zebra fish than beads and fragments56. The size of MPFs is also reported to play
a role in the toxicological effects to organisms, where studies show that longer fibers are more
toxic to shrimp58 and zebra fish60. However, the fibers used in those studies had a diameter of
20 µm which is much larger than the diameter of fibrils found in this study. Microplastics with
smaller size are reported to exert more likely effects54, since smaller particles are more
bioavailable61 and easier to translocate across the gut/extracellular barrier62. Therefore, the
fibrils with much smaller size and diameter may also have different ecotoxicological effects on
aquatic and terrestrial organisms than MPFs, which needs to be carefully assessed in the
future.
We would like to thank Manfred Heuberger from Empa for the valuable feedback and
discussion. This research was partially supported by funds from the Zürcher Stiftung für
Textilforschung. D.M.M. was supported by the Swiss National Science Foundation grant
numbers PZP002_168105 and PCEFP2_1
101
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5. Country-Specific Environmental Risks of Fragrance
Encapsulates Used in Laundry Care Products
Reprinted from the accepted article: Cai, Y., Lin, J., Gimeno, S., Begnaud, F., & Nowack, B.
(2021) Country-specific environmental risks of fragrance encapsulates used in laundry care
products. Environmental Toxicology and Chemistry.
5.1. Abstract
Fragrance encapsulates (FEs) are designed to deliver fragrance components notably in

laundry care products. They are made of thermoset polymeric shells surrounding the fragrance
content. These materials enter the environment mainly during laundry washing, but little is
known about their distribution in and impact on the environment. The aim of this work was to
estimate the environmental concentrations of FE shells in freshwater, sediment and soil
compartments for 34 selected countries and to compare them with ecotoxicological effects.
Probabilistic material flow analysis was used to estimate worst-case predicted environmental
concentrations (PECs). The lowest water concentration was predicted for Finland (0.0001
µg/L), the highest for Belgium (0.13 µg/L). Accumulation of FE shells between 2010 and 2019
was considered for sediment and sludge-treated soils. The PECs in sediments ranged from
3.0 µg/kg (Finland) to 3400 µg/kg (Belgium). For sludge-treated soil, the concentration was
estimated to be between zero (Malta and Switzerland) and 3600 µg/kg (Vietnam).
Ecotoxicological tests showed no effects for FE shells at any tested concentration (up to 2700
µg/L water, 5400µg/kg sediment and 9100 µg/kg soil), thus not allowing to derive a predicted
no effect concentration (PNEC). Therefore, to characterize the environmental risks, the PEC
values were compared with Highest Observed-No-Effect Concentrations (HONECs) derived
from ecotoxicological tests. The PEC/HONEC ratios are 9.3 x 10-6, 0.13 and 0.04 for surface
waters, sediments and sludge-treated soils, which are much below one, suggesting no
environmental risk. As the PEC values constitute an upper boundary (no fate considered) and
the HONEC values a lower boundary (actual PNEC values based on NOECs will be higher),
the current risk estimation can be considered a precautionary worst-case assessment.
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5.2. Introduction
Microplastics are a class of pollutants, defined as plastic particles with a size between 0.1 µm
and 5 mm or plastic fibers possessing a length between 0.3 µm and 5 mm with a length to
diameter ratio above 3 1. These materials have drawn a tremendous amount of attention in
the last few years2. Depending on their origin, microplastics can be categorized into primary
and secondary microplastics1, 3. Primary microplastics are defined as those which are
intentionally manufactured into particles with size of 5 mm or less, such as scrubbers,
microbeads, and plastic powders3, 4 but they are accounting only for a small part (less than
10%) of microplastics found in the environment1. Secondary microplastics are the result of the
breakdown of larger items, such tire abrasion, fibers from textiles and fragments from
weathering processes of plastic packaging products3, which are the major form of
microplastics found in the environment1.
The use of fragrances have endured throughout the centuries and various benefits of
fragrance have long been recognized5, 6. Fragrances are widely used in consumer goods such
as laundry, home and body care products. Since many of the fragrance components are
volatile and some prone to degradation7, 8, fragrance encapsulates (FEs) were designed to
provide long lasting experience notably in laundry care products. They are mainly used in
liquid fabric softeners, with additional benefits of preventing fragrance components from
physical and chemical losses such as evaporation and abiotic degradation processes7, 8. FEs
are spheres with a typical diameter between 5 to 50 µm and a wall thickness below 1 µm 9
containing the fragrance components. FE shells are often made of cross-linked thermoset
melamine-formaldehyde polymer. FE shells can also consist of other cross-linked thermoset
polymers such as polyurethane, polyurea and polyamide, but to a lesser extent10. Diverse
chemistries are employed in the preparation of polymeric FEs involving phase separation
polymerization, interfacial polymerization or both7, 11, 12. Most of the microplastics found in the
environment are the thermoplastic polymers13. Although thermoset polymers and
thermoplastic have different properties, ECHA14 considers FE shells as intentionally added
microplastics. FEs are manufactured mainly by fragrance and consumer goods companies
and the annual release of FE shells was estimated to be 200 t (130 – 275 t) in Europe14. After
the use of FEs in laundry care products they will most likely enter into the environment with
the wash water and after passage through a sewage treatment plant. It is therefore crucial to
understand the environmental fate and effects of these materials.
Considering the data available for MPs in wastewater treatment plants, only about 10% of the
FE shells are expected to be released into surface waters because the major fraction of
microplastics (~90%) is removed by sorption to the sludge during wastewater treatment 15, 16.
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Since sludge is commonly used as fertilizer and more than 50% of the sludge is applied on
agricultural soil in Europe and North America17, a large fraction of FE shells are likely to end
up in soils. So far, there is no study available identifying the occurrence of FEs in
environmental samples. Although the release of FEs shells is insignificant when compared to
the total volume of microplastics (42 000 tons per year) released in Europe18, representing
less than 0.03% of the MPs, the environmental fate of these materials should be addressed
to provide guidance for the development and selection of ecofriendly FEs.
Since microplastic measurements are often spatially inhomogeneous and the information for
certain environmental compartments (e.g. soil) is limited, modeling can be a valuable
substitute to estimate the exposure level of microplastics in the environment. A recent study
using probabilistic material flow analysis (PMFA) quantified the mass flows of macro- and
microplastics released from a large variety of products to the environment19. The emission of
macroplastics to freshwater and soil in Switzerland was estimated to be 109 and 4400 t/y
respectively, which was about 7 times higher than the emission of both primary and secondary
microplastics (freshwater: 15 t/y; soil: 600 t/y)19. Construction pipes (137 t/y), agricultural films
(114 t/y) and post-consumer processes (e.g. littering) (89 t/y) ranked the three largest sources
of microplastics in soil, while for microplastics in freshwater, littering (3.6 t/y), clothing fibers
(3.1 t/y) and microbeads in personal care products (2.6 t/y) were the biggest contributors 19. It
should be noticed that in the meantime microbeads in personal care products have been
banned in several countries and won’t be a source of microplastic anymore20.
Ecotoxicity of microplastics has been investigated for both aquatic and terrestrial organisms3,
21-23
. The ecotoxicological effects by plastic debris range from no observed effects to effects
at cellular and organism level24. The greatest concern regarding microplastic pollution is the
risk of ingestion25-28, which can result in several negative effects. There is evidence showing
that ingestion of microplastic fibers by terrestrial snails can result in decreased food intake 29,
while the uptake of microbeads by mussels can lead to inflammation26. Other detrimental
effects such as mucosal damage, longer egestion times and reduced growth have also been
reported30-32. However, it should be noted that often unrealistically high concentrations were
applied in some experiments, which raises questions about their environmental relevance33.
Currently, only a very limited number of risk assessments of microplastics has been published
in the peer-reviewed literature34-37. The predicted no-effect concentration (PNEC) for
freshwater was calculated based on species sensitivity distributions (SSD) to be 4.2 x 10-2
µg/L34. The PNEC was obtained by considering all types of microplastics spheres, fragments,
and fibers tested in toxicological experiments with a size mainly between 0.1 to 1000 µm. The
risk assessment showed that only a very small percentage (0.12%) of the probability
110
distribution calculated for the global risk characterization ratio was above one34. However, the
study by Adam, et al.34 provides a generic risk assessment for all types of microplastics without
distinguishing between the polymer types. The environmental risks posed by FEs made of
thermoset polymers have so far not been quantified.
The aim of this work was to estimate the environmental exposure levels of FE shells in
freshwaters, sediments and soils for 34 selected countries and to compare the environmental
concentrations with ecotoxicological effects. A probabilistic material flow analysis (PMFA)
model38 was applied to estimate the flows of FE shells to the environment and to obtain the
predicted environmental concentrations (PEC). Ecotoxicological tests with FE shells were
conducted to measure potential effects on freshwater, sediment and soil organisms. Finally,
the environmental risk was characterized by comparing the PEC values to ecotoxicological
threshold values.
5.3. Methods
5.3.1. Material flow model description
A PMFA model was programmed on the platform R39, based on the basic PMFA algorithm by
Gottschalk, et al.38. The model was developed to assess the mass flows of anthropogenic
materials to the environment through their complete life cycle, from production, manufacturing
and use to the end-of-life (EoL) management and the release to the environment. The model
was adapted and parameterized for FE shells (Figure 5-1). The release during FE production
and laundry care products manufacturing was estimated to be less than 0.1% of the total
production and was not considered here. The assessment was performed at a national scale
for 34 selected countries including EU 27, UK, Switzerland, Norway, USA, Mexico, Japan and
Vietnam, where FEs are used in laundry care products. These countries were selected
because of their specific habits representing various continents (surrogates for consumer habit,
infrastructure and release). In some countries a large portion of the grey wastewater is directly
discharged to the environment. Four waste treatment processes are generally present:
wastewater treatment plants (WWTP), incineration, landfilling, and recycling. FE shells as
organic material ultimately decompose to water and carbon dioxide at a high temperature,
therefore FEs flowing into incineration plants are eliminated, which also applies to FE shells
contained in sludge that is incinerated. The landfill was considered a final sink for the scope
of our model. The presence of microplastics in leachates of municipal solid waste landfill has
been confirmed in China (0.42 to 24.58 items/L) and Nordic countries (0-0.17 µg/L for treated
leachate)40, 41, but the correlation of the total amount of microplastics landfilled compared to
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the amount leached is unknown. Since recycling solely applies to the plastic containers where
the laundry care products are contained in, the flows of FE shells out of plastic recycling was
considered as waste water based on the model by Rajkovic, et al.42. A small fraction of the
laundry care products (including FE shells) remains in the containers and is removed in
washing steps during recycling. Three environmental compartments were included in the
model: surface water, sediment and soil. For soil, only the concentration in sludge-treated soil
was considered as no pathways onto other soil type were included in the model and because
sewage sludge is widely used in many countries as organic fertilizer17. The use of grey water
for soil irrigation was not considered due to lack of data.
Figure 5-1. Definition of the system. The system boundary was outlined by the red dashed
line. Sinks are labeled as grey boxes. WWTP represents wastewater treatment plant.
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5.3.2. Input parameters
Production, manufacturing and consumption volume
FEs are a technology to protect fragrance components from evaporation and degradation43
and are reported to be mainly used in laundry care products20. According to sales data, more
than 95% of the FEs are used in laundry detergents and fabric softeners. Of the total EU
market, approximately 10 – 20% of laundry detergents and about 60% of fabric softeners
contain FEs, while less than 1% of deodorants and other cosmetic, personal care and cleaning
products contain FEs9. In the model, we therefore assumed all of the FEs were used in laundry
care products.
The total mass of FE shells released in Europe for the year of 2019 was calculated by ECHA
according to the information reported by industry14. The mass released in each European
country was estimated from the total mass released in Europe and the relative retail volumes
of fabric softeners in European countries obtained from Euromonitor International44, since
fabric softener is the main application for FEs. For the other four countries outside Europe
(USA, Mexico, Vietnam and Japan), the mass of FE shells released was calculated based on
the country-specific release mass of one of the major manufacturers and the estimated market
share of the manufacturer (Table A4-1). A triangular distribution was introduced into the model
to address uncertainties of the release volume. The mode, minimal and maximum values of
the distribution were defined as the mean, the lower and upper boundaries provided by the
original dataset. For the four non-European countries where only the mean value was
available, an uncertainty of 50% was assumed as the width of the distribution.
To assess the accumulation of FE shells over the years in sediments and soils, the historic
releases of FE shells were estimated. The releases from 2010 to 2019 were scaled from either
the global (for EU27, UK, Norway and Switzerland) or country-specific (for US, Mexico, Japan
and Vietnam) FE shells consumption trends shown in Table A4-2. These trends were
calculated based on technical data, sales and estimated market shares of one of the major
manufacturers. Since the market of FEs was only well established after the year 2015, an
additional uncertainty of 5%/year was applied to all countries for the years starting from 2015
backward. The uncertainty increased with the distance of the year to 2015 by 5% (i.e. 5% for
2015, 10% for 2014)
Transfer coefficients
Transfer coefficients describe the distribution of product flows at all life-cycle stages,
depending on the product application. Softeners containing FEs are used during washing and
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95% of FEs in softeners were assumed to flow to the wastewater. The other 5% of FEs were
assumed to remain in the package and to be discarded as solid waste42. The WWTP removal
efficiency of FE shells was estimated based on the removal efficiency of microplastics. The
selection of studies was based on two high-quality reviews published recently45, 46, where the
removal efficiency from 81 WWTPs around the world were listed based on 26 publications
(Table A4-3). The removal efficiencies range from 35% to 99% with an average of 90%. A
distribution was constructed by randomly sampling from the 81 collected values. The other
transfer coefficients at the EoL stage were either obtained from Eurostat, OECD and EEA
databases for European countries or from the literature for the four non-European countries
(USA, Mexico, Japan and Vietnam) (Figure A4-1 to A4-3, Table A4-4 to A4-9). Data from the
latest years was always preferred in the data collection. Similar to the consumption volume, a
distribution was introduced to reflect the uncertainties. A triangular distribution was applied for
other transfer coefficient, where the mode of the distribution was defined by the value collected
from databases or literature, while an uncertainty of 50% was defined as the width of the
distribution.
Volume of environmental compartments
To predict the environmental concentration in surface water, sludge-treated soil and sediment,
volumes of each compartment were collected for all countries considered in the model. The
area of the surface water was obtained by averaging the inland water area for each country
from the "land use" and "land cover" databases from FAO47, 48 (Table A4-10). The sediment
area was assumed to be equal to the area of surface water. The area of sludge-treated soil
was obtained by dividing the sludge volume in each country (Table A4-11) with the average
sludge application rate (5000 kg/ha)49, To calculate the volumes of the environmental
compartments, the depth of water, sediment and soil was taken as suggested by the REACH
guidance49. For freshwaters, a residence time of water (40 days) was applied as suggested
by ECHA49.
Worst-case scenarios were used to estimate PEC values excluding any possible fate
processes in the environment: 1) for freshwater, complete suspension of the FE shells was
considered (conservative scenario without any removal processes); 2) for sediment, complete
sedimentation of FE shells from surface water was considered; 3) for soil, no biodegradation
or other degradation reactions were considered and only accumulation of FE shells was
modelled. All compartments were assumed to be homogenous and well-mixed. The
concentration for freshwater was predicted from a static model that only considered the
114
release in the year of 2019. For sediments and soils, a dynamic approach was used to
estimate the concentration considering the accumulation of FE shells from previous years
(2010-2019). This dynamic modeling was based on the approach developed by Gottschalk, et
al.50. 100,000 iterations of models were run to obtain a probabilistic distribution of PECs.
5.3.3. Hazard assessment
Ecotoxicological experiments were carried out at Fraunhofer Institute for Molecular Biology
and Applied Ecology (Germany) and the detailed information can be provided upon request.
The tests were conducted for 10 species in freshwater, sediment and soil using two types of
FE suspensions. Typical melamine-formaldehyde fragrance-delivery systems used in laundry
care products was used to prepare the test material. A protocol for preparing such a FE
suspension at a lab scale has been reported by Gasparini, et al.10
Test material
Fragrance encapsulations utilized in consumer products are sold as a slurry that contains the
encapsulations suspended in water plus additives (less than 5%) such as colloidal stabiliser,
deposition aid-materials and preservatives. Encapsulations are thermoset polymers forming a
shell of a thickness generally well below 1 µm surrounding a liquid fragrance droplet (total
average diameter from 10-25 µm). The shells are designed so that the contained fragrance is
released by the action of friction or pressure which will rupture the shells. Since the test
material of interest is one composing the polymeric shells, a protocol was developed to remove
the fragrances and the additives from the capsules 10. The protocol consisted of several steps
of drying, grinding and extraction by organic solvents or water. The resulting purified and
ground test material was light yellow fine powder of roughly sphere particles. The diameter of
the particles was around 1 µm and the density of the powder was estimated by
ultracentrifugation to be 1.3 to 1.4 mg/L. The test materials were therefore a suspension of FE
shells in water with (commercial) or without additives (purified).
Ecotoxicological tests
Rangefinder tests were first performed with the commercial suspension of FE shells. The
ecotoxicological tests were conducted following either the OECD 201 (Algal Growth
inhibition test with Raphidocelis subcapitata), 202 (Daphnia magna immobilization), 236
(zebrafish embryo, Danio rerio), 209 (sediment test with the sediment dweller, Lumbriculus
variegatus), 208 (plant growth inhibition with 4 species, ie. oat (Avena sativa), corn (Zea
mays), bean (Phaseolus aureus) and turnip (Brassica rapa), 217 (soil microbial carbon
115
transformation) and 222 (worm reproduction test with the earthworm Eisenia andrei) and ISO
15685 (soil microbial nitrogen transformation). The soil used was Hagen AM 2013 (loamy
sand [US, DIN], 73% sand, 22% silt, 5 % clay and 1.1% Corg, 1.2 g N/kg). The soils were pre-
loaded with test material at a concentration of 0.5 to 5.35 mg FE shells per kilogram soil.
When any adverse effects were observed, the test was repeated with a broader range of
concentrations and with a purified suspension of FE shells, thus without additives to rule out
their potential effect. Both suspensions had a concentration of 5.35% FE shells. An overview
of the tests with test duration and end point is given in Table 5-1.
116
Table 5-1. Overview of ecotoxicological tests.
Concentration range
FE shells
Compartment Guideline Test species Endpoint Duration (mg FE shells /L water
suspension
or /kg soil or sediment)
Raphidocelis
Freshwater OECD 201 Commercial Growth 72 h 0.00535 to 0.0535
subcapitata
Raphidocelis
Freshwater OECD 201 Purified Growth 72 h 0.0535 to 2.67
subcapitata
Freshwater OECD 202 Commercial Daphnia magna Immobilisation 72 h 0.00535 to 0.0535
Freshwater OECD 236 Commercial Danio rerio Survival or growth 96 h 0.00535 to 0.0535
Commercial Lumbriculus
Sediment OECD 225 Mortality and weight 28 d 0.535 to 5.35
variegatus
Soil OECD 217 Commercial Soil microorganisms Carbon transformation 28 d 0.535 to 5.35
Soil ISO 15685 Commercial Soil microorganisms Nitrogen transformation 28 d 0.535 to 5.35
Soil OECD 208 Commercial Avena sativa Growth 14 d 0.535 to 5.35
Soil OECD 208 Purified Avena sativa Emergence, survival and growth 14 d 1.09 to 9.1
Commercial Emergence, post-emergence
Soil OECD 208 Zea mays 14 d 0.535 to 5.35
survival, growth
Soil OECD 208 Commercial Phaseolus aureus Shoot fresh weight 14 d 0.535 to 5.35
Emergence rate, post-
Soil OECD 208 Purified Phaseolus aureus emergence survival and 14 d 1.09 to 9.1
biomass
Commercial Emergence rate, post-
Soil OECD 208 Brassica rapa emergence survival and 14 d 0.535 to 5.35
biomass
Soil OECD 222 Commercial Eisenia andrei Reproduction 56 d 0.535 to 5.35
Reproduction, survival and
Soil OECD 222 Purified Eisenia andrei 56 d 1.09 o 9.1
weight
117
5.4. Results
5.4.1. Exposure assessment
Consumption volume
This work provides the first environmental exposure and hazard assessment of FE shells. It
concerns a material that according to ECHA definition has to be considered as a primary
microplastic. FEs are used worldwide and the consumption of FEs generally increases with
purchasing power parity (PPP) (Figure 5-2). The mean consumption volume of FE shells in the
year of 2019 for European countries range from 0.14 t for Malta to 31 t for Germany with a total
volume of 165 t. Of the four non-European countries, the highest annual release was found for
USA (99 t) followed by Mexico (66 t) and Vietnam (46 t). It is interesting to note that Mexico
and Vietnam consume a considerable amount of FEs, although both countries have much
smaller PPP compared with many countries. The consumption of liquid fabric softeners that
are one of the main uses of FEs is strongly influenced by the laundry care habits of different
cultures.
Figure 5-2. Consumption volume of FEs (tons of shells) versus the purchasing power parity
(PPP) for each country in the year 2019. The PPP was collected from World Bank 51
The historic consumption of FEs between 2010 and 2019 was estimated using the
consumption volume of 2019 (Table A4-1) and the sales trends (Table A4-2). For European
countries, the historic release volumes were estimated from the global sales trend of one major
manufacturer, resulting in a total release of 1249 t over the 10 years. For the four non-European
118
countries, the historic consumption was estimated from country-specific sales trends, and the
cumulative consumption volume was found to range from 249 t for Japan and 693 t for USA.
Since there is no information indicating if all the products were used up within a year, the
assumption was made to equate consumption and release.
Fragrance encapsulate mass flows in 2019
FEs flowed into the system through "production" and were distributed to technical and
environmental compartments depending on transfer coefficients. The mode, mean, Q5 and
Q95 of the distribution were extracted from the probability distributions of each mass flow.
Figure 5-3 shows simplified flow diagrams which give an overview of the differences in the
flows from consumption to the receiving compartments for the different regions/countries. The
relative importance of flows to different compartments varied highly among regions (Table A4-
12). For Europe and USA, the dominant flow was to sludge-treated soil which accounted for
38% (63 t) and 32% (31 t) of the total flows respectively, while for Japan, Mexico and Vietnam,
the mass flowing to the sludge-treated soil was below 10%. On the other hand, the flow to
surface water accounted for 10 to 20% of the total mass released for most of the selected
countries, except for Mexico, where more than 30% of the capsules ended up in surface water.
For Mexico and Vietnam, the flow to incineration plants was zero.
119
120
Figure 5-3. Flow diagrams of fragrance encapsulate shells in Europe (average), USA, Mexico,
Japan and Vietnam in the year of 2019. Unit: tons/year.
Predicted environmental concentration (PEC)
The PEC values of the FE shells were estimated by dividing the aggregated mass flows to the
52
environmental compartments by the mass or volume of the corresponding compartment ,
representing concentrations in well-mixed systems. PECs were estimated for the three
environmental compartments freshwater, sediment and sludge-treated soil. For freshwater,
country-specific PECs were calculated for the year of 2019 as shown in Figure 5-4 and Table
A4-13. The highest concentration was found for Belgium (0.13 µg/L) followed by Malta (0.12
µg/L) and the lowest value was found for Finland (0.00011 µg/L). The European countries had
121
an average concentration of 0.025 µg/L. For the four countries outside of Europe, a relatively
low concentration was found for USA (0.001 µg/L), while for Mexico, Japan and Vietnam, the
values were between 0.026 to 0.047 µg/L.
Figure 5-4. PEC values for FE shells in freshwater for 34 countries based on the flow of 2019.
Accumulation of FE shells was considered for sediment and sludge-treated soil. The PECs
were calculated by dividing the sum of the mass flow over the years from 2010 to 2019 by the
mass of sediment and sludge-treated soil compartments for each country. The PECs are
shown in Figure 5-5, Table A4-14 and A4-15. Similar to surface water, the highest
concentrations for sediment were found for Belgium (3400 µg/kg) and Malta (3300 µg/kg), while
the lowest value was found for Finland (3.0 µg/kg). A mean value of 650 µg/kg was calculated
for the 30 European countries while for the countries outside Europe, the concentration ranged
from 29 µg/kg (USA) to 1500 µg/kg (Vietnam).
For sludge-treated soil, countries including Malta and Switzerland had zero concentration,
since the sludge is not applied on agricultural soil. The highest concentration in sludge-treated
soil worldwide was found for Vietnam (3600 µg/kg). The 30 European countries had an average
PEC of 210 µg/kg for sludge-treated soil. The USA had the lowest concentration (100 µg/kg)
outside Europe, followed by Japan (110 µg/kg).
To explore the contributing factors that may influence the prediction of PECs, we plotted
correlation figures for various parameters including population density, consumption,
122
consumption per capita, percentage of sludge applied on soil, total sludge volume, volume of
sludge applied on soil, area of surface water, sewer connection rate, WWTP treatment rate,
and precipitation. The plots can be found in the Supporting Information Figure A4-4. The
relevant statistics are summarized in Table A4-16. Although some parameters demonstrated
a certain degree of significance, none of the regressions have a R2 larger than 0.5, suggesting
only a poor correlation with single parameters. The PEC values are influenced by multiple
factors at the same time. Therefore, each country has its unique situation and it is not possible
to draw a general conclusion applicable to all countries.
Figure 5-5. PEC values for FE shells in sediment and sludge-treated soil considering
accumulation for 34 countries over the years 2010 to 2019.
123
5.4.2. Hazard assessment
The results from the ecotoxicological tests using the polymeric material of the fragrance
encapsulations are provided in Table A4-17. All the tests met the validity criteria, except the
plant test with oat (A. sativa) due to a low control seedling emergence (63.3% versus the
minimum valid of 70%). Thus, the test was repeated. In most of the range-finder tests, no effect
was observed even at the highest test concentrations. However, the shoot weight of the bean
was reduced at the highest concentration and the worm reproduction was reduced at the
medium and highest concentrations. Therefore the bean test and the worm reproduction test
were as well repeated with a higher number of concentrations and with FEs shells without
additives. In these repeat full tests, no adverse effects were observed and remarkably plant
growth was promoted for both the oat and bean at most concentrations.
The endpoints from the full tests with the purified FE shell suspensions were preferred in the
hazard assessment to focus on the polymeric materials. Therefore, five of the endpoints from
the three tested environmental compartments were considered to be most relevant to evaluate
the hazard effects posed by FE shells (Table 5-2). Because no effects were observed, NOEC
or EC20 values cannot be provided, but the highest tested concentrations can be used as a
HONEC (highest observed no effect concentration). In the absence of NOEC values, HONECs
have been used to derive PNEC values in a precautionary worst-case approach53. For
freshwater and sediment, chronic HONECs were obtained from tests with algae (Raphidocelis
subcapitata, 2.67 mg/L) and a sediment worm (Lumbriculus variegatus, 5.35 mg/kg). Three
data points tested with three different species were collected for soil. The only chronic HONEC
for the soil compartment is for the earthworm (Eisenia Andrei) with a value of 9.1 mg/kg.
Table 5-2: Most relevant ecotoxicological endpoints of fragrance capsules for assessing their
environmental risks.
Environmental
Species Duration Chronic/acute Descriptor Concentration
compartment
Raphidocelis
Freshwater 72 h Chronic HONEC 2.67 mg/L
subcapitata
Lumbriculus
Sediment* 28 d Chronic HONEC 5.35 mg/kg
variegatus
Eisenia
56 d Chronic HONEC 9.1 mg/kg
andrei
Soil Zea mays 14 d Acute HONEC 9.1 mg/kg
Avena sativa 14 d Acute HONEC 9.1 mg/kg
*Experiment conducted with the commercial suspension.
124
5.4.3. Risk characterization
To characterize the risks for each compartment, the distribution of the PEC values was divided
by the HONECs (Figure 5-6, Tables A4-18 to A4-20). The mean of the PEC/HONEC ratio for
surface water for 34 counties is 9.3 x 10-6 (4.2 x10-8 to 4.7 x10-5), which is several orders of
magnitude lower than 1, suggesting a lack of risk in the environment due to the use and release
of FEs. The PEC/HONEC ratios for sediment were higher than those for freshwater ranging
from 5.6 x 10-4 for Finland to 0.63 for Belgium, with an average of 0.13 worldwide. Sludge-
treated soil had slightly lower PEC/HONEC ratios than sediment with a mean value of 0.04 for
34 countries. Except for those countries that had zero soil concentration due to the lack of soil
application of sludge, the lowest value was found for Denmark and Finland (4.9 x 10-3), while
the highest was calculated for Vietnam (0.39). For some countries such as Belgium and Malta,
there was a small percentage of PEC/HONEC ratios above 1 for sediment (Belgium: 14%;
Malta: 17%).
Figure 5-6. Distribution of PEC/HONEC ratios for 34 countries. Boxes represent 25th and 75th
percentiles of the distribution and a white line in a box indicates the median value. Whiskers
represent 95% of the distribution. Red line notes the ratio = 1.
125
5.5. Discussion
Using material flow analysis, the flows of FEs to each environmental compartment were
determined by transfer coefficients. Relatively high-quality data were available for wastewater
and sludge treatment for European countries, USA and Japan, which means that the data
could be acquired from sources such as Eurostat or peer-reviewed publications. However, for
Mexico and Vietnam, the openly accessible information regarding wastewater management
and sludge disposal was extremely scarce. Although some data could be found, it was difficult
to get information on the complete system. For instance, a report covered wastewater
management in Vietnam, but only the situation in urban areas was addressed54. The urban
population for Vietnam only accounted for 38% of the total population in 201955, which means
information regarding the wastewater disposal for a large region of the country was missing.
Therefore, assumptions had to be made that the sewage connection and the wastewater
treatment rate in rural area in Vietnam were zero. The chosen approach is therefore a
conservative approach resulting in worst-case emissions. Moreover, the sludge is reported to
be not removed regularly from septic tanks and even if it is removed, the illegal dumping of
sludge is a very common practice in Vietnam (ARCOWA 2018). This may also result in a
percentage of FEs released from illegal dumping of sludge into soil and freshwater and this
model does not consider this flow due to limited data. More information is required to obtain a
more accurate prediction.
The fraction of FEs removed from wastewater was assumed to be the same as the one of
microplastics. The available data on the removal of microplastics during wastewater treatment
is covering a wide range from 25 to 5000 µm45, 46. Since the size of FEs is between 5 and 50
µm9, the accuracy of the predicted removal efficiency could be improved if size-dependent
removal efficiencies would be available. Despite the fact that there are many studies reporting
the size of microplastics in WWTPs, not much is known about the removal efficiency for
microplastics with different sizes. For instance, a study by Long, et al.56 reported that
microplastics with smaller size tended to be better removed by WWTP, while the opposite trend
was observed by Magni, et al.57, where the removal efficiency for microplastic with a size
between 5 - 1 mm (94%) was 1.4 times higher than for a size between 0.1 - 0.01 mm (65%).
Therefore, future studies are needed to better understand how the size of microplastics
influences the removal efficiency.
Although there is no other study available addressing specifically the environmental flows of
FEs, efforts have been made to understand the source and release of microplastics into the
environment. A recent study quantified the polymer-specific flows of microplastic to water and
soils for Switzerland19. Compared with the annual flows of microplastics from clothing (3.1 t/y)
126
and personal care products (2.6 t/y) to surface waters in Switzerland, the mass of FE shells
released to Swiss surface waters based on our model is only 0.16 t/y. The released FEs shells
correspond to about 5-6% of microplastics released from clothing or personal care products
and only 1% of the total microplastic emission into surface waters (14.9 t/y) as modeled by
Kawecki and Nowack19. If tires are also considered with a predicted release of micro-rubber
into Swiss surface waters of 1800 t/y58, the contribution of FEs to the total microplastic release
to the environment is marginal. FEs therefore make up only a very small fraction of all
microplastics released into surface water. In addition, the major part of the microplastics found
in the environment are expected to be formed by degradation of macroplastic59 and thus the
contribution of FEs to the microplastic burden in the environment will be even smaller (<<
0.009%).
Using our MFA model, we are able to provide a first estimate of PEC values for FEs but it has
to be kept in mind that they represent a worst-case scenario without considering any
degradation in the environment. The PEC calculation for water assumes that all FE shells
remain suspended in water, the one for sediment that all FE shells in water had sedimented
out of the water column. Both constitute therefore the upper boundary of environmental
concentrations that could possibly be observed. In reality, not all FEs would remain suspended
and therefore the water concentration would be reduced. The PEC values assumed one well-
mixed compartment per country. Local hotspots, e.g. after wastewater input into a small river,
are not captured by the model.
The estimated PEC values varied greatly among countries. It is not surprising to find that the
PECs were influenced by the country-specific wastewater management and the sludge
disposal. For instance, the concentration of FE shells was predicted to be zero for the soil
compartments of some countries including Malta and Switzerland. That is because sludge is
not allowed to be applied on soil in those counties, resulting in a zero flow of FEs to soil. On
the other hand, it is interesting to note that although the amount of mass flowing to some
environmental compartments was comparable in some countries, the estimated PECs can be
very different. For example, the amount of FEs flowing to surface water was 0.67 t and 0.71 t
for Belgium and Portugal respectively, while Belgium had a PEC of 0.13 µg/L for surface water
which was 3 times higher than that for Portugal (0.04 µg/L). The reason behind this difference
was that the PEC calculation was influenced not only by the mass flowing to the aquatic
compartment, but also by the mass of the receiving water systems in each country. Belgium
only has about 160 km2 of surface water according to the FAO database47, 48, which is only one
third of that of Portugal (610 km2). The released FE shells were therefore much more diluted
in Portugal than in Belgium, resulting in lower PEC values.
127
The potential hazardous effects posed by FE shells were evaluated for freshwater, sediment
and soil and no detrimental effects to the tested organisms were observed even at the highest
tested concentration. Therefore, only HONECs could be obtained from the experiments.
According to our knowledge, no other study has evaluated the ecotoxicity of FE shells or the
materials they are made of, but there are numbers of studies carried out to investigate the
ecological effects of microplastics21, 22. Adam and Nowack (2019) showed with a meta-analysis
that with the currently available quantitative information on NOEC values, the type of
microplastic has no statistically significant effect on the toxicity. However, the mean freshwater
PNEC reported for microplastics with 0.08 µg/L34 is much smaller than the HONEC of 2.67
mg/L for Raphidocelis subcapitata reported in this study for FE shells. In terms of sediment, no
negative effect was found for Lumbriculus variegatus at the highest concentration (40% plastic
weight of sediment mixture)60, which was in line with the results of FE shells (HONEC= 5.35
mg/kg). The toxicological data for the soil compartment is also very limited because most
studies reported no significant effect on terrestrial organisms at the highest tested
concentration61. One study found that microplastic at a concentration of 28% plastic weight of
sediment can significantly reduce the growth rate of Lumbricus terrestris62, but this tested
concentration was much higher than the HONEC for FE shells (9.1 mg/kg). Therefore,
ecotoxicological experiments at higher concentrations are needed to obtain NOEC/EC20
values for FE shells that can then be used in a standard environmental risk assessment by
calculating PNEC values63.
The environmental risks in our work were only characterized by directly comparing the
distribution of PECs with the HONECs. All PECs estimated by the PFMA model were lower
than the HONECs, indicating that currently no risk exists. Since the actual PNEC values that
should be derived from experimentally observed NOEC values will be higher than HONECs,
the current PEC/HONEC ratios tend to overestimate the risk. In addition, the inclusion of
environmental fate processes will decrease the FE concentrations in water, because this work
used a worst-case scenario with no sedimentation from the water column. Microplastics will
sediment from the water column in a size-dependent way and retention within a flowing river
was predicted to be almost 100% for particles larger than 50 µm64. The FE shells are therefore
within a range where sedimentation can be expected and thus the actual PECs will be lower.
The lower PEC values will therefore even further lower the PEC/HONEC ratios for FE shells,
further increasing the spread between exposure and hazard.
On a longer timescale, the assessment of the environmental risks posed by FEs is subject to
several uncertainties. On the hazard side, as discussed above, actual effects if any probably
occur at much higher concentrations than indicated by the HONECs used in this study. On the
exposure side, FEs are listed as one type of intentionally added microplastics which are
128
proposed to be restricted after a transition period of 5 or 8 years by ECHA1. In addition, the
fragrance industry is striving to replace the traditional FEs with biodegradable materials in the
future. Therefore, it can be expected that the release of FEs made of traditional thermoset
polymers is going to decrease in the next decade. Nevertheless the microplastic global
pollution coming from thermoplastic polymers in the environment is still far from being
addressed.
In summary, a full risk assessment cannot be performed for FE shells at the moment, since
PNEC values cannot be calculated due to limited toxicity. Therefore, PECs estimated by a
PMFA model were compared with HONECs. The results suggest the current environmental
levels of FE shells pose no risk to living organisms in freshwater, soil and sediment for selected
countries. Future studies could be carried out to better understand the levels at which
ecotoxicological effects are actually observed and the environmental fate process of FE shells.
This work was financed by Firmenich SA. We would like to thank Arnaud Struillou and Dawn
Allan for providing valuable information and feedback and Jana Pika, for the valuable
discussions and Drs. Markus Simon and Karsten Schlich for conducting the ecotoxicological
tests at the Fraunhofer Institute for Molecular Biology and Applied Ecology.
129
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6. Conclusions and outlook
This thesis investigated the microplastics released from the textile sector and the work was
divided in four steps. Firstly, the occurrence of MPFs in textile products was explored and the
manufacturing stages responsible for the MPF formation were identified. In the second and
third steps, the release of MPFs during washing and the formation of fiber fragments during
abrasion was investigated. Lastly, the environmental risks concerning the use of laundry care
products was assessed. The conclusions drawn from each part are detailed in the following
sections.
6.1. Conclusions
The thesis has confirmed that MPFs are present in textile products prior to use. Those MPFs
can be extracted and quantified using an ultrasonic extraction method without producing new
MPFs during the extraction process. A variety of textile products along the production line were
investigated and the manufacturing process was found to play an important role in the MPF
formation. The rotor spinning process during yarn production and the surface treatment during
textile finishing seem to be among the most important stages responsible for generating new
MPFs. Besides the cutting methods have a great influence on the number of MPFs extracted
from textile swatches: a significantly lower amount of MPFs was extracted from the laser-cut
samples than the scissor-cut ones. This may be because the MPFs are trapped inside the
yarns and the laser cutting can prevent the migration of the MPFs from the opening end into
the extraction liquid by melting the yarn ends. Even if some new MPFs are formed during the
laser cutting, the majority of them are likely sealed into the molten ends. By comparing the
extraction of the two cutting methods, the contribution by textile surface and edge to the total
extracted MPFs was differentiated and the cut edge was identified as the major source of MPFs.
Although yarn spinning was revealed to be a critical process for MPF formation, the influence
of relevant parameters during yarn spinning (e.g. yarn feeding speed, yarn twisting) could not
be investigated in this work due to the limited availability of textile samples. A better
understanding of those parameters is necessary if we would like to optimize the manufacturing
process and produce textile products with reduced amount of MPFs in the future.
In the next step, the thesis investigated the MPF release during the use phase of textiles, where
the mechanisms controlling the MPF release during washing of textiles were studied. As a
strong decrease of MPF release over repeated wash cycles was observed for all textiles, the
washing process is probably a process of releasing the production-inherited MPFs trapped
within the textiles instead of generating new ones. Similar to the findings from the first article,
136
the MPF release was affected by the textile properties and the textile samples with processed
surface released a significantly more MPFs than the ones with unprocessed surface. The
microfiber fabric released the highest amount of MPFs per gram textiles ever reported by
studies so far, suggesting that this type of textile may be a very substantial source of MPFs.
Since the raw edge was identified as a source of MPFs, more different types of commonly used
cutting/sewing methods were investigated. Except for the laser cutting, none of the other
investigated cutting/sewing methods were found to significantly reduce the amount of MPF
release compared to the scissor cutting. The finding indicates that unless the cut edge is
thermally sealed, the edge treatment with either yarns (e.g. overlock sewing) or fabrics (e.g.
double-folded sewing) cannot prevent the migration of MPFs from the raw edges to the wash
water. Besides, a significantly higher amount of MPFs was found to be released from the
overlock-sewn sample than the one with raw edges. Therefore, one needs to be cautious about
the additional damage to fabrics during the tailoring process, which may result in the formation
of additional MPFs.
In the first and the second articles, the origin of the MPFs in textile products and the release of
MPF during washing was explored. Based on the results, some measures can be suggested
to reduce the production-inherited MPFs and their subsequent release during washing. Firstly,
since the majority of MPFs was found to be released during the first a few wash cycles, a large
percentage of the production-inherited MPFs can be removed and collected by prewashing of
the tailored garments at factory. Secondly, our results have shown that the majority of the
released MPFs during washing originated from edges. The adoption of cleaner cutting methods
is important to reduce the MPF release during washing. The thermal cutting methods (e.g.
laser cutting) are preferred to the mechanical cutting methods.
The first two studies investigated only part of the life-cycle of textiles and excluded possible
formation of MPF during the use phase. Therefore, this thesis investigated in a next step the
formation of fiber fragments as a result of textile abrasion. Two types of fiber fragments with
distinguished morphologies were extracted from the abraded textile samples, confirming the
hypothesis that fiber fibrillation can be induced after a repetitive application of mechanical
stress. The occurrence of fibrils with much smaller diameters and length has been largely
overlooked by previous research. The diameter of the fibrils formed during abrasion falls within
the inhalable size for airborne particles, which raises potential human exposure concerns.
However, it has to be noted that the scenario simulated by the Martindale tester is very limited.
The obtained results only describe the potential of fiber fragments to be formed after a long
period of use, but to which extent those formed fragments can be released into the surrounding
air is still unclear. Besides, the study only quantified particles with fibrous shape. There were
also micron- and submicron-sized particles such as flakes, fragments and spheres visible on
137
the SEM images, which were not characterized in this work and need to be investigated in the
future.
In addition to the release from synthetic textiles, the fragrance encapsulates added into laundry
products contributes to another release pathway of microplastics from the textile sector. The
average PECs were found to be between eight times and six orders of magnitude lower than
the HONECs for different environmental compartments, suggesting no environmental risks of
FEs based on the current data. However, this result is only a preliminary and precautionary
evaluation based on the currently available data. For the exposure assessment, the calculation
of PECs was based on a worst-case model which did not include the any environmental fate
process and may result in an overestimation of the risk. For the hazard assessment, no PNEC
could be derived from current ecotoxicological data, and therefore a standard environmental
risk assessment could not be performed. In fact, the PNEC values can be several times higher
than the HONEC values. Therefore, the use of HONEC values in environmental risk
assessment is more likely to overestimate the risk and therefore constitutes a precautionary
approach. More data from both of the exposure and hazard side is needed in the future to
enhance the accuracy of environmental risk assessment of FEs.
6.2. Outlook
This thesis contributed to the understanding of the microplastic release from the textile sector.
Given the results by this work, there are many research opportunities in the future.
Our work has identified that the yarn spinning may be responsible for the formation of
production-inherited MPFs in textile products. It is known that the yarn properties are
determined by the setting during the production process such as the types of spinning methods,
the delivery speed and the output density1. The influence by those parameters on the formation
of MPFs could not be investigated in this study due to the limited availability of textile samples.
Future collaboration between academia and industry is needed to comprehensively investigate
how those parameters can affect the MPF generation during yarn spinning. Ideally,
experiments will be carried out with yarns produced from the same starting material by different
spinning methods. The results from such a controlled study are likely able to provide the
scientific basis for the optimization of textile production line.
Secondly, continued efforts need to be made to understand the fiber fragment formation and
release during wearing of textiles. In this study, only limited samples and abrasion conditions
were applied. It would be interesting to investigate how the textile properties, the duration and
the pressure during abrasion can influence the formation of fibrils. Besides, the Martindale
138
tester used in this study can only simulate very limited application scenarios of the use of
textiles, and the correlation between the results from the abrasion test and real world scenarios
has not been well established. Therefore, a chamber study is needed in the future to determine
the release of fiber fragments formed from aged textiles during normal use.
Thirdly, the small size of fibrils has triggered the concern of human exposure issues. It is
believed that a fraction of small MPFs have the potential to be inhaled by humans 2, 3 and may
be persistent in the respiratory system4, 5. For stiff fibers, the aerodynamic diameter is
controlled by the diameter or width, which subsequently determines the location of pulmonary
deposition6, 7. However, fibrils from synthetic textiles often demonstrate a high degree of
curvature and flexibility. The aerodynamic behavior of those fibrils is still unknown. Future
research is needed to investigate how those fibrils transport in human respiratory system and
the subsequent toxicity. It is important to distinguish if the toxicity of fibrils is induced by inhaling
fine particles or leaching of chemicals from synthetic polymers. If the adverse effect is merely
due to the inhalation of particles, then the toxicity of synthetic fiber is not necessarily different
from the one of natural fibers. In addition, the ecotoxicity of microplastics is believed to depend
on the size8, 9 and the shape of particles9. For instance, a study reported that fibers with a size
less than 50 µm are more hazardous to shrimp than spheres and fragments9. Since fibrils
demonstrates a significantly different morphology than MPFs, it would be interesting to
investigate if this would result in different ecotoxicological effects.
Furthermore, the submicron particles with other morphologies such flakes, fragments and
spheres were not characterized in this work. But they are observed to be released from
synthetic textiles. The advancement of analytical method is needed in the future to allow more
precise identification and analysis of the smaller particles. Further investigation of the formation
and release of submicron- or nanoplastics will contribute to a more comprehensive
understanding of microplastic release from synthetic textiles.
Last but not the least, the environmental risks associated the used of FEs in laundry care
products were assessed in this study. A worst-case model was used to predict the
environmental concentration for freshwater. It is known that sedimentation of microplastics in
rivers is size-dependent10. The further inclusion of environmental fate processes can increase
the accuracy of the model. Besides, the calculation of PNEC for FEs is impossible based on
the current data, since no adverse effect was observed at the highest tested concentration.
Therefore, ecotoxicological experiments at higher concentrations is necessary to determine
the effective concentration such as NOEC and EC20. Then PNEC values can be derived
following the REACH guidance11 and a standard environmental risk assessment can be
performed.
139
6.3. References
2. Vianello, A.; Jensen, R. L.; Liu, L.; Vollertsen, J., Simulating human exposure to indoor
airborne microplastics using a Breathing Thermal Manikin. Scientific Reports 2019, 9, (1), 1-
11.
3. Pauly, J. L.; Stegmeier, S. J.; Allaart, H. A.; Cheney, R. T.; Zhang, P. J.; Mayer, A. G.;
Streck, R. J., Inhaled cellulosic and plastic fibers found in human lung tissue. Cancer
Epidemiology and Prevention Biomarkers 1998, 7, (5), 419-428.
4. Gasperi, J.; Wright, S. L.; Dris, R.; Collard, F.; Mandin, C.; Guerrouache, M.; Langlois,
V.; Kelly, F. J.; Tassin, B., Microplastics in air: are we breathing it in? Current Opinion in
Environmental Science & Health 2018, 1, 1-5.
5. Prata, J. C., Airborne microplastics: Consequences to human health? Environmental

Pollution 2018, 234, 115-126.
6. Donaldson, K., The inhalation toxicology of p-aramid fibrils. Critical reviews in

toxicology 2009, 39, (6), 487-500.
7. Sturm, R., A theoretical approach to the deposition of cancer-inducing asbestos fibers

in the human respiratory tract. The Open Lung Cancer Journal 2009, 2, (1).
8. Jeong, C.-B.; Won, E.-J.; Kang, H.-M.; Lee, M.-C.; Hwang, D.-S.; Hwang, U.-K.; Zhou,
B.; Souissi, S.; Lee, S.-J.; Lee, J.-S., Microplastic size-dependent toxicity, oxidative stress
induction, and p-JNK and p-p38 activation in the monogonont rotifer (Brachionus koreanus).
Environ Sci Technol 2016, 50, (16), 8849-8857.
9. Gray, A. D.; Weinstein, J. E., Size- and shape-dependent effects of microplastic

particles on adult daggerblade grass shrimp (Palaemonetes pugio). Environmental
Toxicology and Chemistry 2017, 36, (11), 3074-3080.
10. Besseling, E.; Quik, J. T.; Sun, M.; Koelmans, A. A., Fate of nano-and microplastic in
freshwater systems: A modeling study. Environmental Pollution 2017, 220, 540-548.
11. ECHA, Guidance on information requirements and chemical safety assessment,

Chapter R.10: Characterisation of dose [concentration]-response for environment, European
Chemical Agency. 2008.
140
Annex 1. Supporting Information for Chapter 2
Table A1-1. SEM images for the sliver, the yarns and the textiles used in this study
Name SEM images of textile surface and of single thread removed from the
textile
Filament
Sliver
Rotor
Air-jet
Ring
(white)
141
Ring
(black)
Interlock S
Jersey S
Rib S
Rib F
Terry S
142
Plain S
Plain F
Twill F
Satin F
Fleece
Plain B
143
Microfiber
144
Dyeing process
Samples were cut into a piece of about 1.5g. The steel vessels of the dyeing machine were
cleaned with DI water.
• Stock solution preparation
0.5 g dark blue BEMACRON E-RD dyes (CHT, Switzerland) was dissolved in 50 ml DI water
by stirring with a magnet to make a 1% dye solution. 5 ml of CHT dispergator , Sarabid TS
300 and Meropan Cit all from CHT (CHT, Switzerland) was diluted with 45 ml to a 1:10
solution respectively.
• Step 1: Dyeing the polyester
1.5 g of the sample was put into a 100 ml steel vessel. Then 1 ml CHT dispergator stock
solution, 2 ml Sarabid TS 300, 2ml Meropan Cit and 3 ml 1% dye solution were added into
the vessel. The final concentration of each chemical is showed in Table A2.
Table A1-2. The composition of the solution for the 1st dyeing step
Chemical Concentration
CHT dispergator 1g/L
Sarabid TS 300 1g/L
Meropan Cit 1g/L
Pigment 3% of the polyester weight
The vessel was then put into the dyeing machine for the dyeing process at 130°C, 60 min
with a heating rate of 1°C per minute and 2°C per minute as the cooling rate.
• Step 2: Fixing the color and removing the extra dyes
0.1 ml of Sarabid dlo conc. (1g/L), 0.3 ml of caustic soda (3ml/L), 0.2 g of hydrosulphite
(2g/L) and 100 ml milliQ water were added to the vessel. The vessel was put into the dyeing
machine again for a process at 80 °C for 15 min with 1°C per minute as the heating rate and
2°C per minute as the cooling rate.
145
Table A1-3. The composition for the solution for the 2st dyeing step.
Chemical Concentration
Sarabid dlo 1g/L
Caustic soda 3g/L
Hydrosulphite 2g/L
Figure A1-1. Length distribution of the MPFs in the aliquots sampled from the same solution.
Three aliquots were labeled as “1”, “2”, “3” in different colors.
146
A B
6000 Jersey S 6000 Rib S
4500 4500
[MPF/g textile]
[MPF/g textile]
3000 3000
1500 1500
0 0
1 2 3 4 5 6 7 8 9 1 2 3 4 5 6 7 8 9
C D
6000 Terry S 6000 Plain F
4500 4500
[MPF/g textile]
[MPF/g textile]
3000 3000
1500 1500
0 0
1 2 3 4 5 6 7 8 9 1 2 3 4 5 6 7 8 9
E F
6000 Satin F 30000 Microfiber
25000
4500
[MPF/g textile]
[MPF/g textile]
20000
3000 15000
10000
1500
5000
0 0
1 2 3 4 5 6 1 2 3 4 5 6 7 8 9
Figure A1-2. The extraction of MPFs from six textiles as a function of the number of extraction
steps. All results are presented in number of MPFs per gram of textile. The black color
represents the scissor-cut samples, the red color the laser-cut samples. Standard deviations
were calculated from triplicate experiments.
147
Figure A1-3. Percentage of MPFs extracted during the 1st extraction compared to the
cumulative number of extracted MPFs. The mean values for the scissor-cut and laser-cut
samples are represented by the black dots and red dots respectively. Standard deviations were
calculated from three parallel experiments.
148
A Jersey S B Rib S

10000 10000
1000 1000
100
100
1 2 3 4 5 6 7 8 9 1 2 3 4 5 6 7 8 9
C Terry S D Plain F

Length of MPF [µm]
10000 10000
1000 1000
100 100
1 2 3 4 5 6 7 8 9 1 2 3 4 5 6 7 8 9
E Satin F F Microfiber
10000 10000
1000 1000
100 100
1 2 3 4 5 6 1 2 3 4 5 6 7 8 9
Figure A1-4. Length distribution of MPFs released during the 1st extraction step. 25th and 75th
percentiles were plotted in the boxes with a line indicating the median. Whiskers represent 95%
of length distribution and outliers were labelled by dots.
149
Figure A1-5. Comparison of fiber diameters between the textile (Table A2) and the released
MPFs (measured by SEM on filters). The distribution of fiber diameters from textiles was shown
either in grey for the knit textiles or in grey and red for the woven textiles. The length distribution
of extracted MPFs is shown in blue. 25th and 75th percentiles were plotted in the boxes with a
line indicating the median. Whiskers represent 95% of length distribution and outliers were
labelled by black dots.
150
Figure A1-6. The edge of Jersey S cut with a laser-cutter (left); the edge of Jersey S cut with
a scissor (right). The edges were indicated by yellow arrows.
151
Table A1-4. Number of MPFs extracted from 12 textiles in MPF/g textile.
Extraction steps
Material Edges Number Sum
1 2 3 4 5 6 7 8 9
mean 7449 2245 947 1164 563 426 426 310 225 13754
Scissor
StD 1854 592 290 459 63 130 123 124 39 798
Interlock S
mean 284 64 34 23 - - - - - 406
Laser
StD 40 10 26 9 - - - - - 49
mean 4447 969 284 219 151 318 243 111 119 6863
Scissor
StD 1044 308 114 104 30 256 157 14 38 1116
Jersey S
mean 247 73 35 35 22 16 - - - 428
Laser
StD 53 20 1 3 3 3 - - - 69
mean 4033 2713 1584 1539 982 775 787 414 234 13059
Scissor
StD 151 1068 746 1135 104 481 369 152 5 781
Rib S
mean 279 91 73 38 32 30 42 18 20 623
Laser
StD 45 24 29 22 17 10 4 3 7 31
mean 4353 1417 578 402 393 299 350 280 176 8248
Scissor
StD 604 59 115 288 178 67 22 111 94 458
Terry S
mean 218 76 56 15 - - - - - 365
Laser
StD 91 9 20 4 - - - - - 90
mean 1992 413 439 209 246 141 203 157 137 3937
Scissor
StD 538 115 117 51 34 29 60 51 41 435
Plain S
mean 94 31 - - - - - - - 125
Laser
StD 7 7 - - - - - - - 14
mean 1758 277 114 85 60 45 2340

Scissor
StD 564 132 58 37 28 16 710
Satin F
mean 222 42 - - - - - - - 264
Laser
StD 62 13 - - - - - - - 69
mean 1336 692 96 56 88 50 49 56 66 2489

Scissor
StD 357 267 28 23 41 22 6 31 24 455
Rib F
mean 102 26 - - - - - - - 128
Laser
StD 7 2 - - - - - - - 5
Plain F Scissor mean 1201 106 78 81 80 137 73 87 77 1919
152
StD 198 22 33 49 30 43 9 20 1 339
mean 252 4 - - - - - - - 256

Laser
StD 124 3 - - - - - - - 127
mean 550 57 49 42 38 19 - - - 755

Scissor
StD 97 16 20 27 16 6 - - - 93
Twill F
mean 91 12 12 - - - - - - 116
Laser
StD 29 3 4 - - - - - - 30
mean 2495 1294 944 917 603 492 385 426 689 8245
Scissor
StD 335 189 431 292 94 156 37 72 223 793
Plain B
mean 421 136 88 52 29 25 - - - 751
Laser
StD 56 39 40 2 13 16 - - - 117
mean 17077 3587 2673 1633 1307 1101 729 709 726 29540
Scissor
StD 1376 992 456 396 149 199 64 330 66 2209
Fleece
mean 5752 2448 862 437 448 302 206 211 134 10799
Laser
StD 335 476 290 131 148 4 72 34 36 948
mean 19446 5852 4977 3451 3456 2389 2064 2003 1760 45398
Scissor
StD 4270 271 1205 358 756 409 407 171 399 2898
Microfiber
mean 5925 1793 1109 628 359 451 364 334 316 11279
Laser
StD 265 266 183 160 55 57 94 96 28 457
153
Table A1-5. Number of MPFs extracted from the sliver and yarns in MPF/g textile.
Dyeing process Extraction steps

Sliver/yarn Statistic Sum
1 2 1 2 3 4 5 6 7 8 9
mean 86 127 67 63 45 31 32 32 24 43 36 585

Sliver
StD 32 27 33 40 5 5 9 13 10 6 3 115
mean 797 884 455 403 215 327 303 221 251 266 189 4310
Rotor
StD 45 154 58 69 90 97 77 99 116 112 63 282
mean 80 49 13 10 - - - - - - - 153
Airjet
StD 20 2 2 4 - - - - - - - 20
mean 43 26 24 11 - - - - - - - 104
Ring (white)
StD 17 12 7 2 - - - - - - - 37
mean - - 117 35 41 23 13 - - - - 228

Ring (black)
StD - - 39 6 15 6 3 - - - - 51
mean - - 11 4 - - - - - - - 15
Filament
StD - - 3 2 - - - - - - - 5
154
Table A1-6. Number of MPFs extracted from a 36 cm2 Interlock S textiles at different
perimeters in MPF/g textile.
Edge
Size (cm x cm) Perimeter (cm) Scissor-cut Laser-cut
mean StD mean StD
6x6 24 5626 499 214 13
6x3 32 9884 901 229 73
3x3 48 13989 4321 160 43
3x2 60 23181 1105 144 26
2x2 72 26685 1797 194 32
155
Table A1-7. Mass of the MPFs extracted from the knit textiles in µg/g textile.
Extraction steps
Material Edges Number Sum
1 2 3 4 5 6 7 8 9
Scissor mean 584.2 195.8 93.4 128.7 66.2 47.7 46.8 35.0 24.5 1222.2
Laser StD 178.3 50.7 30.9 52.1 31.5 14.3 11.2 13.6 4.0 114.5
Interlock S
Scissor mean 25.2 7.3 4.3 2.7 - - - - - 39.5
Laser StD 3.8 1.8 4.0 1.6 - - - - - 5.5
Scissor mean 421.4 91.0 32.4 25.6 17.2 43.4 28.1 12.7 15.1 686.9
Laser StD 129.2 14.9 10.2 11.4 3.5 39.0 19.3 1.5 4.0 121.4
Jersey S
Scissor mean 21.8 8.7 4.5 4.8 2.8 2.9 - - - 45.5
Laser StD 5.5 3.3 0.1 0.4 0.8 0.4 - - - 7.7
Scissor mean 402.8 273.7 182.3 200.0 131.0 107.9 103.5 57.8 33.6 1492.5
Laser StD 58.2 95.5 108.7 153.8 19.6 76.7 46.5 17.2 1.9 98.6
Rib S
Scissor mean 24.3 9.1 8.4 6.3 3.2 4.3 4.3 2.1 2.4 64.5
Laser StD 4.6 1.2 5.1 3.4 1.8 1.5 0.3 0.2 0.5 7.8
Scissor mean 224.5 140.4 20.7 11.6 21.1 11.2 10.4 13.4 14.5 467.9
Laser StD 71.8 54.4 5.9 4.4 10.3 5.6 1.3 7.7 6.1 85.3
Terry S
Scissor mean 14.1 3.9 - - - - - - - 18.0
Laser StD 3.0 0.5 - - - - - - - 2.8
Scissor mean 60.6 5.9 5.9 3.4 4.8 2.4 - - - 83.0
Laser StD 11.0 1.8 2.0 2.1 3.0 1.1 - - - 6.4

Rib F
Scissor mean 11.8 1.4 1.8 - - - - - - 21.3
Laser StD 8.5 0.1 0.6 - - - - - - 1.1
Scissor mean 58.7 36.2 30.5 27.4 18.4 13.7 10.6 12.3 23.1 230.8
Laser StD 6.2 9.5 15.0 11.3 2.2 4.8 2.1 2.3 7.6 19.7
Fleece
Scissor mean 19.1 7.3 4.9 3.0 1.7 1.8 - - - 37.8
Laser StD 3.2 2.3 2.8 0.3 0.8 1.1 - - - 7.1
156
Table A1-8. Mass of the MPFs extracted from the sliver and yarns in µg/g textile.
Dyeing
Extraction steps
Numbe process
Sliver/yarn Sum
r
1 2 1 2 3 4 5 6 7 8 9
18. 13. 14. 10. 129.

mean
11.2 21.1 6.2 9.2 7 9.2 5 8.9 6.3 2 9 3
Sliver
10. 16.
Std
4.2 12.0 5.7 4 4 2.6 4.8 7.2 6.9 7.8 2.3 37.7
13. 17. 15. 15. 15. 16. 16. 12. 180.

mean
24.8 25.2 3 5 8.5 6 1 5 3 8 5 9
Rotor
Std 5.7 5.4 2.9 6.1 2.0 4.3 4.4 8.0 8.7 6.2 5.2 18.3
mean 3.5 2.6 0.9 1.2 - - - - - - - 8.2

Air-jet
Std 1.5 0.4 0.1 0.2 - - - - - - - 1.4
mean 3.7 2.2 1.0 1.2 - - - - - - - 8.1

Ring
(white)
Std 1.6 0.9 0.1 0.2 - - - - - - - 2.3
mean - - 6.3 2.5 3.5 2.3 - - - - - 14.6

Ring
(black)
Std - - 1.9 0.1 1.3 0.8 - - - - - 2.0
mean - - 0.4 0.2 0.6

Filament
0.0 0.1
Std
1 0.2
157
Table A2-1. SEM images for the textiles used in this study. Two images were taken if the
samples have different structures for the front and back side. For the textile with woven
structure, both the warp and weft threads were imaged.
Name SEM images of textile surface and of single yarns removed from the
textile
Satin F
Twill F
Rib F
Plain F
Terry S
158
Plain S
Rib S
Jersey S
Interlock S
Fleece
Plain B
159
Microfiber
160
Figure A2-1. An example of different cutting/sewing methods for Interlock S.
161
Figure A2-2. An example of analyzed filter.
162
(to be continued)
163
(to be continued)
164
(to be continued)
165
Figure A2-3: Examples of MPFs released from 12 textiles during 1st wash cycle.
166
Table A2-2. SEM images for edges of selected samples (Interlock S, Plain F, Plain B,
Microfiber)
Samples Scissor-cut Laser-cut
Interlock
S
Plain F
167
Plain B
Microfiber
168
Table A2-3. Washing conditions modified from ISO standard1, where LAS solution was
used to replace the standard detergent.
Parameter Experimental conditions
Time 45 min
Speed 40 r/min
Temperature 40 ± 2°C
Mechanical stress 10 stainless steel balls
Washing solutions 150 ± 1 g 0.75 g/L LAS solutions*
pH value 9.20 ± 0.1
Number of wash cycles 1
* A 0.75 g/L LAS solution (Alfa Aesar) was adjusted the pH to 9.2 ± 0.1 with 1 mol/L
solution of sodium hydroxide (Sigma-Aldrich).
Assessment of the washing procedure
The level of contamination of the filters during the whole experimental procedure was
determined by analyzing 130 blanks collected during 65 wash cycles. The blanks were
analyzed for four sets of experiments individually. The average number of MPF per filter was
14, 4, 5 and 7 for "textile property", "wash cycle", "mechanical stress" and "cutting/sewing
method" experiment respectively. The overall average for four sets of experiments was 7 MPF.
Furthermore, the reliability of the workflow was evaluated by analyzing triplicate aliquots from
the same solution. Since those aliquots were from the same wash water, the fiber number
should be identical. Any variation in the triplicate aliquots originated from the sample/image
processing. In total, 132 filters from 44 solutions were analyzed for MPF number, resulting in
a mean relative standard deviation of approximately 13%. The washing procedure for Interlock
S and Plain F was repeated four times, for Fleece and Plain S three times, under the same
conditions during the different experiments. A comparison of the number of released MPF was
made for the same textile showing that most of the textiles demonstrated a relative standard
deviation (RSD) below 30% with an average of 16% except for Plain F with a RSD of 87% and
42% for laser-cut and scissor-cut samples respectively (Figure A3).
169
Scissor-cut
Laser-cut
Number released [MPFs/g textile]
10000
1000
100
10
Plain F Plain S Interlock S Fleece
Figure A2-4. Number of MPF released from the same type of textiles under the same
conditions on different days. Standard deviation was calculated based on the average
number of release from the experiments on different days.
170
Table A2-4. Number of MPF released during the 1st wash cycle [MPF/g textile]. SC: scissor-
cut; LC: laser-cut.
Replicates [MPF/g textile] Mean

Cutting/sewing RSD
Textile SD
method [MPF/g [%]
1 2 3
textile]
Satin F LC 662 870 755 762 104 14
Satin F SC 1790 1495 1200 1495 295 20
Twill F LC 232 218 187 212 23 11
Twill F SC 3619 2650 2786 3018 525 17
Rib F LC 276 304 203 261 52 20
Rib F SC 5729 5213 6076 5673 434 8
Plain F LC 905 759 568 744 169 23
Plain F SC 5233 6407 6225 5955 632 11
Terry S LC 482 256 390 376 114 30
Terry S SC 5952 8833 4892 6559 2039 31
Plain S LC 870 1131 1323 1108 227 21
Plain S SC 6573 8684 7846 7701 1063 14
Rib S LC 1048 1399 1219 1222 176 14
Rib S SC 5806 12357 6378 8180 3628 44
Jersey S LC 1142 820 835 932 182 19
Jersey S SC 10618 7926 8667 9070 1391 15
Interlock S LC 680 673 446 600 133 22
Interlock S SC 8720 16628 9294 11547 4409 38
Fleece LC 8671 11700 9953 10108 1520 15
Fleece SC 21752 26280 22179 23404 2500 11
Plain B LC 2497 2245 2190 2311 164 7
Plain B SC 34423 39630 37963 37339 2659 7
Microfiber LC 14519 16635 17788 16314 1658 10
Microfiber SC 68684 70192 78117 72331 5067 7
171
Table A2-5. Length of MPF released during the 1st wash cycle. SC: scissor-cut; LC: laser-cut.
Median Median
Cutting/sewing Cutting/sewing
Textile length length
method method
[µm] [µm]
Satin F LC 288 SC 441
Twill F LC 470 SC 364
Rib F LC 276 SC 756
Plain F LC 392 SC 396
Terry S LC 480 SC 841
Plain S LC 297 SC 480
Rib S LC 480 SC 527
Jersey S LC 416 SC 540
Interlock S LC 465 SC 527
Fleece LC 261 SC 540
Plain B LC 224 SC 464
Microfiber LC 165 SC 231
172
Figure A2-5. Length distribution of MPF released during the 1st wash cycle: A) local plot on a
linear scale plot, where the boxes represent 25th and 75th percentiles with the median
indicated by a line; B) full plot on a log scale, where the outliers are shown by dots.
173
Table A2-6. Number of MPF released during 1st, 2nd, 3rd, 5th, 8th and 10th wash cycle for laser-
cut samples.

Wash
Textile SD RSD [%]
Cycle
1 2 3 [MPF/g textile]
Plain F 1 1937 2034 1203 1725 454 26
Plain F 2 47 31 46 41 9 22
Plain F 3 10 10 10 10 0 0
Plain F 5 5 5 5 5 0 0
Plain F 8 9 10 22 14 7 53
Plain F 10 12 14 17 14 3 18
Plain S 1 667 1423 1224 1105 392 35
Plain S 2 585 531 568 561 28 5
Plain S 3 431 292 426 383 79 21
Plain S 5 354 431 268 351 82 23
Plain S 8 246 210 187 214 30 14
Plain S 10 172 210 211 198 22 11
Interlock 1 714 485 839 679 180 26
Interlock 2 204 207 214 208 5 2
Interlock 3 89 172 118 126 42 33
Interlock 5 96 95 46 79 29 36
Interlock 8 42 50 40 44 5 12
Interlock 10 18 35 17 23 10 43
Fleece 1 7443 8082 7027 7517 531 7
Fleece 2 3021 2712 2372 2702 325 12
Fleece 3 925 1048 1297 1090 190 17
Fleece 5 288 315 275 293 20 7
Fleece 8 201 130 115 149 46 31
Fleece 10 148 99 89 112 32 28
174
Table A2-7. Number of MPF released during 1st, 2nd, 3rd, 5th, 8th and 10th wash cycle for
scissor-cut samples.

Wash
Textile SD RSD [%]
Cycle
1 2 3 [MPF/g textile]
Plain F 2 412 595 653 553 126 23
Plain F 3 320 352 178 283 93 33
Plain F 5 381 274 392 349 65 19
Plain F 8 539 403 539 494 79 16
Plain F 10 646 347 564 519 154 30
Plain S 1 8000 7179 7421 7533 422 6
Plain S 2 3077 4286 2724 3362 819 24
Plain S 3 2179 1750 1066 1665 561 34
Plain S 5 1256 1089 908 1084 174 16
Plain S 8 1436 1214 1046 1232 196 16
Plain S 10 1160 1482 1382 1341 165 12
Interlock 1 24137 10588 13482 16069 7135 44
Interlock 2 1905 10676 7679 6753 4458 66
Interlock 3 1797 1076 4179 2351 1624 69
Interlock 5 494 847 845 729 203 28
Interlock 8 347 312 208 289 72 25
Interlock 10 239 240 250 243 6 3
Fleece 1 28914 21481 31111 27169 5047 19
Fleece 2 14408 12654 12901 13321 949 7
Fleece 3 4263 6296 4722 5094 1066 21
Fleece 5 2368 3796 1778 2647 1038 39
Fleece 8 928 1370 796 1031 301 29
Fleece 10 579 833 556 656 154 23
175
Table A2-8. Median length of the released MPFs during the 1st and 10th wash cycles. A K-W
non-parametric test was used to compare the length distribution of the MPFs. SC: scissor-
cut; LC: laser-cut.
Median (µm)
Cutting/sewing
Textile Significance
method
1st 10th
Fleece LC 320 930 <0.001
Fleece SC 416 1155 <0.001
Interlock S LC 412 481 0.073
Interlock S SC 594 924 <0.001
Plain S LC 331 527 <0.001
Plain S SC 476 828 <0.001
Plain F LC 279 558 0.212
Plain F SC 340 476 <0.001
176
A Plain F B Plain S
10000 10000
MPF length [µm]
1000 1000
NA
100 100
1 2 3 5 8 10 1 2 3 5 8 10
C Interlock S D Fleece
10000 10000
MPF length [µm]
1000 1000
100 100
1 2 3 5 8 10 1 2 3 5 8 10
Figure A2-6. Length distribution of MPF released during the 1st, 2nd, 3rd, 5th, 8th and 10th wash
cycle with complete dataset. NA: less than five MPFs. The values here were a summation of
triplicate experiments.
Table A2-9. Estimated cumulative release during 10 wash cycles. SC: scissor-cut; LC: laser-
cut.
Textile Cutting/sewing method Number [MPF/g textile]
Fleece SC 58345
Interlock S SC 29807
Plain F SC 14740
Plain S SC 21195
Fleece LC 13125
Interlock S LC 1421
Plain F LC 1847
Plain S LC 3939
177
Figure A2-7. A) Influence of mechanical stress on the number of MPF released from four
textiles during the 1st wash cycle. The mean values are represented by the black dots (no steel
balls), red dots (10 steel balls) and blue (20 steel balls). Error bars show the standard deviation
for three experimental replicates. S and L stand for scissor-cut and laser-cut respectively; B)
Length distribution of MPF released during the 1st wash cycle. The values here are a
summation of triplicate experiments. The number of MPF per sample was between 98 and
1178, with an average of 464.
178
Table A2-10. Number of MPF released with 0, 10 and 20 steel balls during washing. SC:
scissor-cut; LC: laser-cut.

Cutting/sewing Balls
RSD
Textile SD
[MPF/g [%]
method [#] 1 2 3
textile]
Plain F LC 0 514 355 250 373 133 36
Plain F LC 10 234 293 267 265 30 11
Plain F LC 20 629 388 207 408 212 52
Plain S LC 0 560 397 461 473 82 17
Plain S LC 10 788 712 731 744 40 5
Plain S LC 20 885 821 782 829 52 6
Interlock S LC 0 683 690 1063 812 217 27
Interlock S LC 10 845 580 741 722 134 18
Interlock S LC 20 890 679 500 690 195 28
Fleece LC 0 10532 10972 8767 10090 1167 12
Fleece LC 10 9486 9144 9479 9370 195 2
Fleece LC 20 8082 7838 9797 8572 1068 12
Plain F SC 0 9127 10848 10707 10227 956 9
Plain F SC 10 9643 11589 10371 10534 983 9
Plain F SC 20 11237 10018 9670 10308 823 8
Plain S SC 0 7220 6659 7192 7024 316 5
Plain S SC 10 8595 8890 8885 8790 169 2
Plain S SC 20 10618 10769 9366 10251 770 8
Interlock S SC 0 7731 11477 19167 12792 5830 46
Interlock S SC 10 12414 14826 12363 13201 1408 11
Interlock S SC 20 22174 15523 20275 19324 3426 18
Fleece SC 0 27400 29615 33958 30324 3336 11
Fleece SC 10 24930 33643 27534 28702 4472 16
Fleece SC 20 34859 31849 31849 32852 1738 5
179
Table A2-11. Number of MPF released from SC (scissor-cut), LC (laser-cut), DS (double-
sown), MC (model-cut) and OS (overlock-sown) samples.
Cutting/sewing Replicates [MPF/g textile] Mean

Wash RSD
Textile SD
Cycle [MPF/g [%]
method 1 2 3
textile]
Interlock S DS 1 7466 3352 4159 4992 2180 44
Interlock S DS 2 2704 1283 1725 1904 727 38
Interlock S DS 3 1404 1327 1533 1421 104 7
Interlock S OS 1 10308 9067 6631 8669 1871 22
Interlock S OS 2 3932 4467 3734 4044 379 9
Interlock S OS 3 1974 2400 1468 1947 467 24
Interlock S MC 1 6910 9281 6193 7461 1616 22
Interlock S MC 2 3576 3870 2030 3159 988 31
Interlock S MC 3 2035 1781 1954 1923 130 7
Interlock S LC 1 932 775 714 807 112 14
Interlock S LC 2 354 220 314 296 69 23
Interlock S LC 3 293 92 71 152 123 81
Interlock S SC 1 6532 10912 6848 8097 2443 30
Interlock S SC 2 2488 3199 2217 2635 507 19
Interlock S SC 3 1267 1896 1435 1533 326 21
Plain F DS 1 4559 3775 4408 4247 416 10
Plain F DS 2 696 454 391 514 161 31
Plain F DS 3 392 159 396 316 136 43
Plain F OS 1 7327 6006 5385 6239 992 16
Plain F OS 2 790 745 957 831 112 13
Plain F OS 3 348 355 273 325 45 14
Plain F MC 1 2578 2783 4101 3154 827 26
Plain F MC 2 340 283 545 389 138 35
Plain F MC 3 284 166 199 216 61 28
Plain F LC 1 250 625 183 353 238 68
Plain F LC 2 8 17 19 15 6 40
Plain F LC 3 2 6 13 7 6 80
Plain F SC 1 4045 4720 4021 4262 397 9
Plain F SC 2 301 157 594 351 223 64
Plain F SC 3 298 122 104 175 107 61
180
Figure A2-8. Length distribution of MPF released during the 1st wash cycle: A) local plot on a
linear scale plot, where the boxes represent 25th and 75th percentiles with the median
indicated by a line; B) full plot on a log scale, where the outliers are shown by dots.
Figure A2-9. Number of released MPFs from samples as a function of the number of wash
cycles for Interlock S and Plain F. Number of MPFs released from four textiles during the 1st
wash cycle. The mean values are represented by black (laser-cut), red (double-sewn), blue
(model-cut), green (scissor-cut) and purple (overlock-sewn). Error bars show the standard
deviation for three experimental replicates.
181
Figure A2-10. Length distribution of released MPFs from samples as a function of the
number of wash cycles for Interlock S and Plain F. The length distributions are represented
by black (laser-cut), red (double-sewn), blue (model-cut), green (scissor-cut) and purple
(overlock-sewn). The values here are a summation of triplicate experiments.
182
Figure A2-11. Fiber ends caused by different mechanisms:1)Scissor cutting; 2) Laser cutting;
3) Stretched by high tensile force.
183
Table A2-12. Mass of MPF released during the 1st wash cycle for knitted textiles. SC: scissor-
cut; LC: laser-cut.
Cutting/sewing Diameter Mass of Mass of

Textile [mg/g]
method [µm] MPFs [mg] samples [g]
Interlock S LC 12.21 0.034 2.53 0.07
Jersey S LC 12.8 0.034 2.6 0.10
Rib S LC 12.74 0.065 3.59 0.14
Rib F LC 15.87 0.021 2.45 0.03
Fleece LC 11.65 0.085 2.22 1.93
Terry S LC 13.04 0.024 2.46 0.05
Interlock SC 12.21 0.050 2.52 1.00
Jersey S SC 12.8 0.080 2.74 0.88
Rib S SC 12.74 0.041 3.73 0.82
Rib F SC 15.87 0.222 2.44 1.36
Fleece SC 11.65 0.105 2.38 0.66
Terry S SC 13.04 0.068 2.74 1.25
184
Figure A2-12. Comparison of results from different studies. Values taken from the 1st wash
cycle were transformed into number of MPF per gram textile. The red dashed lines represent
the range of the results from this study (212 - 72331 MPF/g). The cyan represents the results
from experiments using gyrowash and the purple represents the results from experiments
using domestic washing machine.Values were taken from the studies2-11.
185
Figure A2-13. Comparison of results from different studies. Values taken from the 1st wash
cycle were transformed into mg MPF per gram textile. The red dashed lines represent the
range of the results from this study (0.021 - 0.222 mg/g). The cyan represents the results
from experiments using gyrowash and the purple represents the results from experiments
using domestic washing machine. For the study by Hartline, et al.12, the mass per garment
was assumed to be 500 g. For the study by Pirc, et al.13, we assumed the area of a garment
is 1 m2 and mass is 500 g. Values were take from the studies3, 4, 6, 8-15.
186
References
1. ISO, 105-C06:2010: Textiles—Tests for Colour Fastness Part C06: Colour Fastness to
Domestic and Commercial Laundering. 2010.
1199.
3. De Falco, F.; Di Pace, E.; Cocca, M.; Avella, M., The contribution of washing processes
of synthetic clothes to microplastic pollution. Scientific Reports 2019, 9, (1), 6633.
4. De Falco, F.; Gentile, G.; Di Pace, E.; Avella, M.; Cocca, M., Quantification of
microfibres released during washing of synthetic clothes in real conditions and at lab scale⋆.
The European Physical Journal Plus 2018, 133, (7), 257.
248, 1028-1035.
Bulletin 2016, 112, (1-2), 39-45.
19321.
187
2016, 23, (21), 22206-22211.
Release of Microplastic Fibers from Laundry. Environmental Science & Technology l 2019,
53, (20), 11735-11744.
188
Table A3-1. Characterization of the textile properties
Surface Structure Type Yarn Density [g/m2] Fiber diameter [µm]
Processed Knit Fleece Filament 185±1* 12.3±2.1**
Unprocessed Knit Interlock Spun 209±1* 12.7±1.5**
* Data taken from previous studies1, 2
**Value determined by randomly measuring 50 fibers with SEM (7 kV, Quanta FEI 650, at
magnification of 500x).
Figure A3-1. SEM images for the fleece and interlock textiles used in this study: A) surface
and B) single yarns from fleece; C) surface and D) single yarns from interlock.
189
Figure A3-2. Side view of the Martindale tester with specimen and abradant indicated.
Figure A3-3. Left: Martindale tester with the steel ring put in place. Right: Experimental set up
to examine the MPF released to air. Here shown is the placement of the double-sided tapes
to capture fibers released into air. Top right is a view from the bottom and the bottom right is
a view from the top when the top plate is removed.
190
Table A3-2. Volume of solution filtered from 150 ml extraction liquid for each series of
experiment.
Fleece Interlock
Experiment Appratus Specimen Abradant Appratus Specimen Abradant
(ml) (ml) (ml) (ml) (ml) (ml)
Abrasion
2 1 2 2 2 3
experiment
Control-
2 1 2 2 2 3
abrasion
Control-
2 1 2 2 2 3
extraction
Control-textile NA 50 5 NA 50 10
Table A3-3. Summary of the experimental conditions and number of samples.
Sample
Experiment Textile
Apparatus Specimen Abradant
Fleece 3 3 3
Abrasion experiment
Interlock 3 3 3
Fleece 1 1 1
Control-abrasion
Interlock 1 1 1
Fleece 3 3 3
Control-textile
Interlock 3 3 3
Fleece NA 3 3
Control-extraction
Interlock NA 3 3
Water wash Fleece 3 3 3
191
Figure A3-4. An example of a composite filter image analyzed for number and length, taken
at a magnification of 200x.
Figure A3-5. An example of a composite filter image analyzed for diameter at a magnification
of 500x.
192
Table A3-4. Assessment of MPFs and fibrils released onto the apparatus. The position
corresponds to the numbers labelled in Figure A3-3.
Replicate (number of fibers)

Position Type Mean number of fibers StD
1 2 3
MPF 0 0 0 0 0
1
Fibril 0 0 0 0 0
MPF 1 0 0 0 1
2
Fibril 0 0 0 0 0
MPF 1 1 0 1 1
3
Fibril 0 0 0 0 0
MPF 0 8 3 4 4
4
Fibril 0 0 1 0 1
MPF 0 7 6 4 4
5
Fibril 0 2 1 1 1
Figure A3-6. Number and distribution of length and diameter of MPFs and fibrils extracted from
fleece and interlock textiles with LAS and water (sum of three replicate experiments). For the
length distribution, the number of MPFs or fibrils plotted per sample was between 112 and 552,
with an average of 260. For the diameter, the number of MPFs or fibrils plotted per sample was
between 14 and 154, with an average of 61. 25th and 75th percentiles are represented by the
boxes and the median is indicated by a line. The release was normalized to the mass of textiles.
Table A3-5. Sum of MPFs and fibrils extracted from abraded samples with water. Unit:
number of MPF/fibril per g textile.
Replicate
Textile Type Mean StD
1 2 3
MPF 120 81 140 120 32
Fleece
Fibril 140 99 180 140 40
193
Table A3-6. Length and diameter of MPFs and fibrils extracted from abraded samples with
water.
Category Textile Type Median Length or diameter [µm]

Fleece MPF 225
Length Fleece Fibril 99
Fleece MPF 12.8
Diameter Fleece Fibril 3.0
Table A3-7. Significant test between the MPF/fibril extracted with LAS and water.
Textile Fragment Length Diameter

MPF 0.052 0.080
Fleece
Fibril 0.000 0.000
Figure A3-7. Number and distribution of length and diameter of MPFs and fibrils extracted from
fleece and interlock textiles after abrasion (summing up three replicates). Shown is the
absolute release of MPFs and fibrils from apparatus, specimen and abradant. For the length
distribution, the number of MPFs or fibrils plotted per sample was between 39 and 357, with
an average of 156. For the diameter, the number of MPFs or fibrils plotted per sample was
between 9 and 87, with an average of 35. 25th and 75th percentiles are represented by the
boxes, the median is indicated by the line.
194
Table A3-8. Number of MPF and fibrils released to the apparatus and extracted from
specimen and abradant after abrasion. Unit: number of MPF/fibril per g textile.
Replicate
Textile Sample Type Mean StD
1 2 3
MPF 320 860 490 560 280
Apparatus
Fibril 150 170 120 150 24
MPF 9000 5700 14000 9600 4300
Fleece Specimen
Fibril 40000 39000 57000 45000 9900
MPF 260 890 1700 950 710
Abradant
Fibril 420 3800 4900 3700 2300
MPF 1100 900 560 850 270
Apparatus
Fibril 1300 1300 540 1000 440
MPF 12000 14000 14000 13000 1300
Interlock Specimen
Fibril 34000 44000 41000 40000 5400
MPF 500 420 450 460 39
Abradant
Fibril 1700 1900 1600 1700 170
Table A3-9. Length of MPF and fibril released to apparatus and extracted from specimen and
abradant after abrasion.
Median length [µm]

Textile Type
MPF 852 181 201
Fleece
Fibril 453 57 53
MPF 483 317 241
Interlock
Fibril 110 92 98
Table A3-10. Diameter of MPF and fibril released to apparatus and extracted from specimen
and abradant after abrasion.
Median diameter [µm]

Textile Type
MPF 11.5 12.0 12.2
Fleece
Fibril 2.9 2.6 2.2
MPF 13.1 12.7 12.2
Interlock
Fibril 7.1 4.4 5.0
195
Table A3-11. Significant test between different abraded samples.
Textile Fragment Sample Length Diameter

MPF Abradant vs specimen 0.671
MPF Abradant vs apparatus 0.000 0.189
MPF Specimen vs apparatus 0.000
Fleece
Fibril Abradant vs specimen 0.005 0.001
Fibril Abradant vs apparatus 0.000 0.019
Fibril Specimen vs apparatus 0.000 0.280
MPF Abradant vs specimen 0.021
MPF Abradant vs apparatus 0.000 0.481
MPF Specimen vs apparatus 0.000
Interlock
Fibril Abradant vs specimen 0.112 0.113
Fibril Abradant vs apparatus 0.000 0.000
Fibril Specimen vs apparatus 0.145 0.007
Figure A3-8. Reliability of filtering an aliquot of the extraction liquid.
196
Table A3-12. Assessment of reliability of the aliquot method.
Subsample
[number per 150 ml Volume
Textile Sample Type solution] Mean StD RSD filtered
[ml]
1 2 3
MPF 1500 1300 2100 1600 400 25% 2
Apparatus
Fibril 370 450 820 550 240 44% 2
MPF 1800 1800 2200 1900 230 12% 1
Fleece Specimen
Fibril 8100 10200 8800 9000 1100 12% 1
MPF 4800 3800 4300 4300 500 12% 2
Abradant
Fibril 14000 12000 10700 12200 1700 14% 2
MPF 1900 1600 1800 1800 150 8.3% 2
Apparatus
Fibril 1900 1600 1600 1700 170 10% 2
MPF 2800 2400 2900 2700 260 10% 2
Interlock Specimen
Fibril 8100 8300 10300 8900 1200 13% 2
MPF 1300 1400 1400 1400 58 4.1% 3
Abradant
Fibril 6000 5800 5200 5700 420 7.4% 3
197
Figure A3-9. Characterization of the fibers of the surface of interlock. The images on the left
show the non-abraded sample, on the right side the images show the abraded sample (12 kPa,
5000 rubs): (A) surface of interlock textile, non-abraded; (B) surface of interlock textile, abraded
specimen; (C) solid fiber ends of interlock textile, non-abraded specimen; (D) fibrillated fiber
ends of interlock textile, abraded specimen. SEM images were taken under 7 kV, the
magnification for (A) and (B) was 100x, for (C), (D), it was 2000x. The scale bars in figure (C)
and (D) applied to all the four small images respectively.
Figure A3-10. Characterization of MPFs and fibrils extracted from interlock: (A) MPFs extracted
from non-abraded interlock textile at a magnification of 2000x; (B) MPFs and fibrils extracted
from abraded interlock textile at a magnification of 500x; (C) MPFs and fibrils extracted from
abraded interlock textile at a magnification of 2000x; (D) MPFs and fibrils extracted from
abraded interlock textile at a magnification of 2500x.
198
Table A3-13. Significant test between the number of MPF/fibril extracted from fleece and
interlock textiles with or without abrasion.
Textile Type Abrasion No abrasion
MPF 0.493 0.067
Fleece vs Interlock
Fibril 0.683 NA
Table A3-14. Levene's test of homogeneity of variances. Test between the number of MPF/fibril
extracted from fleece and interlock textiles with or without abrasion.

MPF 0.929 0.117
Fleece vs Interlock Fibril 0.141 NA
Table A3-15. Shapiro-Wilk Test for normality.

MPF 0.998 0.794
Fleece Fibril 0.748 NA
MPF 0.429 0.799
Interlock Fibril 0.888 NA
Table A3-16. Sum of MPFs and fibrils collected after abrasion. Unit: number of MPF/fibril per
g textile.
Replicate
1 2 3
MPF 1100 2100 3000 2100 930
Fleece
Fibril 3200 6400 8500 6000 2700
MPF 2400 2200 1900 2200 250
Interlock
Fibril 5300 6000 4700 5300 640
Table A3-17. Sum of MPFs and fibrils collected from non-abraded samples. Unit: number of
MPF/fibril per g textile.
Replicate
1 2 3
MPF 160 630 440 410 230
Fleece
Fibril 12 40 39 31 16
MPF 73 100 31 69 36
Interlock
Fibril 4 17 4 Below detection limit -
199
Table A3-18. Length of MPFs and fibrils collected from abraded and non-abraded samples.
Textile Experiment Type Median length [µm]

MPF 290
Abrasion Fibril 56
Fleece
MPF 239
No abrasion Fibril 143
MPF 332
Abrasion Fibril 96
Interlock
MPF 632
No abrasion Fibril NA
Table A3-19. Diameter of MPFs and fibrils collected from abraded and non-abraded samples.
Textile Experiment Type Median diameter [µm]

MPF 11.8
Abrasion Fibril 2.4
Fleece
MPF 11.9
No abrasion Fibril 2.8
MPF 12.9
Abrasion Fibril 4.9
Interlock
MPF 12.7
No abrasion Fibril NA
Table A3-20. Significant test between the MPF/fibril extracted from samples with and without
abrasion.
Textile Fragment Length Diameter

MPF 0.000 0.401
Fleece
Fibril 0.000 0.000
MPF 0.000 0.081
Interlock
Fibril NA NA
Table A3-21. The number of MPFs and fibrils analyzed to determine the length and diameter.
Length Diameter
Sample Textile
MPF Fibril MPF Fibril
Fleece 217 552 58 154
Abraded
Interlock 271 835 48 156
Fleece 139 13 26 9
Non-abraded
Interlock 68 0 21 0
Water wash Fleece 112 158 16 14
200
References
1. Cai, Y.; Yang, T.; Mitrano, D. M.; Heuberger, M.; Hufenus, R.; Nowack, B., Systematic
Study of Microplastic Fiber Release from 12 Different Polyester Textiles during Washing.
2. Cai, Y.; Mitrano, D. M.; Heuberger, M.; Hufenus, R.; Nowack, B., The origin of
microplastic fiber in polyester textiles: The textile production process matters. Journal of
Cleaner Production 2020, 267, 121970.
201
Table A4-1. Estimated masses of FE shells consumed in 34 countries in year of 2019. Unit:
tons/year.
Country Lower boundary Mean Upper boundary

Austria 1.3 2 2.8
Belgium 2.5 3.9 5.3
Bulgaria 0.69 1.1 1.5
Croatia 1.1 1.8 2.4
Cyprus 0.2 0.31 0.42
Czechia 1.7 2.6 3.5
Denmark 0.36 0.56 0.76
Estonia 0.13 0.2 0.28
Finland 0.48 0.74 1
France 11 17 24
Germany 20 31 43
Greece 1.5 2.3 3.1
Hungary 2.9 4.4 6.1
Ireland 0.54 0.84 1.20
Italy 12 19 26
Japan 29 58 87
Latvia 0.12 0.18 0.25
Lithuania 0.19 0.29 0.4
Luxembourg 0.13 0.19 0.26
Malta 0.09 0.14 0.19
Mexico 33 66 100
Netherlands 2.7 4.1 5.6
Norway 0.53 0.82 1.1
Poland 5.8 8.9 12
Portugal 3.5 5.3 7.3
Romania 3 4.6 6.3
Slovakia 0.98 1.5 2.1
Slovenia 0.35 0.53 0.73
Spain 19 29 40
Sweden 1.1 1.7 2.3
Switzerland 0.82 1.3 1.7
United Kingdom 11 17 23
USA 49 99 148
Vietnam 23 47 70
202
Table A4-2. Estimated trends of consumed amount of FE shells release from 2010 to 2019.
Unit: unitless.
Year Global Japan Mexico USA Vietnam

2010 0.23 0 0.16 0.13 0.26
2011 0.26 0 0.33 0.29 0.52
2012 0.82 0.04 0.65 0.6 1.04
2013 0.83 0.09 1.02 0.47 2.26
2014 0.97 0.17 1.02 0.86 2.43
2015 0.78 0.4 0.8 0.72 1.58
2016 0.77 0.84 0.83 0.75 1.35
2017 0.91 0.86 0.92 1.27 1.16
2018 1 0.9 0.96 0.98 1.15
2019 1 1 1 1 1
203
Table A4-3. WWTP removal efficiency of microplastics.
Study Location Removal efficiency

Akarsu, et al.1 Turkey 0.57
Bayo, et al.2 Spain 0.988, 0.9553
Bayo, et al.3 Spain 0.903
Conley, et al.4 USA 0.976, 0.852, 0.855
Edo, et al.5 Spain 0.937
Gies, et al.6 Canada 0.983
Liu, et al.7 China 0.644
Magni, et al.8 Italy 0.65
Mintenig, et al.9 Germany 0.97
Murphy, et al.10 UK 0.984
0.995, 0.987, 0.994, 0.9977, 0.9995, 0.9999, 0.999,
0.9995, 0.99995, 0.999, 0.99994, 0.9993, 0.9998,
0.9998, 0.99973, 0.9988, 0.995, 0.995, 0.998, 0.9994,
0.9997, 0.998, 0.999, 0.999, 0.998, 0.967, 0.998, 0.9997,
Park, et al.11 Korea 0.999, 0.9999, 0.997
Wang, et al.12 China 0.44, 0.98, 0.81, 0.35, 0.56, 0.78, 0.6, 0.54, 0.38
0.9059, 0.918, 0.9183, 0.9715, 0.9612, 0.9654, 0.9576,
Xu, et al.13 China 0.8917, 0.9656, 0.9602, 0.9651, 0.9516
Talvitie and
Heinonen14 Russia 0.9563
Magnusson and
Norén15 Swedish 0.9969
Dris, et al.16 Paris 0.89
Talvitie, et al.17 Finland 0.98
Carr, et al.18 USA 0.999
Netherland
Leslie, et al.19 s 0.72
Ziajahromi, et
al.20 Australia 0.9
Gundogdu, et
al.21 Turkey 0.79, 0.73
Lares, et al.22 Finland 0.898
Lee and
Kim23 Korea 0.985
Simon, et al.24 Denmark 0.993
Wiśniowskaa, et
al.25 Poland 0.97
Long, et al.26 China 0.951, 0.97, 0.995
204
Exfiltration
5 4
1 Sewage
WWTP
system
6
2 On-site
Wastewater 7 Overflow
treatment
8
3 Surface
water
Figure A4-1. Pathways considered for wastewater management.
205
Table A4-4. Sources of transfer coefficients about wastewater management.
No of Flow to Source Comments

flow in
Figure
A4-1
1 Sewage system European countries: Eurostat27, The most recent data were
extracted from the database
OECD28
USA: OECD28
Mexico: CNA29
Japan: OECD28
Vietnam: ARCOWA30
2 On-site Same as Rajkovic, et al.31: the Including septic tanks, pit-dry

treatment total amount equals to the and flush/pour flush pit 31
fraction of wastewater not flowing
to the sewer. Original data The value equals to (1-
comes from Cairns-Smith, et al.32 wastewater to sewer)*11/14
3 Surface water Including open defecation 31

(from
wastewater) The value equals to (1-
wastewater to sewer)*3/14
4 WWTP European countries: Eurostat27, The most recent data were

extracted from the database
OECD28
USA: OECD28
Mexico: CNA29
Japan: OECD28
Vietnam: ARCOWA30
5 Exfiltration Rutsch, et al.33, Rajkovic, et Wastewater which is exfiltrated

al.31 to the subsurface
6 Overflow Rajkovic, et al.31 -
7 Surface water Estimated from fraction of wastewater collected by sewer but not
(from sewer) going to WWTP
8 Surface water Assuming 100% of overflow going to surface water for the countries
(from overflow)
206
Table A4-5. Sewage connection rate and WWTP treatment rate collected for each country.
Sewer connection WWTP treatment

Country Source Year
rate rate
Austria OECD 2018 100% 96%

Belgium Eurostat, OECD 2017 88% 83%
Bulgaria Eurostat 2017 76% 63%
Croatia Eurostat 2017 55% 53%
Cyprus EEA, Eurostat 2014 42% 30%
Czechia OECD 2018 82% 82%
Denmark OECD 2018 100% 92%
Estonia Eurostat, OECD 2017 83% 83%
Finland OECD 2018 85% 85%
France OECD 2018 81% 81%
Germany Eurostat, OECD 2016 99% 97%
Greece Eurostat, OECD 2016 93% 93%
Hungary OECD 2018 80% 80%
Ireland Eurostat, OECD 2017 64% 63%
EEA, Eurostat, 2015,
Italy
OECD 2009 94% 63%
Japan OECD 2017 79% 79%
Latvia OECD 2018 80% 80%
Lithuania OECD 2018 79% 76%
Luxembourg Eurostat, OECD 2017 100% 99%
Malta Eurostat 2017 99% 99%
Mexico CNA29 - 91% 64%
Netherlands OECD 2018 100% 100%
Norway OECD 2018 87% 85%
Poland OECD 2018 74% 74%
Portugal Eurostat, OECD 2017 89% 88%
Romania Eurostat 2017 51% 50%
Slovakia Eurostat 2017 68% 67%
Slovenia OECD 2018 72% 68%
Spain OECD 2016 89% 88%
Sweden Eurostat, OECD 2017 87% 87%
EEA, Eurostat, 2015,
Switzerland
OECD 2013 98% 98%
United 2015,
OECD, EEA
Kingdom 2010 100% 100%
USA OECD 2012 76% 76%
Vietnam* ARCOWA30 - 23% 13%
* For the urban area of Vietnam, the sewage connection rate was 60% and 21% of
wastewater was reported to be treated by ARCOWA30. Assumption was made for the rural
area that 0% of wastewater was collected and treated. Then the final value was weighted by
the percentage of urban and rural population34.
207
Figure A4-2. Pathways considered for sludge management.
Table A4-6. Source of transfer coefficients regarding sludge disposal.
No of flow Flow to Source Comment

in Figure
A4-2
1 Soil European countries: Eurostat35, The most recently

OECD36 available data were
2 Landfill extracted from the
USA: Mahapatra, et al.37 database
3 Incineration
Mexico: CNA29
Japan: MLIT38
Vietnam: ARCOWA30
208
Table A4-7. Data collected for sludge disposal.
Country Source Year Agriculture Landfill Incineration

Austria Eurostat 2016 43% 0% 57%
Belgium Eurostat 2010 13% 0% 87%
Bulgaria Eurostat 2017 79% 21% 0%
Croatia Eurostat 2017 36% 64% 0%
Cyprus Eurostat 2016 73% 0% 27%
Czechia Eurostat 2013 90% 7.3% 2.4%
Denmark Eurostat 2010 68% 1.3% 31%
Estonia Eurostat 2009 83% 17% 0%
Finland OECD 2010 98% 2.1% 0%
France Eurostat 2017 79% 1.7% 19%
Germany Eurostat 2016 35% 0% 65%
Greece Eurostat 2014 29% 36% 35%
Hungary Eurostat 2017 72% 0.55% 28%
Ireland Eurostat 2017 100% 0% 0%
Italy Eurostat 2010 39% 57% 4.5%
Japan MLIT38 2018 15% 24% 61%
Latvia Eurostat 2017 99% 0% 1.1%
Lithuania Eurostat 2017 92% 7.9% 0%
Luxembourg Eurostat 2017 81% 0% 19%
Malta Eurostat 2017 0% 100% 0%
Mexico CNA29 2018

40% 60% 0%
Netherlands Eurostat 2016 1.3% 0% 98%
Norway Eurostat 2017 86% 14% 0%
Poland Eurostat 2017 53% 6.0% 42%
Portugal Eurostat 2016 73% 27% 0%
Romania Eurostat 2017 18% 82% 0%
Slovakia Eurostat 2017 55% 18% 27%
Slovenia Eurostat 2017 3.1% 2.3% 95%
Spain Eurostat 2012 80% 16% 4.2%
Sweden Eurostat 2016 94% 2.3% 3.2%
Switzerland Eurostat 2013 0% 0% 100%
United Kingdom Eurostat 2012 78% 0% 21%
USA Mahapatra, et al.37 - 54% 31% 15%
Vietnam* ARCOWA30 - 20% 80% 0%
*According to the report, most of the sludge in Vietnam was dumped in landfill 30. Therefore,
an assumption was made that 80% of the sludge flowed to landfill, while 20% was applied on
agricultural soil.
209
Figure A4-3. Pathways considered for solid waste management
Table A4-8. Source of transfer coefficients regarding solid waste management.
No of flow Flow to Source Comment

in Figure
A4-3
1 Incineration European countries: Eurostat39, The most recently

OECD40 available data were
2 Landfill extracted from the
USA, Mexico and Japan: OECD40 database
3 Recycling
Vietnam: Nguyen41
210
Table A4-9. Data collected for solid waste management.
Country Source Year Landfill Incineration Recycling

Austria Eurostat, OECD 2018 3% 58% 38%
Belgium Eurostat, OECD 2018 1.2% 55% 44%
Bulgaria Eurostat 2018 62% 7.4% 30%
Croatia Eurostat 2018 75% 0.10% 25%
Cyprus Eurostat 2017 84% 0% 16%
Czechia Eurostat 2018 53% 18% 29%
Denmark Eurostat, OECD 2018 1.2% 60% 38%
Estonia Eurostat, OECD 2018 25% 47% 28%
Finland Eurostat, OECD 2018 0.80% 66% 34%
France Eurostat, OECD 2018 26% 43% 31%
Germany OECD 2018 0.30% 39% 61%
Greece OECD 2017 84% 1.1% 15%
Hungary Eurostat, OECD 2018 54% 15% 32%
Ireland OECD 2017 26% 37% 37%
Italy Eurostat, OECD 2018 31% 28% 42%
Japan OECD 2017 1.0% 79% 20%
Latvia Eurostat, OECD 2018 74% 2.4% 24%
Lithuania Eurostat, OECD 2018 40% 20% 40%
Luxembourg Eurostat, OECD 2018 7.9% 56% 36%
Malta Eurostat 2018 93% 0% 7.0%
Mexico OECD 2012 93% 0% 7.0%
Netherlands Eurostat, OECD 2018 2.0% 60% 38%
Norway Eurostat, OECD 2018 3.7% 60% 36%
Poland Eurostat, OECD 2018 45% 26% 29%
Portugal Eurostat, OECD 2018 62% 23% 16%
Romania Eurostat 2018 86% 5.3% 8.9%
Slovakia Eurostat 2018 61% 9.2% 30%
Slovenia Eurostat, OECD 2018 15% 17% 68%
Spain Eurostat, OECD 2018 62% 16% 22%
Sweden Eurostat, OECD 2018 0.80% 64% 36%
Switzerland Eurostat, OECD 2018 0% 61% 39%
United Kingdom Eurostat, OECD 2018 18% 48% 34%
USA OECD 2017 57% 14% 29%
Vietnam Nguyen41 NA 100% 0% 0%
211
Table A4-10. Area of surface water. Two databases from FAO, land use and land cover
databases, were considered42, 43. Unit: 1000 ha.
Land cover
Country Land use Average*
MODIS CCI_LC
Austria 136 25 71 92
Belgium 25 8.6 16 19
Bulgaria 244 64 125 169
Croatia 63 41 85 63
Cyprus 1.0 1.5 7.0 2.6
Czechia 166 5.1 60 99
Denmark 93 214 264 166
Estonia 187 202 223 200
Finland 3453 2001 3331 3060
France 153 222 430 239
Germany 788 213 447 559
Greece 306 224 342 295
Hungary 177 83 136 143
Ireland 139 120 197 149
Italy 720 275 402 529
Japan 1341 619 907 1052
Latvia 246 63 123 170
Lithuania 265 33 121 171
Luxembourg 16 0 0.70 8.2
Malta NA 0.11 0.81 0.46
Mexico 2043 1187 1585 1715
Netherlands 372 78 120 236
Norway 2010 1357 2211 1897
Poland 651 137 454 473
Portugal 62 27 94 61
Romania 832 188 289 535
Slovakia 95 7.3 32 57
Slovenia 13 0.56 4.2 7.8
Spain 639 128 430 459
Sweden 4012 2145 3854 3506
Switzerland 177 103 142 150
United Kingdom 168 232 453 255
USA 68592 9210 18402 41199
Vietnam 2116 333 731 1324
* The average was calculated by giving a 50% weight to the values from land use and land
cover databases.
212
Table A4-11. Volume of sludge. Unit: thousand tons.
Applied on
Country Source Year Total
agricultural soil
Austria Eurostat35 2016 238 102
Belgium Eurostat35 2010 131 17
Bulgaria Eurostat35 2017 45 36
Croatia Eurostat35 2017 3.4 1.2
Cyprus Eurostat35 2016 7.4 5.4
Czechia Eurostat35 2013 260 234
Denmark Eurostat35 2010 115 78
Estonia Eurostat35 2009 22 18
Finland OECD36 2010 143 140
France Eurostat35 2017 809 639
Germany Eurostat35 2016 1773 621
Greece Eurostat35 2014 119 35
Hungary Eurostat35 2017 232 167
Ireland Eurostat35 2017 59 59
Italy Eurostat35 2010 954 372
Japan MLIT38 2018 2279 342
Latvia Eurostat35 2017 25 25
Lithuania Eurostat35 2017 41 38
Luxembourg Eurostat35 2017 8.6 7.0
Malta Eurostat35 2017 10 0.0
Mexico CNA29 2018 110 44
Netherlands Eurostat35 2016 325 4.2
Norway Eurostat35 2017 121 104
Poland Eurostat35 2017 585 310
Portugal Eurostat35 2016 119 87
Romania Eurostat35 2017 283 51
Slovakia Eurostat35 2017 55 30
Slovenia Eurostat35 2017 37 1.1
Spain Eurostat35 2012 1083 866
Sweden Eurostat35 2016 191 180
Switzerland Eurostat35 2013 195 0.0
United Kingdom Eurostat35 2012 1078 841
37 3518
USA Mahapatra, et al. - 6514
Vietnam* ARCOWA30, estimated - 28 5.6
*The sludge volume for Vietnam was estimated from the total volume of wastewater treated
per day (750 000 m3) according to the data provided by 30. Then the calculation was done via
the website https://www.lenntech.com/wwtp/calculate-daily-sludge-production.htm and the
typical parameter was taken. The annual sludge volume was estimated to be 27 700 t.
213
Calculation of PECs
∑𝑖 𝐹𝑙𝑜𝑤𝑓𝑟𝑒𝑠ℎ𝑤𝑎𝑡𝑒𝑟𝑖 𝑅𝑒𝑠𝑖𝑑𝑒𝑛𝑐𝑒 𝑡𝑖𝑚𝑒

𝑃𝐸𝐶𝑓𝑟𝑒𝑠ℎ𝑤𝑎𝑡𝑒𝑟 = ∗
𝑉𝑜𝑙𝑢𝑚𝑒𝑓𝑟𝑒𝑠ℎ𝑤𝑎𝑡𝑒𝑟 365 𝑑𝑎𝑦
Where:
𝐹𝑙𝑜𝑤𝑓𝑟𝑒𝑠ℎ𝑤𝑎𝑡𝑒𝑟𝑖 : mass flows to the freshwater
𝑉𝑜𝑙𝑢𝑚𝑒𝑓𝑟𝑒𝑠ℎ𝑤𝑎𝑡𝑒𝑟 : calculated by multiplying the area of the freshwater (Table A9) and the
depth (3 m) as suggested by ECHA44
𝑅𝑒𝑠𝑖𝑑𝑒𝑛𝑐𝑒 𝑡𝑖𝑚𝑒: 40 days 44
∑𝑖 𝐹𝑙𝑜𝑤𝑠𝑒𝑑𝑖𝑚𝑒𝑛𝑡𝑖
𝑃𝐸𝐶𝑠𝑒𝑑𝑖𝑚𝑒𝑛𝑡 =
𝑉𝑜𝑙𝑢𝑚𝑒𝑠𝑒𝑑𝑖𝑚𝑒𝑛𝑡
Where:
𝐹𝑙𝑜𝑤𝑠𝑒𝑑𝑖𝑚𝑒𝑛𝑡𝑖 : mass flows to the sediment which equals to the flows to the freshwater
𝑉𝑜𝑙𝑢𝑚𝑒𝑠𝑒𝑑𝑖𝑚𝑒𝑛𝑡 : calculated by multiplying the area of the sediment which equals to

freshwater area (Table A9), the depth (0.03 m) as suggested by ECHA44 and the density of
dry sediment (260 kg/m3) 45
∑𝑖 𝐹𝑙𝑜𝑤𝑆𝑙𝑢𝑑𝑔𝑒−𝑡𝑟𝑒𝑎𝑡𝑒𝑑 𝑠𝑜𝑖𝑙𝑖
𝑃𝐸𝐶𝑆𝑙𝑢𝑑𝑔𝑒−𝑡𝑟𝑒𝑎𝑡𝑒𝑑 𝑠𝑜𝑖𝑙 =
𝑀𝑎𝑠𝑠𝑆𝑙𝑢𝑑𝑔𝑒−𝑡𝑟𝑒𝑎𝑡𝑒𝑑 𝑠𝑜𝑖𝑙
𝐹𝑙𝑜𝑤𝑆𝑙𝑢𝑑𝑔𝑒−𝑡𝑟𝑒𝑎𝑡𝑒𝑑 𝑠𝑜𝑖𝑙 : mass flows to the sludge treated soil
𝑀𝑎𝑠𝑠𝑆𝑙𝑢𝑑𝑔𝑒−𝑡𝑟𝑒𝑎𝑡𝑒𝑑 𝑠𝑜𝑖𝑙 : calculated by multiplying the area, the depth and the density of the
sludge-treated soil. The area was obtained by dividing the amount of sludge applied on soils
(Table A10) by the application rate of 5000 kg/ha dry weight per year suggested by ECHA44.
44
The depth of agricultural soil was 0.2 m and the density was assumed to be 1500 kg/m3 45
214
Table A4-12. Percentage of mass flows to different compartments.
Compartment Europe Japan Mexico USA Vietnam

Sludge-treated soil 38% 9.5% 10% 32% 2.0%
Surface water 16% 13% 33% 13% 26%
Incineration 22% 41% 0% 10% 0%
Landfill 10% 15% 44% 21% 13%
Subsurface 14% 21% 12% 24% 59%
215
Table A4-13. PECs of FEs for the freshwater compartment.
Country Unit Q5 Mode Mean Q95

Austria µg/L 0.0040 0.0057 0.012 0.037
Belgium µg/L 0.056 0.078 0.13 0.34
Bulgaria µg/L 0.0031 0.0042 0.0054 0.010
Croatia µg/L 0.0094 0.014 0.017 0.035
Cyprus µg/L 0.073 0.10 0.11 0.17
Czechia µg/L 0.0045 0.0063 0.012 0.038
Denmark µg/L 0.00090 0.0013 0.0022 0.0059
Estonia µg/L 0.00018 0.00025 0.00048 0.0015
Finland µg/L 0.000039 0.000056 0.00011 0.00036
France µg/L 0.013 0.019 0.035 0.106
Germany µg/L 0.0072 0.010 0.026 0.093
Greece µg/L 0.00091 0.0013 0.0033 0.012
Hungary µg/L 0.0057 0.0080 0.015 0.045
Ireland µg/L 0.0017 0.0024 0.0033 0.0076
Italy µg/L 0.030 0.043 0.049 0.078
Japan µg/L 0.0095 0.014 0.026 0.078
Latvia µg/L 0.00020 0.00028 0.00051 0.0015
Lithuania µg/L 0.00045 0.00062 0.00097 0.0025
Luxembourg µg/L 0.0028 0.0040 0.011 0.039
Malta µg/L 0.027 0.039 0.12 0.49
Mexico µg/L 0.026 0.040 0.047 0.080
Netherlands µg/L 0.0017 0.0024 0.0074 0.028
Norway µg/L 0.000086 0.00012 0.00022 0.00067
Poland µg/L 0.0040 0.0057 0.0094 0.026
Portugal µg/L 0.013 0.019 0.04 0.13
Romania µg/L 0.0029 0.0041 0.0053 0.011
Slovakia µg/L 0.0066 0.0095 0.014 0.035
Slovenia µg/L 0.023 0.031 0.044 0.10
Spain µg/L 0.011 0.015 0.031 0.099
Sweden µg/L 0.000074 0.00010 0.00022 0.00073
Switzerland µg/L 0.00087 0.0012 0.0036 0.014
United Kingdom µg/L 0.0055 0.0080 0.027 0.11
USA µg/L 0.00045 0.00069 0.001 0.0034
Vietnam µg/L 0.020 0.032 0.034 0.050
216
Table A4-14. PECs of FEs for the sediment compartment.

Austria µg/kg 110 150 310 970
Belgium µg/kg 1600 2100 3400 8800
Bulgaria µg/kg 89 120 140 270
Croatia µg/kg 270 360 460 930
Cyprus µg/kg 2100 2800 3000 4300
Czechia µg/kg 130 170 320 980
Denmark µg/kg 25 35 57 150
Estonia µg/kg 5.0 6.6 13 39
Finland µg/kg 1.1 1.5 3.0 9.4
France µg/kg 380 500 930 2800
Germany µg/kg 200 270 690 2400
Greece µg/kg 26 34 87 310
Hungary µg/kg 160 220 400 1200
Ireland µg/kg 48 63 88 200
Italy µg/kg 860 1100 1300 2000
Japan µg/kg 160 220 390 1200
Latvia µg/kg 5.6 7.5 14 40
Lithuania µg/kg 13 17 26 66
Luxembourg µg/kg 78 110 280 1000
Malta µg/kg 770 1000 3300 12000
Mexico µg/kg 820 1100 1300 2100
Netherlands µg/kg 47 65 200 740
Norway µg/kg 2.5 3.1 5.9 17
Poland µg/kg 120 150 250 690
Portugal µg/kg 380 490 1100 3400
Romania µg/kg 83 110 140 280
Slovakia µg/kg 190 250 370 930
Slovenia µg/kg 660 840 1200 2700
Spain µg/kg 300 390 810 2500
Sweden µg/kg 2.1 2.7 5.8 19
Switzerland µg/kg 24 33 95 350
United Kingdom µg/kg 150 220 720 2800
USA µg/kg 13 17 29 82
Vietnam µg/kg 1100 1400 1500 2100
217
Table A4-15. PECs of FEs for the sludge-treated soil compartment.

Austria µg/kg 45 85 82 110
Belgium µg/kg 130 250 260 410
Bulgaria µg/kg 83 160 150 190
Croatia µg/kg 1400 2700 2700 4100
Cyprus µg/kg 64 120 120 170
Czechia µg/kg 47 86 81 99
Denmark µg/kg 25 47 44 57
Estonia µg/kg 45 81 76 95
Finland µg/kg 26 48 44 54
France µg/kg 100 180 170 220
Germany µg/kg 95 180 180 250
Greece µg/kg 95 180 180 250
Hungary µg/kg 87 160 150 190
Ireland µg/kg 50 94 88 110
Italy µg/kg 66 130 120 180
Japan µg/kg 58 110 110 170
Latvia µg/kg 33 61 57 70
Lithuania µg/kg 31 57 53 66
Luxembourg µg/kg 130 240 220 270
Malta µg/kg 0 0 0 0
Mexico µg/kg 970 1900 1900 3100
Netherlands µg/kg 63 120 130 220
Norway µg/kg 33 61 57 71
Poland µg/kg 61 120 110 150
Portugal µg/kg 220 410 390 490
Romania µg/kg 40 73 81 130
Slovakia µg/kg 100 190 180 240
Slovenia µg/kg 49 94 100 170
Spain µg/kg 140 250 230 290
Sweden µg/kg 45 83 77 93
Switzerland µg/kg 0 0 0 0
United Kingdom µg/kg 93 170 160 200
USA µg/kg 58 110 100 140
Vietnam µg/kg 1560 3000 3600 6200
218
219
Figure A4-4. Correlation plots of PEC in water, sediment and sludge-treated (ST) soil vs.
population density, consumption, consumption per capita, percentage of sludge applied on soil,
total sludge volume, volume of sludge applied on soil, area of surface water, sewer connection
rate, WWTP treatment rate, and precipitation.
220
Table A4-16. Statistical analysis of the correlations shown in Figure A4-4.
Correlation Coefficients Estimate Pr(>|t|) Signif. R2

b 0.011 0.065 .
PEC freshwater = a*Population density + b 0.33
a 0.076 0 ***
b 297.3 0.068 .
PEC sediment = a*Population density + b 0.33
a 2077.5 0 ***
b 364.37 0.036 *
PEC ST soil = a*Population density + b -0.03
a -62.94 0.906
b 0.025 0.001 ***
PEC freshwater = a*Consumption + b -0.03
a 0 0.933
PEC sediment = a*Cumulative consumption + b 634.405 0.002 **
-0.02
b a 0.414 0.656
b 134.23 0.327
PEC ST soil = a*Cumulative consumption + b 0.23
a 2.259 0.002 **
PEC freshwater = a*Consumption per capita + b 0.001 0.955
0.09
b a 0.086 0.046 *
PEC sediment = a*Cumulative consumption b 52.46 0.866
0.12
per capita + b a 291.3 0.028 *
PEC ST soil = a*Cumulative consumption per b -656.04 0.002 **
0.5
capita + b a 472.5 0 ***
PEC ST soil = a*% of sludge applied on soil+ b 658.8 0.018 *
0.02
b a -553.3 0.188
b 396.243 0.012 *
PEC ST soil = a*Total volume of sludge + b -0.02
a -0.082 0.487
PEC ST soil = a*Volume of sludge applied on b 391.859 0.012 *
-0.02
soil + b a -0.147 0.51
b 0.026 0 ***
PEC freshwater = a*Surfacewater area + b -0.01
a 0 0.395
PEC freshwater = a*Sewer connection rate + b 0.036 0.202
-0.03
b a -0.014 0.681
b 0.048 0.051 .
PEC freshwater = a*WWTP treatment rate + b 0
a -0.03 0.32
b 0.031 0.065 .
PEC freshwater = a*Precipitation + b -0.03
a 0 0.674
b 784.443 0.09 .
PEC sediment = a*Precipitation + b -0.03
a -0.127 0.795
b -503.203 0.156
PEC ST soil = a*Precipitation + b 0.15
a 0.985 0.013 *
Signif. codes: 0 ‘***’ 0.001 ‘**’ 0.01 ‘*’ 0.05 ‘.’ 0.1 ‘ ’
221
Table A4-17. Overview of ecotoxicological tests.
Compartm FE shells Duratio Range (mg shells

ent Guideline suspension Species Endpoint n /L water or kg soil) Effect
A 23.8% yield inhibition was
OECD Raphidocelis observed at the lowest
Fresh water 201 Commercial subcapitata Growth 72 h 0.00535 to 0.0535 concentration
OECD Raphidocelis No effect the highest
Fresh water 201 Purified subcapitata Growth 72 h 0.0535 to 2.67 concentration
OECD Daphnia No effect the highest
Fresh water 202 Commercial magna immobilisation 72 h 0.00535 to 0.0535 concentration
OECD survival or No effect the highest
Fresh water 236 Commercial Danio rerio growth 96 h 0.00535 to 0.0535 concentration
OECD Lumbriculus mortality and No effect the highest
Sediment 225 Commercial variegatus weight 28 d 0.535 to 5.35 concentration
Soil
OECD microorganis carbon No effect the highest
Soil 217 Commercial ms transformation 28 d 0.535 to 5.35 concentration
Soil
ISO microorganis nitrogen No effect the highest
Soil 15685 Commercial ms transformation 28 d 0.535 to 5.35 concentration
OECD The control didn't meet the
Soil 208 Commercial Avena sativa growth 14 d 0.535 to 5.35 criteria
emergence,
OECD survival and No effect the highest
Soil 208 Purified Avena sativa growth 14 d 1.09 to 9.1 concentration
emergence,
post-
ermegence
OECD survival, No effect the highest
Soil 208 Commercial Zea mays growth 14 d 0.535 to 5.35 concentration
222
An effect on shoot fresh weight
OECD Phaseolus shoot fresh at the highest concentration and
Soil 208 Commercial aureus weight 14 d 0.535 to 5.35 a NOEC value of 2.675 mg/kg
Emergence
rate, post-
emergence No adverse effect at any
OECD Phaseolus survival and concentration and a NOEC
Soil 208 Purified aureus biomass 14 d 1.09 to 9.1 value > 9.1 mg/kg
Emergence
rate, post-
emergence
OECD survival and No effect the highest
Soil 208 Commercial Brassica rapa biomass 14 d 0.535 to 5.35 concentration
An effect on the reproduction at
the mid and highest
OECD concentration and a NOEC value
Soil 222 Commercial Eisenia andrei reproduction 56 d 0.535 to 5.35 of 0.535 mg/kg
No adverse effect at any
OECD reproduction, concentration and a NOEC
Soil 222 Purified Eisenia andrei survival, weight 56 d 1.09 to 9.1 value > 9.1 mg/kg
223
Table A4-18. A summary of the PEC/HONEC ratios for freshwater.
Country Q5 Median Mean Q95

Austria 1.5E-06 2.8E-06 4.3E-06 1.4E-05
Belgium 2.1E-05 3.5E-05 4.7E-05 1.3E-04
Bulgaria 1.2E-06 1.8E-06 2.0E-06 3.9E-06
Croatia 3.5E-06 5.6E-06 6.5E-06 1.3E-05
Cyprus 2.7E-05 4.1E-05 4.2E-05 6.3E-05
Czechia 1.7E-06 3.0E-06 4.6E-06 1.4E-05
Denmark 3.4E-07 6.0E-07 8.2E-07 2.2E-06
Estonia 6.6E-08 1.2E-07 1.8E-07 5.6E-07
Finland 1.5E-08 2.6E-08 4.2E-08 1.3E-07
France 5.0E-06 8.7E-06 1.3E-05 4.0E-05
Germany 2.7E-06 5.4E-06 9.7E-06 3.5E-05
Greece 3.4E-07 6.7E-07 1.2E-06 4.4E-06
Hungary 2.1E-06 3.7E-06 5.5E-06 1.7E-05
Ireland 6.3E-07 1.0E-06 1.2E-06 2.9E-06
Italy 1.1E-05 1.7E-05 1.8E-05 2.9E-05
Japan 3.5E-06 6.7E-06 9.8E-06 2.9E-05
Latvia 7.4E-08 1.3E-07 1.9E-07 5.7E-07
Lithuania 1.7E-07 2.7E-07 3.6E-07 9.5E-07
Luxembourg 1.0E-06 2.2E-06 4.0E-06 1.4E-05
Malta 1.0E-05 2.3E-05 4.7E-05 1.8E-04
Mexico 9.7E-06 1.6E-05 1.8E-05 3.0E-05
Netherlands 6.3E-07 1.4E-06 2.8E-06 1.1E-05
Norway 3.2E-08 5.6E-08 8.3E-08 2.5E-07
Poland 1.5E-06 2.6E-06 3.5E-06 9.8E-06
Portugal 5.0E-06 9.0E-06 1.5E-05 4.9E-05
Romania 1.1E-06 1.7E-06 2.0E-06 4.0E-06
Slovakia 2.5E-06 4.1E-06 5.3E-06 1.3E-05
Slovenia 8.6E-06 1.4E-05 1.7E-05 3.8E-05
Spain 4.0E-06 7.2E-06 1.1E-05 3.7E-05
Sweden 2.8E-08 5.0E-08 8.2E-08 2.7E-07
Switzerland 3.3E-07 7.0E-07 1.4E-06 5.1E-06
United Kingdom 2.1E-06 4.9E-06 1.0E-05 4.1E-05
USA 1.7E-07 3.2E-07 4.4E-07 1.3E-06
Vietnam 7.5E-06 1.2E-05 1.3E-05 1.9E-05
224
Table A4-19. A summary of the PEC/HONEC ratios for sediment.

Austria 2.1E-02 3.7E-02 5.8E-02 1.8E-01
Belgium 3.0E-01 4.6E-01 6.3E-01 1.6E+00
Bulgaria 1.7E-02 2.4E-02 2.7E-02 5.1E-02
Croatia 5.0E-02 7.4E-02 8.6E-02 1.7E-01
Cyprus 4.0E-01 5.4E-01 5.6E-01 8.0E-01
Czechia 2.4E-02 3.9E-02 6.0E-02 1.8E-01
Denmark 4.7E-03 7.9E-03 1.1E-02 2.9E-02
Estonia 9.4E-04 1.5E-03 2.4E-03 7.3E-03
Finland 2.1E-04 3.5E-04 5.6E-04 1.8E-03
France 7.0E-02 1.1E-01 1.7E-01 5.2E-01
Germany 3.8E-02 7.2E-02 1.3E-01 4.5E-01
Greece 4.8E-03 8.9E-03 1.6E-02 5.7E-02
Hungary 3.0E-02 4.9E-02 7.3E-02 2.2E-01
Ireland 9.0E-03 1.3E-02 1.6E-02 3.7E-02
Italy 1.6E-01 2.3E-01 2.4E-01 3.8E-01
Japan 3.0E-02 5.0E-02 7.4E-02 2.2E-01
Latvia 1.0E-03 1.7E-03 2.5E-03 7.4E-03
Lithuania 2.4E-03 3.6E-03 4.8E-03 1.2E-02
Luxembourg 1.5E-02 2.9E-02 5.3E-02 1.9E-01
Malta 1.4E-01 3.1E-01 6.2E-01 2.3E+00
Mexico 1.5E-01 2.2E-01 2.4E-01 3.9E-01
Norway 4.6E-04 7.3E-04 1.1E-03 3.3E-03
Poland 2.1E-02 3.4E-02 4.7E-02 1.3E-01
Portugal 7.1E-02 1.2E-01 2.0E-01 6.4E-01
Romania 1.6E-02 2.3E-02 2.6E-02 5.2E-02
Slovakia 3.5E-02 5.4E-02 7.0E-02 1.7E-01
Slovenia 1.2E-01 1.8E-01 2.2E-01 5.0E-01
Spain 5.7E-02 9.4E-02 1.5E-01 4.8E-01
Sweden 3.9E-04 6.6E-04 1.1E-03 3.5E-03
Switzerland 4.5E-03 9.2E-03 1.8E-02 6.6E-02
USA 2.4E-03 3.9E-03 5.5E-03 1.5E-02
Vietnam 2.0E-01 2.8E-01 2.8E-01 3.8E-01
225
Table A4-20. A summary of the PEC/HONEC ratios for sludge-treated soil.

Austria 4.9E-03 9.1E-03 9.0E-03 1.2E-02
Belgium 1.4E-02 2.8E-02 2.9E-02 4.5E-02
Bulgaria 9.2E-03 1.7E-02 1.6E-02 2.1E-02
Croatia 1.5E-01 3.0E-01 3.0E-01 4.5E-01
Cyprus 7.1E-03 1.3E-02 1.3E-02 1.9E-02
Czechia 5.2E-03 9.2E-03 8.9E-03 1.1E-02
Denmark 2.8E-03 5.0E-03 4.9E-03 6.2E-03
Estonia 4.9E-03 8.7E-03 8.4E-03 1.0E-02
Finland 2.9E-03 5.1E-03 4.9E-03 5.9E-03
France 1.1E-02 2.0E-02 1.9E-02 2.4E-02
Germany 1.0E-02 2.0E-02 2.0E-02 2.8E-02
Greece 1.0E-02 2.0E-02 1.9E-02 2.7E-02
Hungary 9.5E-03 1.7E-02 1.7E-02 2.1E-02
Ireland 5.5E-03 1.0E-02 9.7E-03 1.2E-02
Italy 7.2E-03 1.4E-02 1.4E-02 2.0E-02
Japan 6.4E-03 1.2E-02 1.3E-02 1.9E-02
Latvia 3.7E-03 6.5E-03 6.3E-03 7.7E-03
Lithuania 3.4E-03 6.1E-03 5.9E-03 7.3E-03
Luxembourg 1.4E-02 2.5E-02 2.4E-02 3.0E-02
Malta 0 0 0 0
Mexico 1.1E-01 2.1E-01 2.1E-01 3.4E-01
Norway 3.7E-03 6.6E-03 6.3E-03 7.8E-03
Poland 6.7E-03 1.2E-02 1.2E-02 1.7E-02
Portugal 2.5E-02 4.5E-02 4.3E-02 5.4E-02
Romania 4.3E-03 8.7E-03 8.9E-03 1.4E-02
Slovakia 1.1E-02 2.0E-02 2.0E-02 2.7E-02
Slovenia 5.4E-03 1.1E-02 1.1E-02 1.9E-02
Spain 1.5E-02 2.7E-02 2.6E-02 3.2E-02
Sweden 5.0E-03 8.8E-03 8.4E-03 1.0E-02
Switzerland 0 0 0 0
USA 6.4E-03 1.2E-02 1.2E-02 1.6E-02
Vietnam 1.7E-01 3.7E-01 3.9E-01 6.8E-01
226
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231
Curriculum Vitae
Personal information
Name Yaping Cai

Date of Birth 27 September, 1990
Place of Birth Beijing, China
Nationality Chinese
Education
2017 – 2021 ETH Zürich, Zürich, Switzerland,

PhD in Environmental Sciences
2014 – 2017 ETH Zürich, Zürich, Switzerland

Msc in Environmental Sciences
Major in Biogeochemistry and Pollutant Dynamics
2009 – 2013 Nanjing University, Nanjing, China

Bsc in Environmental Sciences
Major in Environmental Biology
2006 – 2009 High School Affiliated to Renmin University of China, Beijing, China
High School Diploma
Research Experience
08/2017 – 03/2021 PhD Student, Environmental Risk Assessment and Management

Group, Swiss Federal Laboratories for Material Science and
Technology, St. Gallen, Switzerland
Project: Microplastics and the Textile Sector: Experimental Studies
concerning the Release from Fabrics and Environmental Risk
Assessment in Laundry Care Products
01/2017 – 07/2017 Intern, Environmental Risk Assessment and Management Group, Swiss
Federal Laboratories for Material Science and Technology, St. Gallen,
Switzerland
Project: Collection of Ecotoxicological Data and Identification of Specific
ENM-Effect Patterns in the Context of Environmental Risk Assessment
of Engineered Nanomaterials
05/2016 – 10/2016 Master Thesis Student, Safety and Environmental Technology Group,
ETH Zürich, Zürich, Switzerland
Project: Exposure Assessment of Bisphenol S and F
232

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Research Collection

Microplastics and the Textile Sector: Experimental Studies

MICROPLASTICS AND THE TEXTILE SECTOR:

A dissertation submitted to attain the degree of

DOCTOR OF SCIENCES OF ETH ZURICH

M.Sc., ETH Zurich

born on 27 September 1990

accepted on the recommendation of

Prof. Dr. Bernd Nowack, examiner

Prof. Dr. Denise M. Mitrano, co-examiner

Prof. Dr. Jing Wang, co-examiner

Daneben stellt die Verwendung von Textilpflegemitteln welche Mikroplastik wie z. B.

1.1. Plastics in the environment

The ubiquitous occurrence of microplastics in the environment emphasizes the need of

Table 1-1. Polymers in the textile sector19.

Type Source of polymers Examples

Natural polymers Cellulosic fiber

Chemical fiber Inorganic polymers Glass fiber

Synthetic polymers Polyester, polyamide, polypropylene

1.3. Occurrence of and source microplastic fibers in the environment

In addition to the occurrence of MPFs in WWTPs, the ubiquitous presence of MPFs in

1.4. Origin of microplastic fibers in textiles

Washing of textiles is commonly recognized as an important pathway of releasing MPFs from

Napper and Polyester, acrylic, Front-load washing

Hernandez, et Interlock, jersey fabric swatch

Dalla Fontana, et Knit fabric (edge sewn with a

1.6. Microplastics in laundry care products

1.7. Environmental risk assessment

Therefore, modeling is a valuable alternative approach to estimate the exposure level of

RCR: risk characterization ratio

PEC: predicted environmental concentration

PNEC: predicted no effect concentration

The research questions of the thesis are:

I. What is the origin of MPFs in textile products?

final version of manuscript.

1. Plastic Europe, https://www.plasticseurope.org/en/about-plastics/what-are-plastics;

8. Can-Güven, E., Microplastics as emerging atmospheric pollutants: a review and

9. ECHA, Opinion on an Annex XV dossier proposing restrictions on intentionally-added

20. Textile Exchange, Preferred Fiber & Materials: Market Report

46. Adanur, S., Handbook of weaving. CRC press: 2001.

69. ECHA, Restriction on intentionally added microplastics (SLOT 1). Socio-Economic

74. ECHA, Guidance on information requirements and Chemical Safety Assessment;

76. Nowack, B., Evaluation of environmental exposure models for engineered

83. ECHA, Restriction on intentionally added microplastics SEAC-Microplastics

2.3.1. Sliver, yarns and textiles

Density Fiber diameter

Sliver - - - - White - 12.0±1.3

- - Rotor* Spun White - 12.5±0.7

- - Air-jet* Spun White - 11.9±0.7

Yarn - - Ring* Spun White - 12.3±0.6

- - Ring* Spun Black - 12.8±1.5

- - - Filament Black - 10.8±0.4

Interlock Spun Black 209±1 12.2±0.8

Jersey Spun Black 226±1 12.8±0.8

Knit Rib Spun Black 294±2 12.7±1.1

Rib Filament Black 199±1 15.9±2.2

Unprocessed Terry Spun Black 208±2 13.0±1.3

Plain Spun Black 100±0 12.7±0.5/13.4±0.9**

Plain Filament Black 149±1 7.5±0.6/7.9±0.5**

Satin Filament Black 75±0 13.0±0.7/16.4±1.7**

Knit Fleece Filament Black 185±1 11.7±1.3

* Spinning methods of spun yarns

2.3.2. Sample preparation