Science of the Total Environment 818 (2022) 151812

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Science of the Total Environment

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Airborne microplastic concentrations and deposition across the Weser

River catchment
Sarmite Kernchen a, Martin G.J. Löder b, Franziska Fischer c, Dieter Fischer c, Sonya R. Moses b, Christoph Georgi d,
⁎ ⁎
Anke C. Nölscher a, Andreas Held d, , Christian Laforsch b,
a
Department of Atmospheric Chemistry, University of Bayreuth, Bayreuth 95440, Germany
b
Department of Animal Ecology I and BayCEER, University of Bayreuth, Bayreuth 95440, Germany
c
Leibniz Institute of Polymer Research Dresden, Dresden 01069, Germany
d
Chair of Environmental Chemistry and Air Research, Technische Universität Berlin, Berlin 10623, Germany

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• Average airborne MP concentration of

91 ± 47 particles per m3 (>4 μm)
• Average total MP deposition rate of 99 ±
85 particles per m2 per day (>11 μm)
• Atmospheric deposition must be consid-
ered as a diffuse MP source.
• Proximity to sources, especially to cities,
increase MP numbers in the atmosphere.
• PP and PE fragments predominate in air in
Central and Northwest Germany.

A R T I C L E I N F O A B S T R A C T

Article history: Microplastic (MP) appears to be omnipresent in the atmosphere, raising concerns about dispersion across environmen-
Received 6 August 2021 tal compartments, ecological consequences and human health risks by inhalation. To date, data on the sources of at-
Received in revised form 1 November 2021 mospheric MP and deposition to river catchment areas are still sparse. We, therefore, took aerosol and total
Accepted 15 November 2021
atmospheric deposition samples in the catchment area of the large German river Weser to estimate microplastic depo-
Available online 20 November 2021
sition fluxes (DFs) at six specific sites and airborne MP concentrations. Sampling in rural, suburban, and urban envi-
Editor: Kevin V. Thomas ronments and wastewater treatment plants (WWTPs) was performed, aiming at a variation in airborne MP pollution
and elucidating potential MP source areas. Aerosol samples were taken twice in April and October while monthly
Keywords: total deposition samples were collected over a period from March to October. Microplastics were detected in all
Plastic pollution analysed aerosol samples by Raman spectroscopy down to 4 μm, and in all 32 total deposition samples by μFT-IR
Airborne microplastics down to 11 μm. Average MP number concentrations of 91 ± 47 m−3 were found in aerosol samples. The measured
Deposition of microplastics total MP number DFs ranged between 10 and 367 N m−2 day−1 (99 ± 85 mean ± SD) corresponding to total

Abbreviations: MP, microplastic; DF, deposition flux; nDF, number deposition flux; mDF, mass deposition flux; μFT-IR, Fourier-transform infrared micro-spectroscopy; FPA, focal plane array;
SERS, surface-enhanced Raman spectroscopy; TERS, tip-enhanced Raman spectroscopy; WWTP, wastewater treatment plant; PE, polyethylene; PP, polypropylene; PET, polyethylene terephthalate;
PVC, polyvinyl chloride; PS, polystyrene; SI, silicone; PA, polyamide; EVAc, ethylene vinylacetate copolymer; PAN, polyacrylonitrile; ABS, acrylonitrile butadiene styrene; PMMA,
polymethylmethacrylate; PC, polycarbonate; PU, polyurethane; PBT, polybutylene terephthalate; POM, polyoxymethylene; PPS, polyphenylene sulfide; PPSU, polyphenysulfone; PSU, polysulfone;
CA, cellulose acetate; EVOH, ethylene vinyl alcohol; PHB, polyhydroxybutyrat.
⁎ Corresponding authors.
E-mail addresses: held@tu-berlin.de (A. Held), Christian.Laforsch@uni-bayreuth.de (C. Laforsch).

http://dx.doi.org/10.1016/j.scitotenv.2021.151812
0048-9697/© 2021 Elsevier B.V. All rights reserved.
S. Kernchen et al. Science of the Total Environment 818 (2022) 151812

Weser River catchment deposition of 0.05 ± 0.1 kg ha−1 per year and to an estimated 232 metric tons of plastic being deposited in the Weser
μFT-IR spectroscopy River catchment annually. MP number DFs were higher in urban than rural sites. An effect of WWTPs on the MP abun-
Raman spectroscopy dance in air was not observed. Polypropylene, polyethylene, polyethylene terephthalate, polyvinyl chloride, polysty-
rene, and silicone fragments were found as the predominant polymer types in total deposition samples, while
polyethylene particles dominated in aerosol samples. The results suggest that proximity to sources, especially to cities,
increase the numbers of MP found in the atmosphere. It further indicates that atmospheric MP considerably contrib-
utes to the contamination of both aquatic and terrestrial habitats.

1. Introduction
Global plastic production increases and is expected to double within
the next 20 years (Lebreton and Andrady, 2019). As a consequence,
mismanaged plastic waste is expected to reach 155–265 million metric
tonnes annually by the year 2060 (Lebreton and Andrady, 2019). In
the environment, plastic litter is prone to fragmentation due to the influ-
ence of mechanical forces, light, temperature, pH and other factors in
tandem with slow degradation processes (Cai et al., 2018; Kale et al.,
2015). This results in a growing number of plastic particles in macro
(>5 mm), micro (5 mm to 1 μm), and nano (<1 μm) sizes (Galgani
et al., 2021; Song et al., 2017; Song et al., 2020). Environmental pollu-
tion with microplastics (MP) raises concerns in terms of the viability
of ecosystems (Reimonn et al., 2019) and public health (Prata, 2018).
Plastic particles smaller than 5 mm in diameter may be dispersed,
ingested and accumulated (Sharma and Chatterjee, 2017). Moreover,
the production and disposal of plastics are responsible for significant
greenhouse gas emissions (OECD, 2018).
Nowadays, it is nearly impossible to find plastic-free ecosystems
(Akdogan and Guven, 2019; Auta et al., 2017; Eerkes-Medrano
et al., 2019; Möller et al., 2020; Patti et al., 2020; Peeken et al.,
2018; Smith et al., 2018; van Cauwenberghe et al., 2015; Wu et al.,
2018). Despite MP pollution in marine, freshwater and terrestrial en-
vironments including sanctuaries (Bauer et al., 2008; Guerrini et al.,
2019), remote islands (Andrades et al., 2018), and deserts (Abbasi
et al., 2021), atmospheric contamination with plastic particles has
only recently attracted research activity (Enyoh et al., 2019; Zhang
et al., 2020). MP has been studied in urban, rural and pristine envi-
ronments and was found in bulk atmospheric deposition (Allen
et al., 2019; Cai et al., 2017; Dris et al., 2016; Klein and Fischer,
2019; Stanton et al., 2019; Wright et al., 2020), sampled air (Abbasi
et al., 2019; Dris et al., 2017; Gaston et al., 2020; Kaya et al., 2018;
K. Liu et al., 2019; Syafei et al., 2019), snow (Bergmann et al.,
2019; Scopetani et al., 2019), and settled dust (Abbasi et al., 2017;
Dehghani et al., 2017; C. Liu et al., 2019). MP global atmospheric
transport and potential source areas were recently modeled by
Brahney et al. (2021) and Evangeliou et al. (2020); however, field
surveys supporting models for the reliable assessment of MP pollution
in the atmosphere on a global scale are still lacking.
Emitted into the atmosphere, MP is subject to short- and long-range
atmospheric transport and deposition providing one of the routes for
MP dispersion. Recent studies suggested that MP particles with irregular
and elongated shapes possess low settling velocities in the range of
0.001 m s−1 (Trainic et al., 2020). This is similar to the majority of air-
borne submicron particles which allows MP particles to travel over long
distances up to thousands of kilometers (Emerson et al., 2020). For fi-
brous and non-fibrous MP particles with settling velocities down to
0.06 m s−1, short-range transport up to 60 km was estimated (Trainic
et al., 2020; Wright et al., 2020). The aerodynamic behaviour of differ-
ently shaped microplastics is still only barely understood. Long-range
atmospheric transport is typically associated with MP particles smaller
than 10 μm (Evangeliou et al., 2020), even though long-range transport
of giant mineral dust particles (>75 μm diameter) has been observed
(e.g. Betzer et al., 1988; van der Does et al., 2018). Thus, airborne
MPs could represent a significant source of background microplastic
pollution around the globe (K. Liu et al., 2019), and along with the
adsorbed pollutants (Dris et al., 2015) they harbour the risk of consider-
able long-term threats to ecosystems (Löder et al., 2015; Löder et al.,
2017).
To date, airborne MP origin and emission mechanisms are not well
studied. MPs in a size that facilitates atmospheric transport may origi-
nate from e. g. industrial emission like dust from plastic production, pro-
cessing and transport, plastic waste incineration (Yang et al., 2020) and
decomposition of construction materials (Prata, 2018). Considerable
MP pollution is expected from urban areas and households (Wright
et al., 2020), i.e., airborne MPs may originate by abrasion from plastics
of daily usage. Automotive tire and road abrasion may contribute up to
93 vol% of traffic-related particulate matter from 10 μm to 80 μm in size
(PM10–80) near roads (Sommer et al., 2018). Due to their aerodynamic
behaviour, fibres are prone to becoming airborne. Therefore, particular
attention should be paid to synthetic clothing and other fabrics as a
dominant airborne fibre source. Synthetic clothes release millimeter
and sub-millimeter-sized fibres in their life cycle, especially during
wearing, laundering, and drying processes (Dris et al., 2015). As syn-
thetic fibres were found in higher amounts in indoor air, microplastic fi-
bres in outdoor air can result from mixing with indoor air (Dris et al.,
2017). Furthermore, MP may be emitted into the atmosphere from surface
waters via bubble burst or jet ejection (Allen et al., 2020), and blown off
from landfills, urban surfaces (Abbasi et al., 2017) and roads (O’Brien
et al., 2021) by wind, thus, contributing to the atmospheric particulate
load. Removal from the atmosphere by wet or dry deposition closes the
so-called atmospheric plastic cycle (Prata, 2018; Wright et al., 2020).
Rivers are considered the major pathways transporting 91% of
mismanaged plastic waste to the ocean (Lebreton and Andrady, 2019).
However, global simulations of atmospheric transport of MP particles pro-
duced by road traffic show high transport efficiencies of these particles to
remote regions. It was suggested that direct deposition of airborne particles
is likely the most important source of road-derived MPs for the oceans
(Evangeliou et al., 2020) and the input of atmospheric MPs through precip-
itation to land and sea could be a key source of microplastics in the coastal
environments (Zhou et al., 2017). The largest contributions to modeled
plastic deposition in the western United States were reported reemissions
from road dust sources (84%), the ocean (11%), and agricultural field
dust (Brahney et al., 2021).
In this study we investigated atmospheric MP pollution and MP deposi-
tion in the catchment of the Weser River, which connects urban, agricul-
tural and rural areas in Central and Northwest Germany with the North
Sea. Methodologically harmonized sampling of atmospheric MPs was con-
ducted in 2018 at six different sites to assess atmospheric MP concentra-
tions and MP deposition fluxes (DFs). Study sites reflecting different land
use areas, i. e. urban, suburban, and rural, which were expected to show
varying degrees of MP pollution in air, were sampled. Additionally, MP de-
position at two waste water treatment plants (WWTPs) was investigated to
assess whether waste water treatment procedures in partially open-to-
atmosphere tanks are associated with elevated airborne MP pollution.
Aerosol snapshot samples were taken twice a year in April and October
while monthly total deposition samples were collected site specifically
over a period from March to October. For all MP particles, the polymer
type, size and shape were identified by Fourier-transform infrared micro-
spectroscopy (μFT-IR) and/or Raman spectroscopy. Potential MPs source
areas and transport to the field sites were elucidated using local wind
field plots and backward air trajectory calculations.

2
S. Kernchen et al.
2. Materials and methods
2.1. Sampling sites
Atmospheric contamination with MP was investigated at six sites
across the Weser River Catchment in Northwest and Central Germany
covering almost 13% of the German land area. All sampling sites were
selected to cover regions which were expected to show varying degrees
of MP pollution in air. Four stations were located next to weather sta-
tions, i.e. in the port city of Bremerhaven, in the agriculturally used
area Weserbergland (Weser uplands) near the city of Rinteln, in the for-
ested Solling landscape, and at the remote mountain site Wasserkuppe.
Two sampling sites were located at the WWTPs Kasselwasser located
downstream of the city of Kassel (study site Kassel), and hanseWasser
Bremen Seehausen located downstream of the city of Bremen (study
site Bremen). All sampling sites are displayed in Fig. 1 (detailed descrip-
tion in SM).
2.2. Contamination control
Special care was taken to keep all the units and solutions which came
into contact with the samples clean from plastic particles. All reagents
and rinsing solutions were filtered through a 0.2 μm (0.45 μm for enzyme
solutions) membrane filter (47 mm, cellulose acetate, Whatman, Japan) be-
fore use. All glassware, sampling funnels, tweezers, stainless steel filters,
Fig. 1. Study area and geographical distribution of sampling locations across the Weser River Catchment (Map: Oliver Archner (UBT, Bayceer), the map data were retrieved
from the UBA Viewer database, with an access to the ArcGIS Feature Server, Eurographics, EuroGlobalMap (EGM, 2017) and BKG DLM 1000, 2018).
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Science of the Total Environment 818 (2022) 151812
sieves, thermometers, Petri dishes, and all components of the vacuum filtra-
tion devices were thoroughly rinsed with pre-filtered MilliQ water,
followed by rinsing with pre-filtered 35% EtOH, and afterwards repeatedly
washed with pre-filtered MilliQ water. All pre-cleaned units were stored
covered with non-plastic lids or wrapped in aluminium foil to minimize
contamination from lab air. Stainless steel filters were placed in the ultra-
sound bath and sonicated for 15 min before the above mentioned standard-
ized rinsing process to ensure desorption of particles from the surface.
Reagents and solutions were stored either in glass bottles, or in stainless
steel or Teflon spray bottles. The use of plastic tools, containers and other
lab equipment was avoided. The lab, where most of the work was done,
is equipped exclusively for MP analyses and no external tasks are allowed.
Cotton lab coats were always worn during the procedures to prevent any
contamination of synthetic fibres from clothing. 9 out of 28 total deposition
procedural blanks were free from MP. The rest of the blank samples
contained variable amounts of MP which did not exceed on average 20%
of the MP count in field samples. Blank values were consequently
subtracted from the field samples. In aerosol field blanks, MP particles
were not detected.
2.3. Sampling, sample processing and analytical methods
MP contamination of the atmosphere was examined in two complemen-
tary atmospheric samples: (1) aerosol samples and (2) total atmospheric de-
position samples.
S. Kernchen et al.
Aerosol samples were collected using two well-established sampling
methods: active pump sampling on a filter and size-selective sampling of
airborne particulates using a cascade impactor (see also SM, Fig. S1a–c).
Sampling with cascade impactor was performed due to the fact that only
particles with specific aerodynamic diameter are collected on different im-
paction surfaces, thus facilitating confocal Raman analysis, and because of
the sampling specificity to arrange particles on a tiny strip rather than dis-
persing them over the entire exposed filter area, thus significantly increas-
ing the speed of the scanning analytical methods (see SM Fig. S1g). Total
atmospheric deposition (dry and wet) was collected using already de-
scribed and established methods (adapted from Dris et al., 2016 and
Klein and Fischer, 2019) and was funneled through a stainless-steel funnel
in glass bottles (SM, Fig. S1d, e). MPs were determined in the two sample
types by two different analytical methods: aerosol samples were analysed
by Raman due to lower analysable particle sizes, which allowed us to deter-
mine the number of potentially respirable MP particles (<10 μm); and total
deposition samples were analysed using the freely accessible μFT-IR instru-
ment to enable many samples to be measured. Both of these vibrational
spectroscopic methods are the most popular ones applied in MP studies,
and it has been suggested to use them in tandem for complete and reliable
chemical characterization of MPs (Käppler et al., 2016). In our work the in-
strumental limitations were down to 4 μm by using Raman and 11 μm using
μFT-IR, which were determined by the diffraction limit and applied settings
(see below). It is worth mentioning that μFT-IR instruments equipped with
focal plane array (FPA) (126 × 126) detectors capable for acquiring of 2D
FT-IR imaging can achieve lateral resolution of below 10 μm (Cincinelli
et al., 2021; Morais et al., 2020), and by using Raman imaging the smallest
MP particles measured in a real sample were down to 100 nm in size
(Sobhani et al., 2020). Advanced techniques such as surface-enhanced
Raman spectroscopy (SERS) were applied for detection of MP <1 μm in
size (Xu et al., 2020), and tip-enhanced Raman spectroscopy (TERS) has
been used to analyse atmospherically relevant nanoparticles in a size
range of 10–20 nm (Ofner et al., 2016). Future studies using these technol-
ogies could provide more reliable airborne particle counts and deposition
rates.
Aerosol samples were used to calculate MP concentrations in air (N m−3
and ng m−3), while total deposition sample analysis allowed us to estimate
number deposition fluxes (nDF) and mass deposition fluxes (mDF)
expressed in N m−2 day−1 and kg ha−1 a−1, respectively. Impactor frac-
tions were assessed only qualitatively (see discussion in Section 4.1). Differ-
ent sampling methodology and analysis of both types of samples did not
enable comparison between each other.
2.3.1. Aerosol sampling
Active sampling of airborne particulates was conducted once in April
and once in October 2018, at all study sites (SM, Table S1). Aerosol samples
were collected on aluminium oxide filter (pore size 0.2 μm, ⌀ = 25 mm,
Anodisc25, Whatman, Germany) placed in an open-face stainless steel filter
holder from Sartorius (⌀ = 25 mm, exposed area of 272 mm2). All parts of
the filter holder consist of non-plastic materials except the silicone O-ring
but here we do not expect any abrasion to occur. A custom-built pump
with a nominal volume flow rate of 9 l min−1 powered with a Li-ion battery
pack (Hacker Top Fuel ECO X-20C Lipo Akku 4S/14,8 V 5800 mAh) was
connected to the filter holder and was left running for 3 h. The flow was
constant throughout the sampling period, and the actual flow of
3.4 l min−1 enabled a throughput of 0.6 m3 air volume. The actual flow
was measured using Sensidyne Gilian Gilibrator 2 Primary Flow Calibrator
801804-1. The air filtration device was placed on an aluminium tripod at a
height of 1.6 m above ground level (SM, Fig. S1a). After sampling, the filters
were placed in pre-cleaned stainless steel Petri dishes, covered additionally
with aluminium foil, transported with caution avoiding shaking, and stored
in a walk-in refrigerator at +4 °C until analysis.
At the sites Kassel, Bremen, and Weserbergland, in parallel to filter sam-
pling, size-selective sampling of airborne particles was carried out using a
cascade impactor (Sioutas Personal Cascade Impactor), which was con-
nected to the pump as described above maintaining a constant flow rate
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Science of the Total Environment 818 (2022) 151812
of 9 l min−1 (required for Sioutas impactor). Particles were separated in
five aerodynamic diameter ranges by the principle of inertial impaction,
and two fractions, >2.5 μm and 2.5–1.0 μm collected on Anodisc filters
were used for further analysis. The mean wind velocity during the impactor
sampling was always lower than 2.2 m s−1. The sampling duration of 3 h
was long enough to collect sufficient particles for Raman analysis (around
120,000 particles per filter sample and 60,000 particles per impactor frac-
tion). It is to be noted that not all bulk samples and impactor fractions
were analysed due to the long analytical performance by Raman spectros-
copy (analysed filters and impactor fractions are summarized in Table 1
and in SM Tables S1, 2).
2.3.2. Total atmospheric deposition
Total atmospheric deposition samples were collected at the sites
Wasserkuppe, Kassel, Bremen and Bremerhaven monthly over a period
from March 2018 to September/October 2018 and twice in spring and au-
tumn (2018) at the sites Weserbergland and Solling (SM, Table S3). Six
custom-made open-face aluminium/stainless steel collectors were con-
structed and installed at the sampling sites. The collectors consist of an alu-
minium frame (300 mm × 300 mm × 1000 mm), a stainless steel funnel
(⌀ = 257 mm, Sartorius), an amber glass bottle (2.2 l), stainless steel
anti-bird spikes and stainless steel anchoring wires (SM, Fig. S1d, e). Collec-
tors were open to the atmosphere for the entire monthly sampling period.
The 240 mm funnel depth helps to prevent deposited particles from being
resuspended but the contribution of dry deposition may be underestimated
with our sampler. At the sites Wasserkuppe, Kassel, Bremen and Bremerha-
ven, on-site staff changed the pre-cleaned bottles at pre-determined times
or whenever the bottles were nearly full. Therefore, some variability in
sample collection and duration was inevitable. After collection, the bottles
were covered with glass lids, wrapped with aluminium foil, brought to the
laboratory, and stored sealed in a walk-in refrigerator at +4 °C until work-
up procedures. The average collection time for monthly samples was
26 days. Meteorological data during the sampling period were obtained
from the nearest weather stations or WWTPs (SM, Table S3). In total, 32
monthly total deposition samples were collected.
2.3.3. Sample pretreatment and purification
Filter and impactor samples of airborne particles were analysed directly
on Anodisc filters by Raman spectroscopy, and no additional sample pro-
cessing was necessary.
All 32 total deposition field samples and 28 procedural blanks under-
went pretreatment procedures to remove organic and inorganic impurities
prior to analysis (see SM, Schemes 1, 2). The treatment procedures were
chosen selectively depending on the degree of contamination of the sample.
Some samples were strongly contaminated with plant debris, tissues, pol-
len, algae, insects, and inorganic material, which had to be removed before
analyses. The purification methods used were based on gentle “plastic-
friendly” sample processing, avoiding strong acid or alkaline treatments
that risk degrading sensitive synthetic polymers. Purification methods in-
cluded oxidation with Fenton's reagent (FeSO4 + H2O2), enzymatic diges-
tion, and density separation with ZnCl2. All samples followed fractionated
filtration and oxidation with Fenton's reagent. Shortly, the samples were
fractionally filtered through 500 μm and 5 μm stainless steel filters (1–5 fil-
ters per sample were used, depending on the sample contamination de-
gree). The fraction >500 μm was rinsed several times with pre-filtered
MilliQ water to wash out smaller particles and collect them on the subjacent
5 μm filter. Insects and larger distinct plant material were separated out
with tweezers and washed several times with pre-filtered water, before dis-
posal. The remaining fraction was visually examined under a microscope,
and putative plastic particles in size from 700 to around 6000 μm were
sorted out, photographed and placed in Eppendorf tubes (morphological
criteria for sorting were adapted from Hidalgo-Ruz et al., 2012). The iso-
lated particles were analysed using attenuated total reflectance (ATR) FT-
IR (Tensor 27 FTIR spectrometer equipped with a Platinum-ATR-unit,
Bruker Optics GmbH). The 5 μm filters with the collected solids were placed
into separate 500 ml precleaned glass beakers equipped with a Teflon
S. Kernchen et al.
Table 1
Description of the samples analysed in this study, analytical methods, and quantification measures.
Sample Sampling methods Number of analysed samples
Aerosol Active pump sampling on filter 3 Raman, >4 μm
Active pump sampling with impactor 9 Raman, >4 μm
Total deposition Passive sampling 32
n. d. – not determined; nDF – number deposition flux; mDF – mass deposition flux.
magnetic stirrer and thermometer, and covered with aluminium foil.
Fenton's reagent consisting of 20 ml of 0.5 M FeSO4 and 20 ml of 33 vol%
H2O2 was added, and the beaker was placed on a heating plate. As soon
as the mixture reached 40 °C, the reaction began. This temperature was
kept for 2 h periodically replacing the beaker in between the heater plate
and a cooling bath filled with ice. In some cases, when the reaction was in-
complete, a further 20 ml of 33 vol% H2O2 solution was added, and the re-
action continued for another hour. A colour change of the mixture from
amber to pale yellow indicated the end of the reaction and the suspension
was filtered through stainless steel filters (pore size 5 μm) and washed care-
fully with pre-filtered water to eliminate remaining Fenton's reagent. The
beaker and other filters were thoroughly rinsed several times with the puri-
fied water, and filtered. The filter with residues was either split by using
split pliers (custommade Uni-Bayreuth for stainless steel filters with ⌀ =
47 mm) into subsamples and filtered through Anodisc filter(s) following
FT-IR analysis or placed in another precleaned beaker for further enzymatic
pretreatment.
Additional enzymatic purification and density separation were con-
ducted with the more contaminated samples where the first oxidation
step did not provide sufficient purification. Sample pretreatment followed
a novel, universal oxidative-enzymatic and density separation protocol for
different environmental samples described by Löder et al. (2017). The pre-
treatment includes a series of enzymatic digestions for purifying MPs which
were shown to reduce up to 98% of the sample matrix in surface water sam-
ples with a recovery rate of 84% (Löder et al., 2017). To increase the effi-
ciency of the purification process, single-enzyme digestions were applied
at their optimum pH and temperature. The selection of enzymes was
made based on their selectivity to the typical organic matter in the environ-
mental samples, e.g., algae, plankton, pollen, plant and insect residues. The
sequence of enzyme addition was chosen according to the lability of the
targeted biological substrates − first proteins (protease digestion applied)
followed by cellulose (cellulase digestion applied) and then chitin
(chitinase digestion applied). The incubations were conducted in covered
beakers for ~10 days in a multitone shaking incubator (Infors AG,
Bottmingen, Switzerland) at 40 rpm at specifically adjusted pH and temper-
ature conditions (see SM, Scheme S2 for more details). Before the three en-
zymatic digestions, samples were incubated with anionic surfactant –
sodium dodecyl sulfate (SDS), which has the ability to macerate animal
and plant residues and increase the contact surface for the following enzy-
matic treatments. After enzymatic digestion, second Fenton oxidation as de-
scribed above followed to degrade the partly dissolved organic material
further. After each step, the samples were vacuum filtered through stainless
steel filters to prevent the interference of residues from the previous step
into the following treatment, which is particularly important for enzymatic
digestion. To avoid particle losses, all equipment that came into contact
with the sample was rinsed thoroughly with pre-filtered Milli-Q water. At
the end, the residual particulate matter underwent a density separation
with prefiltered 1.7 kg l−1 ZnCl2 solution to remove mineral particles
from the sample. ~50 ml of ZnCl2 solution was mixed with the sample in
a separation funnel, and the mixture was gently agitated for 10 min and
was left sedimenting for ~2 d at room temperature. The sediment was
discharged through the removal valve and the remaining sample was fil-
tered onto Anodisc filters. To avoid a particle overload on the filter, the re-
maining sample suspension was filtered onto 2 to 5 filters. The first
filtration and the first oxidation were performed in a fume hood with the
flow switched to minimum, and the beakers were always covered either
with glass lids or Al foil. All other steps were conducted in a laminar flow
5
Science of the Total Environment 818 (2022) 151812
Analytical methods, limitations Quantitative measure
Concentrations in air (N m−3 and ng m−3)
n. d.
μFT-IR, >11 μm nDF (N m−2 day−1) and mDF (kg ha−1 a−1)
box. Blank samples were treated in the same manner as the field samples
to evaluate the contamination from the sample treatment procedure.
2.3.4. μFT-IR analysis
Particle chemical assignment was determined with a focal plane array
(FPA) based micro-Fourier-Transform Infrared (μFT-IR) microscope Hype-
rion 3000 (Bruker Inc., Billerica, USA) coupled with the Tensor 27 spec-
trometer (Bruker Optik GmbH, Ettlingen, Germany). The microscope was
equipped with a 3.5× IR objective and liquid nitrogen cooled FPA detector
operating with 64 × 64 pixels for chemical imaging as described by Löder
et al. (2015) resulting in a pixel size of 11 μm. MP particles (>11 μm)
were analysed in transmission mode on a CaF2 transmission window
(⌀ 13 mm × 2 mm). Samples were scanned in the wavenumber range
from 1250 to 3600 cm−1 with a spectral resolution of 8 cm−1, and co-
addition of 6 scans (found as optimum for MPs, Löder et al., 2015). The en-
tire particle loaded area of the filter (~10 × 10 mm2) was scanned. Thus,
an infrared map consisting of around 1 million individual spectra was ac-
quired. Subsamples corresponding to 2–50% of the samples were analysed.
Particle identification and quantification was done using the software
OPUS 7.5 (Bruker Optik GmbH) and ImageLab in combination with a
non-commercial, custom-made software tool based on random forest deci-
sion classifiers as described by Hufnagl et al. (2019). The commercially
available software tool automatically searches for IR spectra of the 20
most common synthetic polymers: polyethylene (PE), polypropylene (PP),
polyethylene terephthalate (PET), polyvinyl chloride (PVC), polystyrene
(PS), polyamide (PA), ethylene vinyl acetate (EVAc), polyacrylonitrile
(PAN), acrylonitrile butadiene styrene (ABS), polymethylmethacrylate
(PMMA), polycarbonate (PC), polyurethane (PU), polyburtylene tere-
phthalate (PBT), polyoxymethylene, (POM, acetal.), polyphenylene sulfide
(PPS), polyphenysulfone (PPSU), polysulfone (PSU), cellulose acetate (CA),
ethylene vinyl alcohol (EVOH), and silicone (SI). The location, maximum
and minimum dimensions of the identified MP particles, colour as well as
polymer assignment were recorded. All automated classified FT-IR spectra
were double checked by trained experts in the field and if necessary, com-
pared with reference spectra from a database and only well-fitted spectra
were assigned as MPs. A percentage measure to determine acceptance of
particles as MPs was not considered.
2.3.5. Raman analysis
The Raman imaging microscope (WITec alpha 300R) was equipped
with a 532 nm laser with a laser power of 5 mW (to reduce fluorescence)
and a CCD detector. Spectra were acquired with a gratings of 600 l/mm,
which allows acquiring the entire spectral range (150–3600 cm−1) with
one shot. Image acquisition was done in darkfield at a magnification of
20×. The Raman integration time for every measured particle was chosen
to be 0.5 s with 5 accumulations so that several thousand particles could be
measured in a reasonable time. We do not exclude the possibility that other
Raman settings applied may result in different particle abundances. The mi-
croscope was remote-controlled through a component object model (COM)
interface (interprocess communication developed by Microsoft) to the
WITec control software. The particles down to 4 μm were measured and
identified with the software GEPARD (GEPARD-Enabled PARticle
Detection) (Brandt et al., 2020). First, an optical image in darkfield illumi-
nation is obtained. Then, a combination of thresholding and a watershed al-
gorithm is used to identify the particles against the background. Based on a
particle's optical image, its size, shape and colour are determined. Next,
Raman spectra were obtained at each particle position. The Anodisc
S. Kernchen et al.
background appeared gray in the optical image, so two thresholds were em-
ployed to detect both particles brighter than and darker than the back-
ground. To ensure correct particle detection despite the uneven Anodisc
surface, between 5 and 14 sections of a sample were analysed that were
1000 × 1800 μm or 3000 × 1800 μm in size. For impactor samples with
the particles distributed along a line across the filter, 26–63% of the particle
containing filter surface were analysed in total. For filters where the parti-
cles were distributed over the whole filter, 9.3% of the particle-containing
surface were analysed (SM, Table S2). Automated batch spectra correlation
was performed using the TrueMatch software (WITec) and in-house curated
databases with spectra of 40 standard polymers, 40 paints, pigments and
dyes used for colouring plastics and 23 inorganic and organic substances
commonly found in environmental samples (e.g. minerals, cellulose, pro-
teins). Results of the automated spectra identification with a hit quality
index (HQI; calculated in TrueMatch as Pearson correlation coefficient) > 5
were checked by an experienced spectroscopist and accepted or corrected
when necessary. Results with HQI < 5 were discarded.
2.4. Data processing & statistical analysis
Weather conditions such as temperature, humidity and rainfall play a
crucial role in ambient distributions of air pollutants. To investigate more
specifically the relationship between weather and MP DFs, Spearman
rank correlations were calculated between DF and meteorological variables
as well as ozone and particulate matter (PM2.5 and PM10) concentrations.
Bivariate correlation analyses with DF at Solling and Weserbergland with
meteorological variables were not performed due to only two observations
per site. The differences between the means and within each mean of DFs at
Wasserkuppe, Kassel, Bremen and Bremerhaven were tested by one-way
ANOVA with Tukey's post-hoc test with a significance level set at 0.05. In
addition, the difference between MP DFs across urban and rural/suburban
areas was tested by Mann-Whitney U test. The study site was categorized as
urban if the local population density was at least 500 persons per km2,
i.e., Bremerhaven, Bremen and Kassel sites were considered urban, while
Wasserkuppe, Solling, and Weserbergland were classified as rural/subur-
ban locations. Moreover, to assess whether human activity contributes to
the increased MP deposition, the relationship between DFs and population
density was measured. Tests and correlations were performed in the soft-
ware Past (v.4.03).
Microplastic total DFs were calculated as follows:
χγ
DF ¼ (1)
at
where DF – number (nDF, N m−2 day−1) or mass (mDF, kg ha−1 a−1) de-
position flux, respectively; χ – blank subtracted count (N) or mass (kg) of
plastic particles in a field subsample found by μFT-IR; γ – subsample size;
a – exposed surface area of the collecting funnel (0.05187 m2/
5.187 × 10−6 ha); t –duration of sampling (days/year).
The mass of individual particles was calculated by multiplying the den-
sity of the polymer type and the particle volume. The particle volume was
calculated by Eq. (2) assuming that the particle is an elliptical cylinder
(due to prevalence of fragment shape) with a height of 67% of the minor di-
mension of the particle similarly as in work by Simon et al. (2018) for ellip-
soid shape:
V ¼ 0:25πd 1 d2 h (2)
where V – particle volume, d1, d2 and h – major and minor dimensions, and
height of the particle, respectively.
The atmospheric residence times τres and transport distances l of de-
tected MP particles were approximated based on simplified calculations
from deposition velocities Vd, atmospheric mixing heights H, and wind
speed U (Eqs. (3) and (4)). The atmospheric mixing heights were estimated
in HYSPLIT based on the potential temperature profile of the 2.5-degree re-
analysis data, yielding mixing heights of 190 m in Bremerhaven, 293 m in
Bremen, 417 m in Kassel, 402 m in Wasserkuppe, 256 m in Solling and
6
Science of the Total Environment 818 (2022) 151812
291 m in Weserbergland. Average wind speed was assumed to be
10 m s−1 as applied in the work by Trainic et al. (2020) and in-text citation
(Lewis et al., 2004).
H
τres ¼ (3)
Vd
HU
l¼ (4)
Vd
Supermicron particles (>1 μm) are expected to settle by sedimentation
and due to turbulent motion. Therefore, the deposition velocity (Vd) can
be approximated by Eq. (5) (Aluko and Noll, 2006):
V d ¼ vs þ vt (5)
where vs – particle sedimentation velocity (m s−1); vt –turbulent dry depo-
sition velocity (m s−1). Depending on the particle equivalent spherical di-
ameter (dESD) vt is approximated as 0.01 m s−1 for particles with dESD =
2.5–10 μm, 0.05 m s−1 for particles with dESD = 10–50 μm, and
0.2 m s−1 for particles with dESD larger than 50 μm (TA Luft, 2002).
The sedimentation velocity vs was calculated by Newton's law of resis-
tance, taking into consideration buoyancy effects and particle size and
shape (Eq. (6)):
sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
4 d ESD ρp − ρ
vs ¼ g (6)
3 CD ρ
where CD – dimensionless drag coefficient (calculated acc. Dioguardi et al.,
2017; Saxby et al., 2018 for non-spherical volcanic ash particles); g – grav-
itational acceleration (9.81 m s−2); ρ – air density (1.225 kg m−3 at 1 atm
and 15 °C); and ρp – particle density (kg m−3).
Air mass back trajectories for the study sites and sampling periods were
calculated using the air parcel trajectory model HYSPLIT4 (Stein et al.,
2015) and NCEP/NCAR reanalysis data (Kalnay et al., 1996). The model
was run to calculate a trajectory every 3 h in the backward mode for the du-
ration of 24 h resulting in hourly latitude and longitude data. The trajectory
end-point was set at the sampling sites at an altitude of 300 m above ground
level. In order to visualize air mass origins related to MP deposition fluxes,
back trajectories were weighted by MP nDFs using an approach similar to
Seibert et al. (1994). For each cell in a 1° × 1° grid, the number of trajectory
points was multiplied with the corresponding nDF and divided by the total
number of trajectories.
3. Results
3.1. Microplastic particles in aerosol samples
Three filter samples collected at the sites Bremerhaven, Solling and
Wasserkuppe and nine impactor samples from Weserbergland, Kassel and
Bremen were analysed by Raman spectroscopy for airborne MP particles.
In total, 1 × 104 to 5 × 104 particles per filter and impactor sample were
analysed, and a fraction of 0.02 to 0.12% were of plastic origin. Other air-
borne non-plastic organic compounds of biological origin, pigments, car-
bon, and windborne minerals and were identified, comprising 0.4 to
5.8% of all analysed particles (SM, Table S2).
In total, 107 particles made of polymers were identified in impactor
samples (Fig. 2, see also SM, Fig. S2). 90 particles were identified as syn-
thetic polymers, where PE comprised 78% of all MP particles. 17 particles
contained methylene (CH2) chains, but polymer-type identification by
Raman spectroscopy was not possible. MP particles identified in impactor
samples were in the size range from 4.1 μm to 33 μm, and 67% were smaller
than 10 μm. 79% of particles had an irregular shape, 21% were spherical.
No fibrous particles were detected. With respect to colour, 82% of all parti-
cles were classified as white, followed by blue (5%), transparent (2%),
black (2%), faint blue (2%), brown (1%) and not detectable (7%).
S. Kernchen et al. Science of the Total Environment 818 (2022) 151812

80 average nDFs decreased as follows: Bremerhaven (183 ±

PE
70 124 N m−2 day−1, mean ± SD of a set of 7 measurements) > Bremen
PMMA
(114 ± 81 N m−2 day−1, n = 7) > Kassel (73 ± 21 N m−2 day−1, n =
60 PS 7) > Wasserkuppe (59 ± 30 N m−2 day−1, n = 7) > Solling (48 ±
15 N m−2 day−1, n = 2) > Weserbergland (29 ± 26 N m−2 day−1, n =
Particle count

EVAc
50 2). Statistically significant regional differences of nDF were observed be-
PP
40 tween the sites Wasserkuppe and Bremerhaven (ANOVA, p = 0.026,
PVC Tukey's post-hoc test). MP nDF observed in the WWTPs Kassel and Bremen
30 PET did not stand out and ranged between nDFs at the rural mountain area
Wasserkuppe and the city of Bremerhaven. No clear seasonal characteristics
20 PHB were observed for MP DFs at the study sites over the sampling period from
10 Natural rubber March to October 2018 (SM, Fig. S4). Mann-Whitney U test showed that
CH2 matrix nDF at urban locations differ significantly from rural/suburban locations
0 (U = 56, p = 0.019) (Fig. 3b), although no significant correlation with
4-10 10-33 the population density was observed (rs = 0.65). mDF across the study
Particle size range, μm sites varied between 6⨯10−5 and 0.5 kg ha−1 annually, and the values be-
tween urban and rural/suburban sites do not differ significantly (Mann-
Fig. 2. Polymer type distribution in two particle size ranges for all analysed Whitney U test, U = 453, p = 0.91).
impactor fractions sampled at Weserbergland, Kassel and Bremen.
3.2.2. MP particle size
Polydisperse microplastic fragments in the size range from 11 μm to
In the aerosol filter samples, all identified MP particles ranged from 522 μm (major dimension) and fibres in the length range from 499 μm to
4.4 μm to 29 μm. 67% of MP particles were irregular in shape, 33% were 1945 μm were detected. Note that all these particles passed a filter with
spherical. No fibrous particles were detected. Of the 16 polymer particles 500 μm pore size and were found in the <500 μm sample fraction. 64%
identified in filter samples, 13 were made of PE, one of EVAc, and two of all particles were in the range from 11 μm to 50 μm and 90% from
contained only detectable CH2 matrix. Fifteen of the particles were white, 11 μm to 100 μm. The number of particles decreases significantly with
and one was red. the increase in particle length, similarly as found by other studies (Allen
MP concentrations in the air are presented in Table 2. The highest total et al., 2019; Bergmann et al., 2019) (Fig. 4).
MP concentration was observed at the Bremerhaven site, while the concen-
trations of MPs smaller than 10 μm were similar at the Bremerhaven and 3.2.3. Polymer type distribution
Solling sites. The highest airborne MP mass concentration of 267 ng m−3 In total, particles made of 17 different plastic types were identified. The
was calculated for the Solling site which can be attributed to one single, rel- highest diversity of plastic-types was found at the site Bremerhaven (16 dif-
atively large PE particle (29 μm × 28 μm) and is therefore very likely to be ferent polymer types), followed by Bremen (13), Kassel (9), Solling (8),
an overestimation due to extrapolation. Impactor samples were not quanti- Wasserkuppe (7), and Weserbergland (5) (Fig. 5) (see also SM Fig. S5a–f).
tatively extrapolated to air concentrations due to only partial analysis of The predominant polymer types (exceeding ≥5% of total amount) were
non-uniform impaction patterns. PP, PE, PET, PVC, PS, and SI accounting for 90% of all MP particles (high-
lighted in Fig. 5). Fibres made of PET, PAN, and PA were identified.
3.2. Total atmospheric deposition of microplastics
3.2.4. Correlation with meteorological variables
MP particles were found in all 32 bulk deposition sample fractions Total nDF at four sites (Wasserkuppe, Kassel, Bremen, and Bremerha-
<500 μm but no particles made of plastic materials were found in fractions ven) were correlated with the following meteorological and air quality var-
>500 μm. In total, 3068 particles were identified as potential plastics by iables: precipitation, count of rainy hours, wind speed, wind direction,
μFT-IR random forest decision analysis, of which 483 particles as small as temperature, relative humidity, air pressure, global radiation, PM2.5,
11 μm were verified as MP after manual quality control by two experienced PM10, and atmospheric ozone concentrations (O3). In most cases, the abso-
researchers (SM, Fig. S3). MP fragments in different forms (96.9%) com- lute values of the Spearman rank correlation coefficients rs were less than
prised most of the detected particles, followed by fibres (2.9%) and spheres 0.7 (SM, Table S3). A significant positive correlation was observed between
(0.2%). Gray (58%), transparent (20%) and white (15%) particles predom- nDFs and precipitation at the site Bremerhaven (rs = 0.79, p < 0.05). Signif-
inated, but since the hydroxyl radical-mediated oxidation step with icant positive correlations (rs > 0.85) were observed at sites Bremen, Bre-
Fenton's reagent may bleach the dye from certain synthetic microfibres merhaven and Kassel between DFs and the count of rainy hours.
(Peller et al., 2019), the colour of MP in total deposition samples is not fur- However, at the Kassel site, the correlation between DFs and the count of
ther discussed here. rainy hours was negative (rs = −0.86, p < 0.05). A strong negative corre-
lation between DFs and temperature (rs = −0.89, p ≤ 0.01) and a strong
3.2.1. Deposition fluxes positive correlation with relative humidity (rs = 0.87, p ≤ 0.05) were ob-
The calculated total atmospheric DF of MPs (according to Eq. (1)) are served at the site Bremen. At the Wasserkuppe site, significant correlations
shown in Fig. 3. The nDF ranged from 10 to 367 particles per m2 per day between DFs and meteorological or air quality parameters were not found.
(99 ± 85 N m−2 day−1, mean ± SD) (Fig. 3a) (see also SM, Table S3). nDFs of MPs were investigated with respect to the local wind speed and
The highest average nDF was found in the city of Bremerhaven. The wind direction within a 10 km radius at each study site and each sampling
collection period in order to find out whether local wind conditions play a
role in MP pollution. Overall, 7 wind speed intervals, 16 wind directions,
Table 2 and 7 (or 2) different nDF profiles per study site were used giving a total
<10 μm and total MP particle number concentrations, and total mass concentrations
of 38 individual entries in pollution rose plots shown in Fig. 6 (wind
in aerosol samples at three study sites sampled in October 2018.
speed plots are given in SM Figs. S7–S12).
Study site <10 μm, N m−3 Total, N m−3 Total mass, ng m−3 At the site Bremerhaven, the highest MP nDF was recorded when SW
Bremerhaven 60 121 108 winds from across the port prevailed. At the site Bremen, the average
Wasserkuppe 19 37 58 wind during the sample collection with the highest MP loads was blowing
Solling 58 115 267
from SE, where the city center of Bremen is situated. The highest DFs at

7
S. Kernchen et al. Science of the Total Environment 818 (2022) 151812

400 2000 400 0.5

Urban area Number DF
350 WWTP 350 Mass DF
Rural area Mean DF 0.4
300 Suburban area 1500 300

Residents per km2

nDF [N m-2 day-1]

nDF [N m-2 day-1]

mDF [kg ha-1 a-1]

Mean
250 Population density 250 0.3
200 1000 200
150 150 0.2

100 500 100

0.1
50 50
0 0 0 0

Urban

Urban
Rural / suburban

Rural / suburban
Wasserkuppe

Bremen
Weserbergland

Solling

Kassel

Bremerhaven
a) b)

Fig. 3. Total atmospheric DF of: a) MP number (nDF) at the six study sites; b) average MP number (nDF) and mass (mDF) at rural/suburban (Weserbergland, Solling,
Wasserkuppe) and urban locations (Kassel, Bremen, Bremerhaven). Boxes represent the 25th and 75th percentiles, the black lines within the boxes the median values, the
vertical lines the maximum and minimum values of the DF, and the yellow and red squares the mean values and population density (residents per km2 in 2019), respectively;

Kassel site were observed when SSW winds prevailed during the sampling.
The highest MP DF at the site Wasserkuppe was observed when W winds
dominated during the sample collection. The second highest MP amount
was collected during the predominance of E winds.
At the Solling site, W winds were observed during the collection of the
most MP-loaded samples, and E winds at the Weserbergland site.
Since local wind fields may be affected by local obstacles, they may dif-
fer from the regional winds and may be misleading for source assessment.
Thus, the potential long-range MP transport to the study sites was investi-
gated by means of back trajectory analysis.
Air mass origins during sampling periods are expressed as a superposi-
tion of trajectories weighted by MP nDFs (Fig. 7a–f). Fig. 7a clearly shows
that in Bremerhaven, significantly higher MP nDFs were observed when
air masses passed over the land and not the sea. At the sites Bremen, Kassel,
Wasserkuppe and Weserbergland some similarities with the pollution rose
plots (Fig. 6) can be seen. At the site Bremen, the more polluted air masses
arrived from the south and passed over the land as well (Fig. 7b). At the Kas-
sel site (Fig. 7c), high MP nDFs are associated with air masses arriving from
the West, and at the site Wasserkuppe, air masses arriving both from East
and West show similar MP nDFs.
25
20
Relative abundance [%]
3.3. Particle residence time and transport distance
The calculated atmospheric residence times for particles smaller than
11 μm were up to τres = 10 h with transport distances up to l = 400 km.
For particles in the size range from 11 μm to 30 μm, the calculated average
τres and l were 1.5 h and ∼60 km, respectively. Particles in the size range
from 30 μm to 60 μm were estimated to reside in the atmosphere for 1 h
and were transported for ~40 km. For particles larger than 60 μm, less
than 20 min residence time and less than 20 km transport distance were
estimated.
75% of all particles found in aerosol samples (impactor and filter) were
estimated to travel for long distances over 100 km, and 25% were estimated
to be transported within a 100 km range. Transport distance estimates for
the particles found in total deposition samples by μFT-IR were limited to
80 km due to the size related detection limit of 11 μm
In total deposition samples particles with the largest average transport
distance ~60 km prevailed at the sites Bremerhaven and Wasserkuppe,
whereas larger particles with the smallest transport distance estimates
prevailed at Bremen and Weserbergland sites. Most of PP and PET particles
had larger transport distances ~60 km, whereas most of PS particles were
estimated to be transported for less than 20 km (see also SM Fig. S6).
Fragments 4. Discussion
Fibers

Spheres 4.1. Microplastic particles in aerosol samples

15 The airborne MP number concentrations of 37, 115, and 121 N m−3 at

Solling, Wasserkuppe and Bremerhaven sites (mean ± SD, 91 ±
10 47 N m−3) derived from Raman spectroscopy (Table 2) in our work are
higher than the majority of MP concentrations in ambient air reported by
other studies (MP concentrations from 14 other studies are summarized
5 in SM, Table S5). This is likely due to the sampling sites, and also due to
the 4 μm size limit of detection in our work, while many other studies focus-
0 ing on MP concentrations in air have larger size detection limits (cf. SM
400-500
100-120
120-140
140-160
160-180
180-200
200-300
300-400

500-600
11-20
20-30
30-40
40-50
50-60
60-70
70-80
80-90
90-100

600-1000
1000-2000

Table S5). Trainic et al. (2020) reported MP concentrations of ~0.01–0.1

particles per m3 in the remote marine atmosphere over the North Atlantic
Ocean, while Levermore et al. (2020) reported 2502 particles per m3 near
urban roads in London (UK) (Levermore et al., 2020), which were derived
Major dimension range [μm] from Raman analyses down to >5 and 4.7 μm, respectively. Similar analyt-
ical performances in our work with those mentioned above enable direct
Fig. 4. Size distribution of all identified MP particles in deposition samples. comparison. Thus, our results measured in the rural forested Solling area,

8
S. Kernchen et al. Science of the Total Environment 818 (2022) 151812

Fig. 5. Plastic-type distribution in total deposition samples among the study sites over the sampling period; predominating plastic-types are highlighted.

rural mountainous Wasserkuppe, and highly industrialized city Bremerha-
ven show an average MP pollution between the extreme values reported
in literature so far. In Surabaya (Indonesia), polymer particles were found
in comparable concentrations from 56 to 175 m−3 (Syafei et al., 2019) as
in our work, and (Li et al., 2020) reported 5700 fibres m−3 in Beijing
(China), which is likely the highest value reported so far, although a differ-
ent analytical technique was applied, i.e. μFT-IR and scanning electron mi-
croscope with energy dispersive X-ray spectrometry (SEM-EDX).
In most of the studies on MPs in air samples, plastic fibres dominated
both in rural and urban environments, as well as in indoor and in outdoor
air (SM, Table S5). Contrary, we found no fibres in our aerosol samples al-
though our filter sampling methodology and analytical methods do not ex-
clude fibre detection. The applied particle detection software GEPARD
considers all particle shapes and sizes. Optical images of the whole filters
obtained at 20× magnification and brightfield illumination at the optical
microscope show only very few fibres, revealing that this MP shape was

Fig. 6. a–f. Pollution rose plots of the relationship between nDF of MPs and averaged wind direction at the study sites. The number scale in the figures represents nDF
[N m−2 day−1]. The time series for each sample collection is given in SM Table S3. Wind speed and wind direction data were retrieved from the nearest weather stations
located within 10 m in Bremerhaven, Wasserkuppe, Solling and Weserbergland, and within 1.5 km and 3 km in Bremen and Kassel, respectively. Maps were created
using Datawrapper https://app.datawrapper.de/create/map.

9
S. Kernchen et al.
Fig. 7. a–f. Potential source regions of MP deposition derived from air mass back trajectories weighted by MP nDFs. The colour scale indicates regions with low or high
potential contribution to MP deposition at the study sites (black circles).
very rare in the investigated samples and therefore fibres were not included
in the measured subsample area (9.3% of the sample area). However, there
are also studies that report other dominant MP shape types in air samples:
plastic fragments dominated in indoor and outdoor air in semi-urbanized
areas in California (USA) (Gaston et al., 2020), and films prevailed in
urban and industrial areas in Asaluyeh County (Iran) (Abbasi et al.,
2019). Regarding the chemical identity of airborne plastic types, we
found exclusively PE particles in our samples, but a higher diversity of poly-
mer types was observed in other studies (SM, Table S5). This indicates that
the form and type of MP particles likely to depend on the specific region
and the prevailing pollution source. The airborne MP mass concentration
calculated from Raman spectroscopy results ranged from 58 to
267 ng m−3 (Table 2). Taking the PM10 mass concentration that ranged
from 10 to 18 μg m−3 (SM, Table S1) during sampling as a proxy for the
total aerosol mass concentration, the mass fraction of MP particles in our
samples can be estimated to be roughly 1%.
In cascade impactor sampling, accurate measurements of the particle
size distribution requires that particles remain on the collection surface
after impaction. The size separation depends on the aerodynamic behav-
iour of the particle as a function of particle size, shape, and density
(Hinds, 1999). We analysed first and second stage filters of the cascade im-
pactor samples which correspond to the aerodynamic cut-off diameters of
>2.5 μm (first stage filter), and diameters from 2.5 μm to 1.0 μm (second
stage filter).
Plastic particles larger than 4 μm were identified in both stages. The re-
sults imply that the size separation of particles was imperfect, possibly due
to particle bounce or particle blow off that can happen during impactor
sampling (Esmen and Lee, 1980). Particle bounce depends on many factors
such as the impaction surface characteristics, particle surface properties,
type, size and shape, particle loading on the impaction surface, sampling
conditions, and impaction substrate design (Lai et al., 2008). MP particle
re-entrainment is probably linked to the low density and non-polar nature
10
Science of the Total Environment 818 (2022) 151812
of MP particles, which could rebound from the polar aluminium oxide filter
surface. The blow-off effect could be reduced by using other collection filter
material or by applying suitable coatings.
Filter and impactor samples showed similarities in polymer type and
size distribution: PE particles smaller than 10 μm highly predominated.
We only found plastic particles in the size range from 4 μm to 33 μm in filter
and impactor samples in contrast to other studies where particles also larger
than 50 μm were detected (SM, Table S5). This observation is most likely
linked to the analysed air volume, which was ∼0.6 to 1.6 m3 in our work
(Table S1). Higher air volume throughput would probably enable the iden-
tification of larger particles which is likely not the dominant size.
4.2. Total atmospheric deposition of MP & potential sources
Calculated average MP DFs at the studied sites show that on average
more MP is deposited in urban environments than in rural/suburban loca-
tions (Fig. 3b). This falls into line with the general consideration that cities
are major MP sources (Dris et al., 2018; Wright et al., 2020), and denser
population generates more plastic waste and litter (Dehghani et al.,
2017). MP pollution in cities is related to increased anthropogenic activities
that involve plastics and MPs including synthetic clothing, packaging,
transportation, electronics, buildings, and construction materials (Dris
et al., 2018). Hence, plastic contamination is expected to respond propor-
tionally to the population density as shown by C. Liu et al. (2019). How-
ever, the DFs found in our study did not clearly correlate with the local
population density, indicating that other factors should be considered as
well. The average nDF in the port city of Bremerhaven (population of
180’000 in 2019) was higher than at the site Bremen (population of
567’559 in 2019) and nearly twice as high as at the site Kassel (population
of 202’137 in 2019). The port city of Bremerhaven experiences intense ma-
rine traffic with over 4000 seagoing vessels called annually (Ferreira and
Lattner, 2019). Bremerhaven is also the biggest container port in
S. Kernchen et al.
Germany and Europe's most important site for the handling, industrial pro-
cessing and distribution of European automobiles. Industrial activities
might thus contribute to increased MP pollution at the site. Moreover, pre-
vious work showed that plastic litter from shipping industry contaminates
marine environments (Culin and Bielic, 2016), and it is conceivable that
airborne MPs were emitted locally by ships and dispersed by wind
(Bergmann et al., 2019). Another MP source in Bremerhaven is probably
the plastic disposal and processing industry located within 7 km from the
sampling site. Generally, airborne MPs may originate from accidental re-
lease via plastic processing activities, leakage from pellet storages, or by
abrasion during waste transfer and by waste incineration (Wright et al.,
2020). Thus, highly industrialized areas are expected to experience higher
MP pollution.
MP found in total deposition samples had a calculated average resi-
dence time of 60 min, and the average transport distance was 40 km. This
suggests that particles from local MP sources should dominate in our sam-
ples. In addition, the average dry period between two rainfall events across
the study sites and samples was 2.1 days. With low average wind speeds
(<3 m s−1, except at the site Wasserkuppe) this corroborates the domi-
nance of local MP sources.
The pollution rose plot (Fig. 6a) and local wind fields (SM, Fig. S7g) at
the site Bremerhaven show that during the elevated MP deposition events,
weak SW wind dominated, which is likely the direction from the port and
city of Nordenham. In addition, air mass back trajectories weighted by
MP nDFs clearly show that most polluted air passed over land before
reaching the study site (Fig. 7a). Thus, the highest nDFs found in this
study are associated with continental and not maritime air masses. This is
consistent with the work of Szewc et al. (2021), where higher MP deposi-
tion was observed when the incoming air masses were terrestrial and
lower when they were marine.
The second and third highest MP nDFs were observed at the study sites
Bremen and Kassel. Both sites were located in WWTPs approximately
100 m from open-air water tanks. WWTPs remove up to 95–99% of MP
coming from municipal water systems (Mason et al., 2016). Wastewaters
undergo chemical and biological treatment in partially open-air tanks,
which are exposed to the atmosphere, thus facilitating the potential for
small MP particles to become airborne. However, the average nDF in Kassel
was only slightly higher than the nDF in the rural mountain area
Wasserkuppe, and values at both locations do not differ significantly. Sim-
ilarly, the average nDF at the WWTP in Bremen was lower than in Bremer-
haven but with a low statistically significant difference. Therefore, our
results suggest that WWTPs do not act as strong point sources for airborne
MPs. Both WWTPs are located downstream of the cities of Bremen and Kas-
sel which may contribute to the measured MP contamination at the sites.
Our results suggest that the proximity to the cities plays a larger role than
MP particle release by wastewater treatment procedures.
The pollution rose plot at the study site Bremen clearly shows that high
nDFs were measured with SW winds (Fig. 6b). Additionally, larger particles
>60 μm prevailed, which are estimated to travel less than 20 km (SM,
Fig. S6a) and indicating the dominance of local MP sources.
At the site Kassel situated northeast of the city Kassel, the highest nDFs
were measured when SSW prevailed (Fig. 6c), thus when wind is passing
over the city of Kassel. At this site, particles >30 μm predominated (SM,
Fig. S6a), which are prone to sedimentation close to the source. Therefore,
our data show that MP particles carried from urban areas located in the
inflowing dominant wind direction can be a leading factor determining
the pollution at the sites. Air mass back trajectories at these sites (Fig. 7b
and c) support this finding since high MP nDFs were associated with the
air masses which could have crossed the nearest cities.
The rural site Wasserkuppe is located in a mountain area 930 m above
sea level and experienced stronger winds (average 5.6 m s−1) than other
study sites (average 2.0 m s−1) during the sampling period. The pollution
rose plot (Fig. 6d) and back trajectories weighted by MP nDFs (Fig. 7d)
show the highest DF in relation to W and E winds, which in case of W
wind predominance may have passed over the close city of Fulda located
20 km W of the site. MP particles <30 μm dominated at this site (SM,
11
Science of the Total Environment 818 (2022) 151812
Fig. S6a) comprising 35% of all detected particles, which is the highest pro-
portion of small particles among all study sites. Thus, long-range transport
of MP particles may contribute to the site, since a greater number of ele-
vated wind periods and interspersed calm periods may assist in transport
and deposition of MP fragments (Allen et al., 2019).
At the rural Solling area and the suburban Weserbergland site, the nDF
were the lowest found during the period of our observations. At these sites
only two samples were taken for MP analyses; therefore, the results have to
be discussed with caution. At the Solling site, the pollution rose plot shows
that during the collection of both samples W winds dominated (Fig. 6e),
which did not pass over large cities within 10 km from the sampling site,
thus potentially preventing the site from elevated MP pollution.
Finally, the suburban site in the Weserbergland is located 3 km SE of the
city center of Rinteln and is surrounded by agricultural areas and some in-
dustry. Higher nDF of MP was observed for the spring sample when easterly
winds dominated. Within 1 km to the east and southeast of the study site,
there are several industrial objects including polymer manufacturers,
which could contribute to the total MP pollution at the site. The autumn
sample had the lowest nDF observed among the whole data set. The wind
rose plot shows that the air arrived predominantly from the SW during
the sampling, and no potential MP point sources within 10 km were
identified.
Trees surrounded both the Solling and Weserbergland sites; therefore, a
comb-out effect for MP particles as proposed by Klein and Fischer (2019)
could play a role, but since the nDFs were the lowest at these sites, our re-
sults do not show increased MP deposition.
4.3. Polymer type distribution in total deposition
In total deposition samples, particles made of PP, PE, PET, PVC, PS, and
SI were prevalent, and on average comprised up to 90% of the total ob-
served MP particles. PP, PE, PET, PVC, and PS polymer types were also
most prevalent in the French Pyrenees, where PS and PE predominated,
followed by PP, PVC and PET (Allen et al., 2019). In the metropolitan re-
gion of Hamburg, PE and EVAc particles were most common in total depo-
sition samples (49% and 22%, respectively) (Klein and Fischer, 2019).
Snow samples from Bremen, Bavarian Alps and Heligoland (Germany)
contained predominantly varnish, rubber, PE, PP and PA (Bergmann
et al., 2019), and in snow samples close to Lahti (Finland), the most abun-
dant plastics detected were PE and PP followed by PA (Scopetani et al.,
2019). However, a direct comparison of total deposition and snow samples
is rather difficult, since the ability of snow crystals or rain drops to scavenge
particles differs (Jylhä, 1999).
In our study, PP was the most frequent polymer comprising 39% of the
total count. With 17%, PE was the second most common plastic found in
our samples. PE is the polymer with the highest industrial demand (15
Mt. per year in Europe acc. Plastics Europe, 2020) and is found mostly in
shopping bags, food packaging, synthetic clothing, agricultural films,
pipes, and houseware (Plastics Europe, 2020). PP is the second most used
plastic after PE worldwide (Plastics Europe, 2020). PP is used for the pro-
duction of food packaging, lids, bottles, synthetic fibres, automotive bum-
pers, aircraft units, synthetic clothing, and others. Abrasion resulting in
MPs happens anytime these products meet with abrasive materials. Thus,
when opening plastic packaging, millions of MP particles can be generated
(Sobhani et al., 2020). PP and PE were found as predominant polymer types
in surface waters of the southern North Sea (Lorenz et al., 2019) and the At-
lantic Ocean (Enders et al., 2015). They can be transferred to the atmo-
sphere from seawater via sea spray from waves or bubble bursting (Vauk
and Schrey, 1987). Thus, contamination of terrestrial environments and es-
pecially coastal areas with marine plastic is possible, which is potentially
relevant for the study site Bremerhaven. PET, PVC, PS, and SI were the
next common plastic types identified across the Weser River Catchment.
PET is applied in synthetic fibres production (accounting for 60% of PET
global demand) and production of PET bottles (about 30% of PET global de-
mand). PS is used for food containers, building insulation, and packing ma-
terial. PVC is used mainly in the production of pipes, profiles, resistant
S. Kernchen et al.
textiles, medical devices, and cable insulation (Plastics Europe, 2020). Sili-
cone is used in a wide variety of products, including automotive and trans-
port applications, construction materials especially in the sanitary area,
medical devices, food packaging as well as in textile, leather, fibre industry,
and others (Andriot et al., 2007).
The numbers of PP and PE particles at all study sites decrease in order
Bremerhaven > Bremen > Kassel > Wasserkuppe > Weserbergland
~Solling. However, 44% of all PET particles found during our sampling
campaign were sampled at the Wasserkuppe site (SM, Fig. S5g). PET parti-
cles prevailed in the smallest studied size range from 11 μm to 30 μm (SM,
Fig. S6b). This may point to more remote sources, since smaller particles on
average travel greater distances. The majority of PVC particles prevailed in
the size >30 μm (SM, Fig. S6b), and were found more in urban areas than in
more sparsely populated areas, indicating that local point sources deter-
mined the occurrence of this plastic at the study sites. Most PS particles
were found at the Bremen site accounting for 55% of the total PS count
found across the River Weser basin (SM, Fig. S5g). This observation
might be linked to elevated activities consuming PS and expanded polysty-
rene (EPS) articles, since Bremen is the largest city monitored in this study.
Most airborne silicone MP were found at the Kassel site, and 77% of all SI
were found in urban areas (see SM, Fig. S5g). Thus, it is more likely that air-
borne SI particles are generated locally by human activities.
The surface river water was sampled in April 2018 upstream and down-
stream of the WWTP Kassel discharges close to our bulk atmospheric depo-
sition collector (distance of 560 m and 250 m). Furthermore, the tributary
Lesum in proximity to our study site in Bremen was sampled in May 2018,
and the same sample treatment and analytical methods were used as in this
study (S. R. Moses, unpublished data) facilitating a reliable comparison
with our data. Interestingly, the polymer composition in the river sample
upstream of the WWTP Kassel discharge was nearly identical to our sample
collected in March/April and similar to the total polymer distribution at the
Kassel site (Fig. 5c). Similarities in polymer distribution were observed be-
tween total deposition samples at the site Bremen and the Lesum water
sample as well. PP prevailed in both river water and total atmospheric de-
position samples. Most of the other polymers PET, PVC, PS and PE were
found in similar proportions in both water and atmospheric deposition sam-
ples as well. Thus, atmospheric deposition may contribute to MP pollution
in the river Weser, and it is very likely that MP pollution both in the atmo-
sphere and in the river water are then – at least partially - affected by similar
sources.
4.4. Comparison of atmospheric DFs
Airborne MP has been found in megacities, suburbs, rural locations,
mountain landscapes, and in pristine areas. Total atmospheric deposition
of MPs found by other studies ranged from insignificant levels to 1008 par-
ticles m−2 day−1 (SM, Table S4). But, since no standardized methodologies
are implemented for microplastic sampling, extraction, purification, detec-
tion and quantification, and identification ranged from visual inspection to
reliable chemical assessment of whole sample filters, the existing studies
are difficult to compare.
To our knowledge, there are two published studies in Germany, where
the MP total deposition rates and concentrations in snow were investigated
in urban and in rural locations (Bergmann et al., 2019; Klein and Fischer,
2019). Average DFs of 275 particles m−2 day−1 were found by Klein and
Fischer (2019) in the Hamburg metropolitan area. This study was con-
ducted ~100 km from our Bremerhaven and Bremen sites. The average
nDF at these sites was 149 ± 107 N m2 day−1. Taking into consideration
that the population in Hamburg is nearly threefold compared to Bremen
and Bremerhaven together, and different analytical methods were applied
(FTIR vs Raman), the results are rather comparable. The average total
nDFs at our study sites are also comparable with the MP total deposition
in remote U.S. conservation areas (132 N m−2 day−1) (Brahney et al.,
2020).
Fragments prevailed (98%) in our samples, followed by fibres and
spheres. Similar observations were made in the Hamburg metropolitan
12
Science of the Total Environment 818 (2022) 151812
area where fragments made up 95% of the total particle numbers (Klein
and Fischer, 2019). In the French Pyrenees, fragments were also the major-
ity of identified MP (Allen et al., 2019). Fibres (synthetic and natural) were
found highly predominant in total atmospheric deposition samples from
the European megacities Paris (Dris et al., 2016) and London (Wright
et al., 2020), and from Dongguan (Cai et al., 2017) and Yantai city (Zhou
et al., 2017) in China, as well as from the River Trent catchment (Stanton
et al., 2019). Our samples underwent oxidative treatment with Fenton's re-
agent, which was used to break down and eliminate natural fibres plastic-
friendly (Peller et al., 2019). However, the effect of hydrogen peroxide
alone on natural textile fibres is expected to be limited (Stanton et al.,
2019). Thus, our study does not provide information about the total
number of fibres (natural and synthetic), and our findings are hardly
comparable with studies where other sample processing prior to analyses
was conducted and subsamples of specific shape were analysed (SM,
Table S4).
4.5. Correlation with meteorological variables
Several studies concluded that wet deposition is important for MP
‘washout’ from the atmosphere (Allen et al., 2019; Dris et al., 2016). Studies
by Dris et al. (2016, 2017) revealed that 5 to 10 times more fibres were col-
lected during rain events compared to dry conditions (Dris et al., 2016; Dris
et al., 2017). Work by Dris et al. (2015) and Dris et al. (2016) also suggested
that rainfall seems to be an important factor influencing the ‘fallout’ of MP
although no clear correlation to MP amount was observed. Rain and snow-
fall intensities have shown moderate to strong correlations with the MP
count in the French Pyrenees as well (Allen et al., 2019). In contrast,
some studies did not observe any relationship of MP deposition with rain-
fall (Klein and Fischer, 2019; Wright et al., 2020), and thus this assumption
is discussed controversially (Stanton et al., 2019).
We studied the correlation of MP nDFs with the precipitation and the
count of rainy hours at four sites, and we found significant positive correla-
tions between both parameters at the sites Bremen and Bremerhaven. Thus,
our results confirm the importance of wet deposition in MP scavenging
from the atmosphere and support the suggestion by Dris et al. (2016) and
Allen et al. (2019) that precipitation events may be a positive driver in at-
mospheric MP deposition.
4.6. Ecological and health implications
When aerosol particles of variable sizes are inhaled, a proportion of
them is retained while the remainder are expelled via exhalation. Retained
particles may deposit on respiratory tract mucous membranes and alveolar
surfaces by mechanisms of gravitational sedimentation, inertial impaction,
or Brownian diffusion. Generally, the smaller the particle the deeper it will
penetrate into the respiratory tract and the longer it will be retained
(Heyder, 2004; Martin et al., 2014). Thus, airborne particles of 100 μm
and less can enter the nose and mouth during normal breathing and may ir-
ritate the eyes, nasal mucosa and throat. Particles of 10 μm and less may
pass through the nose, and throat, reaching the lung and may deposit in
the extrathoracic and upper bronchial airways. Particles of less than
2.5 μm may deposit in the lower bronchial airways and alveolar region
and may penetrate the lungs' gas exchange region and translocate into the
circulatory system (Heyder, 2004). Particles of concern to human health
are those smaller than 10 μm, and particles less than 2.5 μm in diameter
pose the greatest adverse respiratory health effects. Recently, MP particles
smaller than 5.5 μm in size, and fibres in range from 8.12 to 16.8 μm
were determined in human lung tissues obtained at autopsies (Amato-
Lourenço et al., 2021). The adverse health effects may be ascribed to
local pro-inflammatory effects, lung disease and increased cancer risk
(Amato-Lourenço et al., 2020; Amato-Lourenço et al., 2021; Prata, 2018).
However, the toxicity of MP will depend on various factors, e.g., particle/
fibre size, burden, density, charge, additives and plastic type in addition
to individual factors and weathering (Amato-Lourenço et al., 2021;
Ramsperger et al., 2020).
S. Kernchen et al.
We measured a mean concentration of 46 N m−3 of airborne MP that
are smaller than 10 μm (mean of 3 measurements, Table 2). Considering
that the average person breathes 11 m3 of air daily, more than 500 MP par-
ticles can potentially be incorporated per day, which may adversely affect
human health. Also, we expect an increasing amount of smaller MP parti-
cles with decreasing size in atmospheric samples and that an analysis of
these smaller particle sizes would verify a much higher potential human in-
corporation rate of MP via breathing air. We also expect higher indoor con-
centrations of MP due to the proximity to the source and lower mixing
rates. MP adverse effects on aquatic and soil organisms (Miller et al.,
2020; de Sá et al., 2018; Wright et al., 2013; Zhang et al., 2021) and soil
properties (de Souza Machado et al., 2020) are already discussed. Our re-
sults suggest that an average MP total nDF of 99 ± 85 N m−2 day−1 and
mDF of 0.05 ± 0.1 kg ha−1 a−1 in rural and urban landscapes should be
considered a critical MP input to these environments. Airborne MP particles
may be dispersed by wind currents, travel over long distances and may de-
posit even at the most pristine places on the Earth far from their sources. At-
mospheric deposition must therefore be considered as an important factor
for background pollution with MPs, however we are just at the beginning
of understanding the atmospheric pathways of MPs, and a deeper under-
standing supported by extensive and reliable data is urgently needed.
5. Conclusions
MP particles were found in all aerosol and total deposition samples in
this study. Atmospheric particle size distributions typically span several or-
ders of magnitude from a few nanometers up to some 100 μm in diameter
(Seinfeld and Pandis, 2016). Therefore, the airborne MP number concentra-
tions and total number deposition fluxes found in this study are certainly
underestimated due to the size limitations of the applied analytical method-
ologies (>4 and >11 μm). Nevertheless, MP concentrations presented in
this work are at the higher end of values of similar studies, and MP nDF
across the Weser River catchment are comparable with DFs reported in
the literature. MP DFs in the Weser River catchment were variable and
did not show clear seasonal characteristics. Moreover, number DFs in
urban environments were larger than in rural landscapes. Plastic abun-
dance and variety were not linked directly to the local population density
but rather to unique conditions at the specific sites combining meteorolog-
ical factors and many potential local sources.
The results of this study do not show a considerable effect of WWTPs on
the local abundance of airborne MPs. Rainfall was found to play a signifi-
cant role in MP scavenging and removal from the atmosphere. Calculated
residence times and transport distances for the particles found in total depo-
sition samples point to local MP sources, which are likely connected to
higher rate of human activities related to cities. Particles found in aerosol
samples were exposed rather to longer-range transport. PP particles were
the most prominent particles in total deposition, whereas PE particles
highly predominated in aerosol samples. Both types of samples were
analysed with two different spectroscopic methods, μFT-IR and Raman,
which provided different limits of detection, respectively. Thus, we assume
that the polymer type distribution varies among the particle size ranges,
and both local and remote particle transport should be considered. How-
ever, neither Raman spectroscopy nor μFT-IR guarantees complete MP par-
ticle identification. Particles not seen with μFT-IR might be detected by
Raman and the other way round, and below a certain size, both can no lon-
ger be applied in MP analysis. This shows that applying different methodol-
ogies may also provide different results. A detailed comparison of methods
is ongoing, and capabilities and limitations of different analytical method-
ologies must always be taken into account when comparing airborne MP
pollution of different studies.
CRediT authorship contribution statement
Sarmite Kernchen: Conceptualization, Methodology, Investigation,
Formal analysis, Writing – original draft, Writing – review & editing. Mar-
tin G.J. Löder: Conceptualization, Methodology, Data curation, Writing –
13
Science of the Total Environment 818 (2022) 151812
review & editing. Franziska Fischer: Methodology, Data curation, Investi-
gation, Writing – review & editing. Dieter Fischer: Methodology, Data
curation, Writing – review & editing. Sonya R. Moses: Investigation,
Data curation, Writing – review & editing. Christoph Georgi: Formal anal-
ysis, Data curation, Writing – review & editing. Anke C. Nölscher:
Resources, Writing – review & editing. Andreas Held: Supervision, Project
administration, Conceptualization, Methodology, Writing – review &
editing. Christian Laforsch: Funding acquisition, Conceptualization.
Declaration of competing interest
The authors declare that they have no known competing financial inter-
ests or personal relationships that could have appeared to influence the
work reported in this paper.
Acknowledgements
The authors would like to thank Agnes Bednorz and Andrej Einhorn
(Atmospheric Chemistry, UBT) for technical support; Ursula Wilczek and
Heghnar Martirosyan (Animal Ecology I, UBT) as well as students Johanna
Schmidtmann and Sanja Blaha for great support in sample processing and
μFT-IR analysis. Many thanks to KasselWasser, hanseWasser Bremen, City
Bremen, HLNUG, and Trade Inspectorate Hildesheim for access to the sam-
pling sites and special thanks to Dr. Franziska Luschtinetz, Claudia Jendrek,
Andrea Schemmel, Wilfried Melchior, and Dr. Andreas Hainsch for the col-
laboration and collection of the samples. Authors are grateful to BMBF and
DFG for the financial support and for the support extension due to Corona
virus crisis.
The project is supported by the Federal Ministry of Education and
Research (BMBF). Project funding ref. nr: 03F0789A, acronym PLAWES.
Part of this work was funded by the Deutsche Forschungsgemeinschaft
(DFG, German Research Foundation) – project nr. 391977956 –
SFB1357.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.scitotenv.2021.151812.
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