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Science of the Total Environment 799 (2021) 149447

Contents lists available at ScienceDirect

Science of the Total Environment

journal homepage: www.elsevier.com/locate/scitotenv

Continental microplastics: Presence, features, and environmental


transport pathways
María B. Alfonso a,b,⁎, Andrés H. Arias a,c, Ana C. Ronda a,d, María C. Piccolo a,e
a
Instituto Argentino de Oceanografía (IADO), Universidad Nacional del Sur (UNS)-CONICET, Florida 8000, Complejo CCT CONICET Bahía Blanca, Edificio E1, B8000BFW Bahía Blanca, Argentina
b
Research Institute for Applied Mechanics, Kyushu University, 6-1 Kasuga-Koen, Kasuga 816-8580, Japan
c
Departamento de Química, Universidad Nacional del Sur, Avenida Alem 1253, B8000DIC Bahía Blanca, Argentina
d
Departamento de Biología, Bioquímica y Farmacia, Universidad Nacional del Sur, Avenida Alem 1253, B8000DIC Bahía Blanca, Buenos Aires, Argentina
e
Departamento de Geografía y Turismo, Universidad Nacional del Sur, 12 de Octubre 1198 4°Piso, B8000CTX Bahía Blanca, Argentina

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

• Continental MPs' presence and path-


ways in air, soils, and freshwater were
addressed.
• Atmospheric fallout, runoff, groundwa-
ter migration, and hydrodynamics are
the main pathways.
• MPs size, shape, polymer composition,
and density interact with environmen-
tal variables.
• Long-term monitoring and interdisci-
plinary research are still needed.

a r t i c l e i n f o a b s t r a c t

Article history: Microplastics (MPs) are ubiquitous contaminants of great concern for the environment. MPs' presence and con-
Received 26 April 2021 centration in the air, soil, marine, and freshwater environments have been reported as a matter of priority in re-
Received in revised form 30 July 2021 cent years. This review addresses the current knowledge of the main pathways of MPs in air, soil, and freshwater
Accepted 30 July 2021
reservoirs in order to provide an integrated understanding of their behaviors in the continental environment.
Available online 2 August 2021
Therefore, MPs' occurrence (as particle counts), sources, and how their features as shape, size, polymer compo-
Editor: Yolanda Picó sition, and density could influence their transport and final sink were discussed. Wind resuspension and atmo-
spheric fallout, groundwater migration, runoff from catchments, and water flow from rivers and effluents were
pointed as the principal pathways. MPs' size, shape, polymer composition, and density interact with environmen-
Keywords: tal variables as soil structure and composition, precipitation, wind, relative humidity, water temperature, and sa-
Microplastics linity. Sampling designs for MPs research should further consider soil characteristics, climate variability and
Plastic pollution extreme events, time lag and grasshopper effects, morphological and hydrological features of aquatic systems,
Pathways and water currents, among others. Furthermore, long-term monitoring and lab experiments are still needed to
Freshwater
understand MPs' behavior in the environment. This information will provide a unified understanding of the con-
Atmosphere
tinental MPs pathways, including the key main findings, knowledge gaps, and future challenges to understand
Soil
this emerging contaminant.
© 2021 Elsevier B.V. All rights reserved.

⁎ Corresponding author at: Instituto Argentino de Oceanografía (IADO), Universidad Nacional del Sur (UNS)-CONICET, Florida 8000, Complejo CCT CONICET Bahía Blanca, Edificio E1,
B8000BFW Bahía Blanca, Argentina.
E-mail address: mbalfonso@iado-conicet.gob.ar (M.B. Alfonso).

https://doi.org/10.1016/j.scitotenv.2021.149447
0048-9697/© 2021 Elsevier B.V. All rights reserved.
M.B. Alfonso, A.H. Arias, A.C. Ronda et al. Science of the Total Environment 799 (2021) 149447

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2. Data collection and analysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3. Continental microplastics pollution: soil, air, and freshwater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.1. Atmosphere . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.2. Soil . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
3.3. Lakes. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.4. Rivers, effluents, and groundwater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.5. Estuaries . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
4. Environmental microplastics' pathways . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
4.1. Atmospheric transport and fallout . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
4.2. Precipitation and runoff . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
4.3. Groundwater migration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
4.4. Freshwater hydrodynamics. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
5. Considerations about MPs features: shape, size, and polymer composition . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
6. Conclusions, knowledge gaps, and future challenges . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
Declaration of competing interest. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12

1. Introduction reducing its primary sources. Unfortunately, there are no estimates of


the MPs' direct input into the oceans (UNEP and GRID-Arendal, 2016)
Nowadays, plastics are considered one of the most relevant pollut- or fluxes among environmental MPs reservoirs (Zhu, 2021). Therefore,
ants worldwide (GESAMP, 2015). Since 1950, the large scale of plastic one of the critical challenges of MPs pollution is understanding their
production, massive consumption, and plastic waste production has multiple transport pathways and quantifying their flux rates to marine
dramatically increased (Rochman, 2018). In 2019, global plastic produc- environments from continental sources (Zhu, 2021).
tion was estimated around 368 million tons and was expected to con- MPs are ubiquitous in a broad type of environments from marine
tinue increasing in the future (Plastics Europe, 2019). Once the plastic (Isobe et al., 2019), freshwater (Besseling et al., 2017; Piehl et al.,
waste is wrongly discarded because of its low degradation rate, most 2019; G. Wong et al., 2020a), terrestrial (van den Berg et al., 2020) to
will remain in the environment, flowing through diverse continental the atmosphere (Enyoh et al., 2019). Their futures as size, shape, tex-
reservoirs to finally end in the marine systems (Zhu, 2021). It was esti- ture, aging status, polymer composition, and density, influence their in-
mated that 1.9 Gt y−1 of municipal solid waste was generated world- teraction with the environmental variables and their final fate. Short
wide (Waste Atlas, 2019), from which between 9% and 11% was and long-range atmospheric MPs transport was registered in diverse
plastic (0.2 Gt) depending on the country's economic income level environment reservoirs as urban centers (Dris et al., 2015), remote
(Kumar and Samadder, 2017). Also, it was estimated that more than mountain catchments (Allen et al., 2019), including Arctic snow
80% of plastic production ends in the oceans (Rochman, 2018). (Bergmann et al., 2019), and the Tibetan glaciers (Zhang et al., 2021).
Jambeck et al. (2015) estimated that between 4 and 12 MT of plastic MPs presence in soils received much less research attention
waste gets into the ocean from coastal regions. Therefore, it is expected (Kutralam-Muniasamy et al., 2020) but were pointed out as one of the
that the plastic impact will not be uniform in a global context, differing main long-term sinks for MPs (Rochman, 2018; Wang et al., 2020).
significantly between developed and developing countries. Moreover, rivers and effluents' water flow were considered a crucial
As a versatile material, plastic is used for various products, from pathway from the continent to the oceans (Rochman, 2018). Lakes
polystyrene (PS), polyethylene (PE), polyethylene terephthalate (PET), and rivers' hydrological characteristics as water flow velocity, depth,
and polypropylene (PP) single-use plastics (SUP) (packaging, trays, bot- bottom topography, and water flow seasonal variation influence plastic
tles), PET and polyamide (PA) synthetic clothes fibers to PE microbeads transport within freshwater reservoirs (Campanale et al., 2020). In addi-
in beauty products (Plastics Europe, 2019). Among them, SUP (36%) and tion, MPs could be ingested by a wide range of organisms (Vroom et al.,
synthetic textile (14%) comprised 50% of the annual global plastic pro- 2017; Arias et al., 2019; Villagran et al., 2020) and incorporated by ad-
duction (Geyer et al., 2017) and were pointed out as the main contribu- sorption in plants (Kalčíková, 2020). So, the role of the biological com-
tors to plastic pollution (Brooks et al., 2018; Zhu, 2021). According to partment on MPs' pathways is significant and complex due to the
Brooks et al. (2018), SUP comprises 6.3 billion MT of plastic waste gen- many processes involved as bioaccumulation and biomagnification
erated worldwide. PE, PP, and PET polymers cover more than 89% of across food webs (Saley et al., 2019; Miller et al., 2020; Krause et al.,
global plastic waste exports, followed by polyvinylchloride (PVC) and 2021).
PS (Brooks et al., 2018). Plastics disposal mismanagement causes their As MPs pollution became a relevant topic, the number of studies in-
spread in the environments where they are brittle and fragmented (by creased significantly in the last few years (Rochman, 2018), and conse-
the effect of heat, UV rays, winds, waves), forming microplastics quently, the number of reviews as well (Li et al., 2020a, 2020b; Du et al.,
(MPs) (Cole et al., 2011), defined as plastic particles less than 5 mm in 2021; Wang et al., 2020). Despite some recent guidelines for methodol-
diameter (Thompson et al., 2004; Frias and Nash, 2019). According to ogies harmonization, there are still discrepancies among studies and fu-
their origin, they can be classified as primary (industrially produced) ture challenges. These include differences in the applied organic matter
or secondary MPs (resulting from plastics weathering and fragmenta- digestion protocols (reagents, concentrations) and the units used to ex-
tion), being the latter the most registered type in the environment press the results, even in the broad nomenclature used to classify them
(GESAMP, 2019). Plastic particles under 0.1 μm are considered or to describe their behavior in the environment. As a result, there is a
nanoplastics and were also reported in the environment, but the infor- high number of incomparable MPs' studies. Furthermore, the informa-
mation is still limited due to the challenges in sampling and detecting tion about the main MPs' source, sinks, and pathways from the conti-
small particles (Peng et al., 2020). Considering that MPs removal from nental reservoirs (air, soil, and freshwater systems) is still limited,
the environment is impossible (Bitter and Lackner, 2020), we should particularly about how MPs' features interact with environmental vari-
be aware that the only way to solve plastic pollution is by tackling and ables in their way through the environment (Zhang et al., 2020;

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M.B. Alfonso, A.H. Arias, A.C. Ronda et al. Science of the Total Environment 799 (2021) 149447

Zhu, 2021). Many reviews and studies comprehensively approach the presented the results in weight (particles kg−1) and area (particle
topic in the different MPs' reservoirs individually, given information m−2 day−1) units for soils and atmosphere studies, respectively.
about particles counts worldwide, but still with limited or fragmented Using analysis tools from Web of Science, “microplastics” searching
knowledge about MPs' behavior in the environment (van Emmerik results were classified by theme in marine and continental studies,
and Schwarz, 2020; Zhou et al., 2020; Li et al., 2020a; Zhang et al., representing 62% and 38%, respectively (Fig. 1). Then, from those in con-
2020; Du et al., 2021; Dusaucy et al., 2021). Therefore, this review's ob- tinental environments (N = 2221) (Fig. 1), 72% corresponded to fresh-
jective was to discuss the current knowledge of the main environmental water environments, 26% to soils, and only 2% to the atmosphere
MPs' pathways on air, soil, and freshwater reservoirs at once to get a (Fig. 1). From the results obtained for continental environments, for
unified vision of their behavior in the continent. In addition, we also dis- each category, between 8% and 26% corresponded to reviews, whereas
cuss MPs' occurrence (as particle counts), sources, and how their fea- between 67% and 89% were articles, and others (books, reports: 2%
tures as shape, size, polymer composition, and density could influence and 16%, respectively) (Supplementary Table 1). Following these pro-
their transport and final sink. This information will provide a unified un- portions, up to 141 items that focused on the scope of the present
derstanding of the continental MPs' pathways, including the key main study were assessed. A semi-systematic review was applied, recom-
findings, knowledge gaps, and future challenges to understand this mended for topics where researchers within diverse disciplines partici-
ubiquitous contaminant. pate and hinder a full systematic review process (Snyder, 2019).
According to Snyder (2019), this approach can map a research field,
2. Data collection and analysis synthesize the state of knowledge, and guide further research. Then,
the obtained information was resumed and discussed in three sections:
For this review, research articles and reviews were searched with in Section 3, the occurrence and characteristics of MPs in soil, atmo-
Web of Science, ScienceDirect, and Google scholar as search engines. sphere, lakes, rivers, effluents, groundwater, and estuaries are presented
The keywords “microplastics”, “plastic pollution”, “plastic polymers”, to introduce the review topic. Section 4 presents and discusses the cur-
“pathways”, “continental”, “freshwater”, “lake”, “river”, “estuary”, rent fragmented knowledge about the main environmental pathways in
“soil”, “terrestrial”, “air”, and “atmospheric fallout” were used for litera- the different MPs' reservoirs to get a more inclusive and comprehensive
ture search. The eligibility criteria were based on the review's scope, understanding of the problem. Finally, in Section 5, we presented how
only considering those (1) up to date (2010–March 2021) and MPs' features as shape, size, polymer composition, and density could
(2) peer-reviewed studies, which discussed (3) microplastic pollution also influence their final fate, concluding with the review's final remarks
in (4) freshwater (5) air, and (6) soil reservoirs. Studies with biological and targeting the main knowledge gaps to address in the future.
assessments or without polymer identification were excluded. We con-
sider those studies comprising MPs between ~10 μm and 5 mm. All the 3. Continental microplastics pollution: soil, air, and freshwater
polymer particles counts were expressed as particles unit−1. For aquatic
environments, only those using volume-related units (e.g., particles Although marine MPs' research remains at the forefront (Fig. 1),
m−3, particles L−1) were considered. Whereas, when possible, we studies on air, freshwater, and soils have begun to occur in this field as

Fig. 1. Analysis of the search results from Web of Science engine: a) percentage of microplastics studies in marine and continental environments, and in lakes, rivers, estuaries, soils, and the
atmosphere. b) Total number of microplastics studies per year. c) Percentage of studies in each type of continental environment per year.

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a matter of priority in recent years. MPs studies start increasing expo- mentioned but should not be considered for particle counting.
nentially, with freshwater environments leading (Fig. 1b, c). In the last Concerning polymer identification, most studies include FTIR or
years, the number of studies in soils increased significantly, but the at- Raman spectroscopy analyses (Table 1), increasing the quality of MPs'
mosphere continues underrepresented (Fig. 1c), so more efforts are results.
still needed in this area. MPs do not end in the ocean without first pass- The increasing number of MPs studies and the lack of global consen-
ing through these continental environments (Fig. 2). Therefore, this sus in sampling, analysis, and results expressions, leads to difficulties in
kind of information is crucial when trying to understand the impact of studies comparisons and bad quality research (Provencher et al., 2020).
plastic pollution and its pathways from the primary sources to one of Therefore, it is essential to clarify that the following sections are not
its final sinks, the oceans (Fig. 2). Up to ten examples of the most recent aimed to exhaustively revise global concentrations at the different envi-
studies about MPs' abundance and characteristics in these environ- ronmental MPs' reservoirs; conversely, it aims to select high-quality and
ments are presented in Table 1, including details about the methodology worldwide representative research papers for a general reference. Then,
applied. Previous MPs studies also pointed out that freshwater environ- we discuss MPs' pollution presence (as particle counts) and their pri-
ment was the most studied category compared to the soil and the atmo- mary sources in the atmosphere, soils, lakes, groundwaters, rivers, efflu-
sphere (Kutralam-Muniasamy et al., 2020; Yang et al., 2021). This could ents, and estuaries from highlighted recent publications to address the
be explained by the similarity between freshwater and marine environ- common MPs' distribution and transport pathways. MPs' shape, size,
ments in MPs samples obtention and processing (GESAMP, 2019; UNEP, and polymer composition in the different reservoirs and their role in
2020), unlike atmospheric and soil samples, where methodologies had the continental MPs pathways are further discussed in Section 5. We de-
to be developed from zero. cided to follow Zhu (2021) proposed terminology to refer to the differ-
From the reviewed literature, it arises that a stricter consensus on ent terms in MPs' pathways. These include “reservoir” (the place where
MPs' methodologies is needed. There are monitoring guidelines for MPs accumulate), “source” (a reservoir where MPs' release > MPs' accu-
freshwater (UNEP, 2020) and marine environments (GESAMP, 2019), mulation), “sink” (the place where MPs' accumulation > MPs' release),
including one to increase research's reproducibility and comparability and “flux” (MPs' amount moving from one location to another per unit
(Cowger et al., 2020). Nevertheless, a great diversity of sampling pro- of time).
cesses, digestion protocols, results expressions, and terminologies
used to describe their behavior in the environment were observed. 3.1. Atmosphere
Also, the details about digestion times, reagents, and temperatures
were limited in some articles (Table 1). Furthermore, according to The number of studies about suspended atmospheric MPs (hereafter
MPs' shape, size range, and polymer type, the expression of results SAMPs) has recently increased (Dris et al., 2016, 2017; Liu et al., 2019;
should be with the best level of detail possible. Many studies compile Bullard et al., 2021), but less than for aquatic systems or soils (Fig. 1).
extensive data but then failed to present the results, hindering valuable Several authors agree that an increase in SAMPs analysis is critically
information. Also, the report of MPs' results out of the methods size needed (Li et al., 2020a; Liss, 2020). The reviewed studies addressed
limits was observed (Table 1). This kind of information could be urban (Dris et al., 2016; Wright et al., 2020) and natural conservational

Fig. 2. Scheme of the continental environmental pathways between the different microplastics reservoirs in the continent.

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M.B. Alfonso, A.H. Arias, A.C. Ronda et al. Science of the Total Environment 799 (2021) 149447

Table 1
Summary of sample treatment details, polymer particles shape, polymer identification and type, methodology lower size limit, size range (μm), and abundance (value, range, or mean
value ± SD) from the atmosphere, soils, groundwater, lakes, rivers, effluents, and estuaries obtained from examples of the reviewed studies (N = 10 for atmosphere, soils, lakes, rivers
and effluents, estuaries and N = 4 for groundwater).

Location Sample treatment Shapes Polymer Polymer type Method Size range (μm) Abundance Reference
identification lower size (particles unit−1)
limit (μm)

Atmosphere
Paris No Fib FTIR Ray, PET, PA 50 50–5000 110 ± 96 Dris et al. (2016)
particles m−2 d−1
Grater Paris -ZnCl2 (1.6 g cm−3) Fib FTIR Ray, PE, PA, PP 1.6 50–3250 (indoor) 1586–11,130 Dris et al. (2017)
50–1650 particles m−2 d−1
(outdoor)
Western Pacific No Fib, Fra, μ-FTIR PET, PE, PES, ALK, EP, 1.6 23.07–9555 0–1.37 particles Liu et al. (2019)
Ocean Pel, Mic PA, PAN, PMA, PP, PS, m−3
PVA, PVC
Pyrenees, France -H2O2 30% (55 °C, 7 d) Fib, Fil, μ-Raman PS, PE, PP, PVC, PET 0.45 <25–2600 365 ± 69 Allen et al.
-ZnCl2 (1.6 g cm−3) Fra particles m−2 d−1 (2019)
French Atlantic -H2O2 30% (55 °C, 7 d) NA μ-Raman HDPE, LDPE, PET, PP, 10 20 ± 13 (pumped 2.9–9.6 particles Allen et al.
coast -ZnCl2 (1.6 g cm−3) PS, PVC air) m−3 (2020)
24 ± 14 (cloud
catcher)
Dongguan, China -Dried 50 °C, 48 h Fib, Fo, μ-FTIR RY, PE, PP, PS 1 <200–4200 175–313 particles Cai et al. (2017)
Fil, Fra m−2 d−1
Central London -Dried 40 °C, 4 h Fib, Fra, FTIR PAN, PET, PA, PU, PP, 20 905 ± 641 (Fib) 712 ± 162 (Fib) Wright et al.
-Ultrasonication (10% Fil, Pel, Ray, PVC, PES, PS, Acr, and 164 ± 167 and (2020)
methanol, 1 min) Fo (non-fibrous) 59 ± 32
-Nile red (non-fibrous)
particles m−2 d−1
Hamburg, Germany -NaClO 0.15:1 Fra, Fib μ-Raman PE, EVA 13 <63–5000 275 particles m−2 Klein and Fischer
-Nile red d−1 (2019)
Shanghai No Fib, Fra, μ-FTIR PET, PE, PES, PAN, PA, 1.6 23.07–9555 0–4.18 particles Liu et al. (2019)
Pel Ray, EVA, m−3
National Parks, EE. -Freeze-dried Fra, Fib FTIR PES, Ny, PE, PP, PVA, 20 4–188 (Fib) 48 ± 7 to 435 ± 9 Brahney et al.
UU. PTFE 20–3000 (Fra) particles m−2 d−1 (2020)

Soils
Croplands and -NaCl (1.20 g cm−3) Fib, Fil, FTIR PU, PE, EVA, PP, PS, 0.4 300–5000 540 ± 320 Corradini et al.
pastures, Chile -ZnCl2 (1.55 g cm−3) Fra, Pel CPE, PA particles kg−1 (2021)
(cropland)
420 ± 240
particles kg−1
(pasture)
Road dust in Japan, -H2O2 30% (25 °C, 7 d) Fib, Fra, FTIR PE, PP, PS, PET, PAK, 100 100–5000 2–39.6 particles Yukioka et al.
Vietnam, and -Dried 50 °C Fil, Pel PVS, EPC, SBR, EPDM, m−2 (2020)
Nepa -NaI (1.6 g cm−3) PU
Yangtze River, -30% KOH:NaClO (50 °C, Fra, Pel, Raman PA, PS, PVC, PE, PP, 0.45 10–˃1000 3877 ± 2356 Zhou et al.
China 48 h) Fib, Fo, PAN, PC particles kg−1 (2021)
-NaCl (1.2 g cm−3) Fil
-ZnCl2 (1.55 g cm−3)
Terra Nova Bay, No Fib, Fra, FTIR PE, PP, Ny, PVC, PS, 300 300–5000 1.15–168.3 Munari et al.
Antarctica Fil PU, PVA, EPR, SBS particles m−2 (2017)
Shanghai, China -NaCl (1.19 g cm−3) Fib, Fra, μ-FTIR PP. PE, PES 20 300–5000 78.00 ± 12.91 Liu et al. (2018)
-H2O2 30% (50 °C, 72 h) Fil, Pel (top soils)
62.50 ± 12.97
(deep soils)
particles kg−1
Franconia, -H2O2 (20 ml) Fil, Fra, FTIR PE, PP, PS 1000 1000–5000 0.34 ± 0.36 Piehl et al.
Germany Fib particles kg−1 (2018)
Shandong, China -NaCl (1.2 g cm−3) Fra, Fo, FTIR PP, PE, PS 300 100–5000 1.3–14,712.5 Zhou et al.
-NaI (1.6 g cm−3) Fib, Pel, particles kg−1 (2018)
Fil
Nanjing and Wuxi, -H2O2 30% (70 °C) Fib, Fra μ-FTIR PE, PP, PET, PAN 20 200–5000 420–1290 Li et al. (2019)
China -NaCl (1.2 g cm−3) particles kg−1
-ZnCl2 (1.5 g cm−3)
-NaI (1.8 g cm−3)
Wuhan, China -30% KOH: NaClO Fra, Pel, Raman PE, PP, PS, PA, PVC 10 10–5000 2.2 × 105 particles Zhou et al.
-NaCl (1.2 g cm−3) Fib kg−1 (2019)
-ZnCl2 (1.5 g cm−3)
Danube River, -NaCl (1.2 g cm−3) Fib, Fra, Pyrolysis PET, PP, PTFE, PMMA, 20 1 159.2 ± 138.4 Pojar et al.
Romania-Bulgaria -KOH 10 M and H2O2 30% Fra, Pel GC–MS PAN, PS, EP particles kg−1 (2021)
(7 d)

Groundwater
Public fountains, No Fib. Fra μ-Raman PTT, EP 0.22 <500–5000 1800 ± 7000 Shruti et al.
Mexico particles m−3 (2020)
Groundwater, India -H2O2 30% Fe (II) Fib, Fo, FTIR PE, PA, PS 50 110–12,500 4200 particles Selvam et al.
Pel, Fil, m−3 (2021)

(continued on next page)

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Table 1 (continued)

Location Sample treatment Shapes Polymer Polymer type Method Size range (μm) Abundance Reference
identification lower size (particles unit−1)
limit (μm)

Fra
Groundwater, -HCl rinse Fra, Fib μ-FTIR PES, PVC, PE, PA EP 20 50–150 0–7 particles m−3 Mintenig et al.
Germany -H2O2 30% (40 °C, 24 h) (2019)
-ZnCl2 (1.6 g cm−3)
Karst groundwater, -Dried 75 °C, 24 h Fib py-GCMS PE 0.45 <1500 860–15,200 Panno et al.
EE.UU. particles m−3 (2019)

Lakes
Lake Victoria, Africa
-H2O2 30% Fe (II) Fra, Fil, FTIR LDPE, HDPE, PP, PS, 300 300–4900 0.02–2.19 Egessa et al.
-NaCl (6 g/20 ml) Fib, Fo PES particles m−3 (2020)
Lake Guaíba, Brazil -H2O2 35% Fe (II) Fra, Fib, μ-FTIR PP, PE, PTFE, PU, PS 60 5–5000 11.9–61.2 Bertoldi et al.
-NaI (1.6 g cm−3) Mic, particles m−3 (2021)
Lake Ontario (North -CaCl2 (1.4 g cm−3) Fib, Fra, FTIR PVC, PE, PET, PP, PA 125 1000 ± 900 800 ± 700 Grbic et al.
America) Fil, Fo, particles m−3 (2020)
Pel,
Lakes, Poland -H2O2 30% (72 h) Fib Raman PET, PU, PP, PE, PS 20 <1000–5000 4930 particles Kaliszewicz et al.
m−3 (2020)
9 Patagonian lakes, -H2O2 30% (40 °C 9 h) Fib, Fo, Raman PET, PU, PS, PP. 38 <200–5000 0.3–1.9 particles Alfonso et al.
Argentina Rub, m−3 (2020)
Fra, Fil
Lake Tollense, -H2O2 30% (7 d) Fib, Fra μ-Raman PP, PE, PET 63 63–5000 19–50 particles Tamminga and
Germany -NaClO (16.7 ml/50 ml) m−3 Fischer (2020)
-Nile red
20 urban lakes, -H2O2 30% (24 h) Fib, Pel, FTIR PET, PP, PE, Ny, PS 50 <500–5000 1660–8925 Wang et al.
Wuhan, China Fil, Gra particles m−3 (2017)
Poyang Lake, China -H2O2 30% (24 h) Fib, Fil, μ-Raman PP, PE 50 <100–5000 5000–34,000 Yuan et al.
Fra, Pel particles m−3 (2019)
Lake Simcoe, No Fib, Fra, FTIR and Raman PE, PP, PS, Ray, PU, 335 125–5000 0.4–1.3 particles Felismino et al.
Canada Fil, Fo, PVC, Acr, PA, PE m−3 (2021)
Mic
Lake Kallavesi, -NaOH (pH 12) and Fib, Fra μ-FTIR PE, PP, PET, PAN, PVC, 333 >300 0.27 ± 0.18 Uurasjärvi et al.
Finland sodium dodecyl sulfate PMMA, PS particles m−3 (2020)
(1 g L−1) (50 °C, 4 h)
-HCl neutralized

Rivers and effluents


Ganges River, India No Fib, Fra FTIR Ray, Acr, PET, PVC, 330 2459 ± 209 38 ± 4 MP Napper et al.
PS, Ny particles m−3 (2021)
Garonne River, -H2O2 30% (25 °C, 24 h) Fra, Fil, FTIR PE, PS, PP 500 700–5000 0.15 ± 0.46 de Carvalho
Spain-France Fib, Pel particles m−3 et al. (2021)
Rivers, Japan -H2O2 30% Fe (II) (70 °C) Fib, Fra FTIR PE, PP, PET, PS 5 50–1000 164,790 ± Kabir et al.
-ZnCl2 (1.5 g cm−3) 171,910 particles (2021)
m−3
Langueyú stream, -H2O2 30% (50 °C, 4 h) Fib, Fra Raman PET, PA, 44 5–<1000 8.7 × 106 particles Montecinos
Argentina m−3 et al. (2021)
Ballenas Stream, -H2O2 33% (60 °C, 24 h) Fib, Fil μ-FTIR PE, Acr, PTFE 100 400–3546 (Fib) 0.00095 particles González-Pleiter
Antarctica -NaCl (36 g/100 ml) 10–1026 (Fil) m−3 et al. (2020)
WWTP, Israel -H2O2 30% Fe (II) (70 °C) Fib, Fra, μ-Raman PET, PVC, PP, PC, 20 1687–1879 (Fib) 65,000 (raw Ben-David et al.
-NaCl (6 g/20 ml) Fil, Pel, PFTE, PU, Ny, PO 308–568 (other) water) (2021)
Fo 2720 (2-step)
1970 (3-step)
particles m−3
4 Rivers, Taiwan -H2O2 35% (30 °C, 24 h) Fra, Fil, FTIR NA 300 300–5000 2.5–83.7 particles G. Wong et al.
Fo, Pel, m−3 (2020a)
Fib
Thames River, UK -KOH 40% (40 °C, 24 h) Fil, Fra, FTIR PE, PP, PEST, Ny, Acr 32 35–5000 8–36.7 particles Rowley et al.
Mic, Pel m−3 (2020)
Netravathi River, -H2O2 30% Fe (II) (75 °C) Fra, Fo, FTIR PE, PP, PET, PVC 300 300–5000 288 particles m−3 Amrutha and
India -ZnCl Fib, Pel Warrier (2020)
Haihe River, China -H2O2 30% (24 h) Fib, Fra, μ-FTIR PE, PA, PS, PP, PU, PET 333 <50–5000 0.69–74.95 Liu et al. (2020)
-NaCl (1.2 g cm−3) Fo, Fil, particles m−3
Pel

Estuaries
Dongshan Bay -H2O2 30% Fe (II) Fo, Fra, Raman PP, PE, PS PA, PE-PP, 330 300 – 5000 0.23–4.01 Pan et al. (2021)
Estuary, China -NaCl (1.19 g cm−3) Fib, Pel, PET particles m−3
Li
Pearl Estuary, China -H2O2 30% (60 °C, 24-72 Fo, Fib, FTIR PE, LDPE, PP, PS, EVA, 355 355–5000 2.376 ± 0.700 Lam et al.
h) Fil, Fra, EPDM particles m−3 (2020)
-NaCl (1.2 g cm−3) Pel
Benoa Bay Estuary, -H2O2 30% (60 °C, 24-48 Fib, Fra, μ-FTIR PP, PE, PS, Ny 300 <300–>1000 0.15–0.36 Suteja et al.
Indonesia h) Gra, Fo particles m−3 (2021)
Chesapeake Bay, EE. -H2O2 30% Fe (II) (75 °C) Fra, Fil, FTIR PE, PP, PS 330 100–8100 0.160 ± 0.287 Bikker et al.
UU. -NaCl (6 g/20 ml) Fib, Fo, particles m−3 (2020)
Pel

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M.B. Alfonso, A.H. Arias, A.C. Ronda et al. Science of the Total Environment 799 (2021) 149447

Table 1 (continued)

Location Sample treatment Shapes Polymer Polymer type Method Size range (μm) Abundance Reference
identification lower size (particles unit−1)
limit (μm)

Minjiang, Jiaojiang -Enzymatic digestion Fib, Gra Raman PE, PP, PVC, PTFE 333 500–5000 100–4100 Zhao et al.
and Oujiang particles m−3 (2015)
estuaries, China
Changjiang Estuary, -H2O2 30% Fib, Fil, FTIR PE, PP, PET, PA, Ny, 60 60–4953 157.2 ± 75.8 Zhao et al.
China Fra PS, PVC PC, PU, ASA, particles m−3 (2019)
ABS
Mississippi and -H2O2 30% Fe (II) Fra, Fib, Laser Direct PE, PP, PU, PA, PP, PE, 25 25–5000 30,000–192,000 Scircle et al.
Alabama coasts Mic Infrared (LDIR) PTFE particles m−3 (2020)
(Gulf of Mexico)
Klang River estuary, -H2O2 30% Fe (II) Fib, Pel, FTIR PA, PE 0.45 66.91–4133 500–4500 Zaki et al.
Malaysia -NaCl 5 M Fra particles m−3 (2021)
Sado estuary, -KOH 10% (25 °C, 48 h) Fra, Fo, FTIR PE, PP, PS, PVA, Ray, 335 335–5000 0.45 ± 0.52 Rodrigues et al.
Portugal -NaCl (1.2 g cm−3) Fil, Fib, PU, PA, PES particles m−3 (2020)
Mic
Haraz River estuary, -H2O2 30% Fe (II) Fra, Fil, Differential EVA, LDPE, PA, 300 NA 1.42–5.27 Naeeji et al.
Iran -NaCl (300 g L−1) Fib, Pel scanning particles m−3 (2020)
calorimetry
(DSC)

Abbreviations: foam (Fo), fragment (Fra), fiber (Fib), pellet (Pel), film (Fil), line (Li) granule (Gra), microbead (Mic), rubber (Rub), ethylene vinyl acetate (EVA), polyethylene chlorinated
(CPE), polyurethane (PU), polypropylene (PP), polyethylene (PE), polystyrene (PS), polyamide (PA), polyester (PES), polyethylene terephthalate (PET), polyacrylate (PAK), polyvinyl stea-
rate (PVS), ethylene/propylene copolymer (EPC), styrene/butadiene rubber (SBR), ethylene/propylene/diene rubber (EPDM), polyacrylonitrile (PAN), polycarbonate (PC), epoxy resin
(EP), alkyd resin (ALK), poly(vinyl acetate) (PVA), poly (trimethylene terephthalate) (PTT), poly-tetrafluoroethylene (PTFE), rayon (Ray), acrylic (Acr), Nylon (Ny), polyolefin elastomer
(PO), styrene-butadiene-styrene copolymer (SBS), Polymethylmethacrylate (PMMA), Styrene acrylonitrile (SAN), acrylate styrene acrylonitrile (ASA), acrylonitrile butadiene styrene
(ABS), not available (NA).

areas (Brahney et al., 2020), sea air samplings (Liu et al., 2019), and lab cited as critical MPs' pollution sources in soils worldwide (Fig. 2). How-
experiments (Bullard et al., 2021). SAMPs registered concentrations ever, sewage sludge from WWTP application in agricultural lands was rec-
were varied (Table 1), ranging from up to 1.37 particles m−3 for the ognized as the main problem (van den Berg et al., 2020). Nizzetto et al.
western Pacific Ocean (Liu et al., 2019), more than 450 SAMPs m−2 (2016a) estimated an annual input in European and North America soils
day−1 in French Pyrenees (Allen et al., 2019) to up to 1008 particles around 63,000–430,000 and 44,000–300,000 tons y−1, respectively,
m−2 day−1 in London (Wright et al., 2020). A consensus about the sam- even exceeding the MPs amounts in the oceans (93,000–236,000
pling methodology and the units used to express the results is still tons y−1) estimated by van Sebille et al. (2015). Due to MPs' hydrophobic-
needed (Table 1). Regardless, it could be inferred that SAMPs concentra- ity, it was pointed out that their presence could lead to changes in soil
tions decreased from those measured in urban centers to those mea- structure (Du et al., 2021).
sured in remote environments (Table 1). MPs concentrations in soil were varied (Table 1). Studies in farm-
Particles size ranged from small particles around 20 μm to larger lands with sewage sludge application registered values from up to
microfibers up to 5000 μm (Table 1). According to their shape, fibers 10,400 particles kg−1 in Chile (Corradini et al., 2019) to up to 430,000
were the most registered, with values between 60% (Liu et al., 2019) and 300,000 particles tons y−1 in farmlands from Europe and North
and 92% of the total sample (Wright et al., 2020). Nevertheless, Allen America, respectively (Nizzetto et al., 2016a). Practices as plastic
et al. (2019) found fragments as the most prevalent shape of SAMPs mulching to improve production conditions (e.g., temperature regula-
samples. These differences could be explained by the sources of the dif- tion, decreasing evapotranspiration, weeds control) lead to up to
ferent particles associated with each study. For example, based on a 502 kg ha−1 of plastic film in soils from China (Zhang et al., 2016). An-
high spatiotemporal resolution study, Brahney et al. (2020) affirmed other study found that MPs particles increased over time in the loca-
that fibers dominated the SAMPs samples, suggesting laundry drying tions where plastic mulching was continuously employed, with mean
as a significant pollution source in natural protected areas from the concentrations values between 80.3 particles kg−1 (5 years) and
United States, even more than the laundry washing process (Pirc et al., 1075.6 particles kg−1 (24 years) in soil fields (Huang et al., 2020).
2016). Alarming deposition rates were estimated at over 1000 metric Also, a recent study in soils with different human influence (agricultural
tons y−1 for these protected lands (Brahney et al., 2020). Finally, the areas, drains, dumping sites, industrial areas, lawns, parks, roadsides,
most common polymers in SAMPs studies were PE, PS, and PP and wastelands) within Lahore district (Pakistan) registered values
(Table 1). Therefore, according to these results, SAMPs could be critical from 1750 to 12,200 particles kg−1 (Rafique et al., 2020). These values
MPs pollution sources, both continental and in the ocean, but more put agricultural and urban soils as significant sources and sinks of MPs
studies are needed to determine if their fluxes are significant. pollution worldwide and are responsible for the varied registered con-
centrations (Table 1). In many studies, agro-industrial activities and
3.2. Soil human littering were the primary plastic pollution sources (Nizzetto
et al., 2016a; Rafique et al., 2020), suggesting that improvements in
MPs presence in soils received more attention than the atmosphere management and legislation resources are highly required.
but significantly less concerning freshwater environments (Fig. 1). Another source of MPs in the soil is vehicle tire abrasion, reporting
More studies should be carried out, considering that soils were pointed global average emissions of 6.1 million tonnes year−1 for tire wear par-
out as leading long-term sinks for MPs (Rochman, 2018; Wang et al., ticles (Kole et al., 2017). A study in Japan, Vietnam, and Nepal registered
2020). Polymer particles' size ranged from 10 μm to 5000 μm MPs in road dust of three urban cities with values of up to 39.6 particles
(Table 1), with fibers and fragments as the most prevailing shapes m−2 (Yukioka et al., 2020). For those soils near aquatic systems, high
(Table 1). Concerning polymer composition, PE and PP were dominant MPs concentrations were also registered. A study in coastal soils near
(Table 1). The use of plasticulture in agriculture (Wang et al., 2019), the Bohai Sea and Yellow Sea (China) presented concentrations of up
open waste dumping (Wang et al., 2020), road littering, tires abrasion to 14,712.5 particles kg−1 (Zhou et al., 2018). The authors associated
(Yukioka et al., 2020), and landfills (Bläsing and Amelung, 2018) are those values with aquaculture, port construction, and tourism

7
M.B. Alfonso, A.H. Arias, A.C. Ronda et al. Science of the Total Environment 799 (2021) 149447

(Zhou et al., 2018). A recent study in riparian soils from the Yangtze According to Siegfried et al. (2017), pollution emissions from
River found values between 4005 ± 2472 particles kg−1 (sub-soils) European rivers differed depending on their socio-economic status
and 3748 ± 2301 particles kg−1 (topsoils), suggesting that sub-soils re- and WWTP technology. MPs concentrations in rivers were varied
tain significantly more MPs particles (Zhou et al., 2021). Also, the higher (Table 1), from only 0.00095 particles m−3 for a stream in a conserva-
values were registered in the river's lowest reaches, with small MPs par- tional area from Antarctica (González-Pleiter et al., 2020), 0.15 particles
ticles (<200 μm) accounting near 70% of samples (Zhou et al., 2021). m−3 in the Garonne River, France (de Carvalho et al., 2021) to up to 288
These results highlight the need for long-term research, including dif- particles m−3 in Netravathi River, India (Amrutha and Warrier, 2020).
ferent soil fractions and sites, to arrive at better conclusions about plas- From these values, it could be inferred that the affirmations of
tic pollution sources and fate in terrestrial ecosystems. Siegfried et al. (2017) could also be extrapolated worldwide according
to countries' economies. Looking at the General National Income per
3.3. Lakes capita (GNIPC) provided by The World Bank information in 2019 for
these examples (https://datacatalog.worldbank.org/dataset/gni-capita-
MPs pollution studies are critical in freshwater systems because of ranking-atlas-method-and-ppp-based), France has one of the highest
their role as biodiversity hotspots and drinking water sources and be- (USD 42,450 per capita), meanwhile for India was USD 2120. A recent
cause they provide valuable information on the MPs flow from conti- study estimated up to 3 billion particles d−1 being discharged into the
nental reservoirs to the oceans. From the continental MPs' research, Bengal Bay in India (Napper et al., 2021). Furthermore, considering
rivers, lakes, and estuarine systems were the most studied worldwide Lebreton et al. (2017) estimations, more than 90% of plastic inputs
(Fig. 1), suggesting wastewater treatment plants (WWTP) near urban corresponded to the top 122 polluting rivers (4% of total surface area
centers, sport and commercial fishing, water management, tourism, and 36% of the global population), from which 103 are located in Asia
and inappropriate plastic disposal as the leading pollution sources in (GNIPC USD 11,734), eight in Africa (GNIPC USD 7880), eight in South
lakes (Sighicelli et al., 2018; Arias et al., 2019; Alfonso et al., 2020; and Central America (GNIPC USD 8794) and only one in Europe
Meng et al., 2020; Xia et al., 2020; de Carvalho et al., 2021; Napper (GNIPC USD 25,205). Nevertheless, we should consider that the number
et al., 2021). of carried studies could provide biased global estimations. Some regions
During the last years, the number of articles on MPs levels in lakes as South America and the Caribbean, Africa, and Asia (except China)
increased (Table 1); nevertheless, in regions such as South America present low (or lack of) studies. So, their role in the release of MPs
(Alfonso et al., 2020; Bertoldi et al., 2021), the Middle East (Picó et al., could be much significant than the one estimated. The same problem
2020), and Africa (Egessa et al., 2020) research efforts should keep was observed for global MPs estimations in the oceans (Isobe et al.,
growing to balance the baseline data available for North America, 2019), so more studies are still needed in these regions.
Europe, Oceania and Asia (Table 1). In lakes, similar or higher MPs con- Finally, in the last years, MPs' presence started to be recorded in
centrations were registered compared to marine systems (Table 1). groundwater systems (Table 1). A study in EE.UU. karst aquifers regis-
Registered values varied from 0.9 particles m−3 in nine Patagonian tered concentrations up to 15,200 particles m−3 (Panno et al., 2019).
lakes (South America) (Alfonso et al., 2020), 800 particles m−3 in Lake Another study analyzed MPs' presence through the drinking water sup-
Ontario (Grbic et al., 2020) to up to 34,000 particles m−3 in Poyang ply chain, from groundwater to drinking water (Mintenig et al., 2019).
Lake (Asia) (Yuan et al., 2019). Among MPs, fragments, and fibers less According to the authors, concentrations were low and varied from 0
than 1 mm dominated water samples, with PE, PP, and PET as the to 7000 particles m−3, registering polymers like PE, PA, PS, and PVC
most common polymers (Table 1). Researchers coincide that strategies (Mintenig et al., 2019). A study in Mexico considered that drinking
such as improving waste management, plastic recycling, and preventing water fountains with groundwater supply were MPs hotspots for
illegal dumping in areas close to these essential water resources should human consumption, registering high average concentrations (18,000
be promoted and implemented (Alfonso et al., 2020; Egessa et al., 2020). ± 7000 particles m−3) (Shruti et al., 2020). Polymer identification
These are particularly relevant under the COVID-19 pandemic, where found poly-trimethylene terephthalate (PTT) and epoxy resins, suggest-
the use of SUP, gloves, and face masks has increased significantly world- ing contamination from wastewater (Shruti et al., 2020). Finally, a study
wide, and stars to being reported in the environment (Ormaza- in India groundwaters registered concentrations of up to 10,100 parti-
González and Castr-Rodas, 2020; Prata et al., 2020; De-La-Torre et al., cles m−3, identifying polymers like PA, PE, and PS (Selvam et al.,
2021). 2021). The authors suggested septic systems, sinkholes, and municipal
sewage systems as potential MPs sources (Selvam et al., 2021). These
3.4. Rivers, effluents, and groundwater results confirm the ubiquitous presence of plastics in the environment
and highlight aquifers' vulnerability to MPs contamination.
Rivers and estuaries worldwide were recognized as significant MPs
contributors to oceans pollution depending on their contamination 3.5. Estuaries
level (Lebreton et al., 2017). It was estimated that up to 2.41 million
tons y−1 of plastic waste from rivers enter the ocean, mainly between Estuarine systems are the limit between freshwater and marine en-
May and October (Lebreton et al., 2017). Besides non-point pollution vironments, receiving and contributing significantly to oceans MPs con-
sources, WWTP are a significant source of MPs in rivers. Despite their centrations (Andrady, 2011; Figueiredo and Vianna, 2018; Arias et al.,
particle removal efficiencies (97%) (Ben-David et al., 2021), high con- 2019). Therefore, estuaries have been documented as plastic pollution
centrations were reported for treated wastewater in Europe, Middle hotspots (Lam et al., 2020). Registered concentrations worldwide
East, EE.UU., and Australia (up to 447,000 particles m−3) (Sun et al., ranged from up to 0.31 particles m−3 in the Juagaribe and the
2019; Ben-David et al., 2021). Furthermore, coinciding with those poly- Timonha-Ubatuba estuaries (Brazil) (Garcia et al., 2020) to up to
mers registered for lakes and oceans (Table 1), PE, PET, PS, and PA 381,000 particles m−3 in Mississippi and Alabama coasts (Gulf of
microfibers prevailed in WWTP samples (Sun et al., 2019; Ben-David Mexico) (Scircle et al., 2020). According to Scircle et al. (2020), MPs con-
et al., 2021). Their dominance could be explained by the massive use centrations increased from the river towards the sea because of frag-
of synthetic polymers in textiles and plastics manufacturing and their mentation into smaller particles. Also, a study in Pearl River Estuary
long thin shape that goes through filters (Ben-David et al., 2021). A re- (China) found higher concentrations in the river's mouth (4357 parti-
cent conservative study for global WWTP emissions estimated around cles m−3) (Lam et al., 2020). These results confirm estuaries' role as po-
1.47 × 1015 particles y−1, whereas the discharge of untreated effluent tential MPs hotspots, which will eventually end in the ocean. Among the
(which accounts for more than 50%) to aquatic environments was registered polymers, PE, PP, and PS were mostly cited (Table 1). Accord-
3.85 × 1016 particles y−1 (Uddin et al., 2020). ing to Pan et al. (2021), the widespread use of these polymers' foams in

8
M.B. Alfonso, A.H. Arias, A.C. Ronda et al. Science of the Total Environment 799 (2021) 149447

local fishing and aquaculture could explain their dominance. Further- 4.1. Atmospheric transport and fallout
more, a study in Elbe River Estuary (Germany) registered 600,000-fold
higher MPs concentrations in sediments than in water (5.57 particles Atmospheric transport is a crucial global pathway for MPs (Zhang
m−3) (Scherer et al., 2020), highlighting the estuarine sediments func- et al., 2020). Through atmospheric fallout, plastic items can travel
tion as MPs final sinks, where plastic particles concentrate over time. from short distances in urban centers (Dris et al., 2017) to open ocean
Nevertheless, this could be affected by sediment depositions rates, and (Liu et al., 2019), and even to remote places as mountains (Allen et al.,
further research should be done. 2019; Zhang et al., 2019; Parolini et al., 2021). Such transportation
could strongly impact MPs dynamics worldwide and between different
4. Environmental microplastics' pathways reservoirs (Zhang et al., 2020). Despite the increase in SAMPs research,
we are far from completely understood their dispersal mechanisms (Liu
In the complex framework of MPs pathways, several cross-related et al., 2019). Only a few studies emphasize in the effect of environmen-
physicochemical, anthropogenic, and climate variables influence MPs' tal variables' on SAMPs presence; among them, rain, snow, and wind
presence and distribution in the environment. Among the MPs' environ- events are cited as responsible for SAMPs transport and deposition
mental reservoirs, wind resuspension and atmospheric fallout, runoff, (Dris et al., 2015; Dris et al., 2016; Liu et al., 2019; Brahney et al.,
freshwater hydrodynamics, tides, and ocean currents could be cited as 2020; Parolini et al., 2021).
the most prevalent ones (Lebreton et al., 2017; Isobe et al., 2019; Brahney et al. (2020) found differences between wet and dry depos-
Brahney et al., 2020; Xia et al., 2020). Nevertheless, there is still limited ited SAMPs from a study in the United States protected areas. The au-
information about the MPs flow between reservoirs to understand their thors suggest that short distance sources prevailed for SAMPs wet
global fate (Rochman and Hoellein, 2020; Zhu, 2021). Besides remedia- deposition events (near urban centers and soils or water resuspension).
tion actions (clean-ups, reduce littering, replace plastics with biode- In contrast, for dry-deposited SAMPs, due to their small size, long-range,
gradable materials, among others), increasing our knowledge about or even global transport was probable. Another study estimated the
monitoring and fluxes/pathways process on continental sources is crit- global transport and deposition of secondary SAMPs as tire wear parti-
ical to solving environmental plastic pollution. As a simplified MPs path- cles (TWPs) and brake wear particles (BWPs) (Evangeliou et al.,
ways conceptualization, agricultural and urban settlements act as the 2020). The authors found that climatic events as the North Atlantic Os-
leading continental source where MPs fluxes across a complex gradient cillation could enhance pollution transportation to remote areas, mainly
to soils, the atmosphere, and aquatic environments (Fig. 2, Table 2). Lit- in winter and spring. Furthermore, strong winds may remobilize depos-
tle is known about MPs' interactions with the environmental variables ited SAMPs, allowing their transport for larger distances, presenting a
such as the hydrodynamics conditions (seasonal water flow, velocity, kind of “grasshopper effect” as other persistent organic pollutants
turbulence, flow, and water depth), catchments topography, salinity, (Evangeliou et al., 2020).
precipitations, runoff, and groundwater transportation, among others Concerning open ocean SAMPs deposition from the continent, differ-
(Table 2). ences between day and night were registered and attributed to relative

Table 2
Main environmental variables involved, key findings, and knowledge gaps for microplastics' environmental path-
ways on the continent.

Soil/ Groundwater
Atmospheric fallout Runoff Hydrodynamics
migration
9 Precipitation 9 Precipitation 9 Rainfall 9 Density/ Wind-
9 Wind 9 Soil conditions driven circulations
9 Relative humidity 9 Turbulence
Environmental 9 Systems
variables morphology
9 Flow rate

9 Grasshopper effect 9 First flush effect 9 Lag time effects 9 Long-range/ Small
9 Short-range/ Wet 9 Lag time/ Storm by surface MPs
deposition sewers irregularities 9 Short-range/ Large
9 Large range/ Dry 9 Riverbank 9 Smaller MPs MPs
Key deposition resuspension 9 Surface/ septic 9 Hotspots by
findings systems sources sedimentation,
wind, circulation,
inputs

9 More studies needed 9 Seasonality 9 More studies 9 Spatio-temporal


9 Seasonality 9 Spatio-temporal needed patterns
Particular 9 Daytime/nighttime patterns 9 Hotspots
knowledge 9 Hydrodynamics
gaps 9 Climate variability

9Interdisciplinary research including more physicochemical and climatic variables


9Quantify fluxes among MPs’ reservoirs
9Harmonization of the methodology, units, and nomenclature
General 9Increase the number of studies on non-developing countries
knowledge 9Prioritized long term over high spatial cover
gaps 9Assessment of specific pollution sources
9Effect of economic level development on MPs distribution

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M.B. Alfonso, A.H. Arias, A.C. Ronda et al. Science of the Total Environment 799 (2021) 149447

humidity conditions (Liu et al., 2019). Specifically, the authors found input balance between southern (East Asia and the Indian Subconti-
that SAMPs pollution decreased ten times from the coastal area towards nent) and northern (Southeast Asia) hemisphere summers (Lebreton
the ocean, being up to twice as abundant during the daytime than dur- et al., 2017). Therefore, local to global spatiotemporal patterns should
ing the nighttime. SAMPs settlement was enhanced by the high relative be considered when studying MPs runoff pathways.
humidity conditions at night, especially on the sea (Liu et al., 2019), sug-
gesting that nighttime hours enhanced SAMPs settlement, increasing 4.3. Groundwater migration
their amount entering to oceans from the atmosphere. Moreover, in a
recent study, Allen et al. (2020) also demonstrate the inverse pathway Little is known and discussed about groundwater migration, which
for SAMPs deposition from seas to the continent. The authors registered is critical considering that drinking water comes from many groundwa-
onshore MPs transported by sea spray, estimating that near 136,000 ter sources (Mintenig et al., 2019; Panno et al., 2019). A recent study
particles ton y−1 leave the ocean by this pathway (Allen et al., 2020). comparing MPs presence in surface and groundwaters from India
These results confirm that continental atmospheric transport (by rain, found that the latter presented smaller MPs (Selvam et al., 2021). Ac-
snow, or wind) is an essential pathway to other environmental MPs' cording to the authors, as MPs migrate from the surface into underlying
reservoirs (soils, freshwater, ocean). Sampling conditions as wind aquifers through soil fractures, larger MPs (0.34–4.30 mm) are retained
speed, relative humidity, time, and seasons are crucial in SAMPs moni- by surface irregularities, with only small MPs (0.12–2.50 mm) reaching
toring and modeling to understand this complex process. the groundwater. Furthermore, groundwaters' lower MPs levels suggest
the existence of retardation during filtration in aquifer lithologies
4.2. Precipitation and runoff (Selvam et al., 2021). Polymer identifications in these plastic particles
suggest that besides surface water inputs, contamination from septic
As was discussed in the previous section, precipitation events affect systems are possible contamination source (Panno et al., 2019; Selvam
MPs' presence and dispersal in the environment. Once MPs are depos- et al., 2021). These results agree with other studies which conceptual-
ited from the atmosphere, they could be transported by runoff from ized that once in the soils (by WWTP or greywater discharge, septic
the continental anthropogenic sources (urban and agricultural areas) tank outflows, or contaminated water injection for aquifer recharge),
towards freshwater aquatic systems to finally reach the ocean (Xia MPs can reach aquifer systems due to leaching or infiltration in soil
et al., 2020). Allen et al. (2019) found that the frequency and intensity pores (Re, 2019; Kim and Lee, 2020). According to Panno et al. (2019),
of rainfall and snowfall events are more relevant than duration. Also, re- surface MPs could migrate to groundwater through crevices, conduits,
cent studies remarked on the importance of rainfall and the first flush branch work caves, springs, and associated sinkholes. Nevertheless,
effect over MPs and associated contaminants dispersion (Piñon-Colin more studies about how this migration process develops and its relation
et al., 2020). This process explains that as the runoff surface increases to other environmental variables as rainfall and soil characteristics are
during a rainfall event, high concentrations of pollutants are recorded still needed to achieve better conclusions.
at the beginning of the event to decrease gradually later (Piñon-Colin
et al., 2020). Nevertheless, MPs' emission estimates' accuracy is cur- 4.4. Freshwater hydrodynamics
rently hindered by the lack of data about MPs' transport efficiency in
runoff water and streams. Another factor to consider when MPs are studied in lakes and rivers
A study in the Keelung River and the Xindian River (Taiwan) found is that hydrodynamics determine the speed at which MPs arrive at the
positive correlations between precipitations and MPs concentrations ocean. We can assume that for a singular plastic particle, the buoyancy
(G. Wong et al., 2020a). This positive relation was also registered in riv- will be different in the case of estuaries where freshwater and saline
ers such as Los Angeles River in the United States (Moore et al., 2011), water effects are combined added to turbulence, which will interact
River Seine in France (Dris et al., 2015), and Venoge River in with particle size, density, and charge, in comparison with freshwater
Switzerland (Faure et al., 2015). According to G. Wong et al. (2020a), environments as rivers (Eerkes-Medrano et al., 2015; Leslie et al.,
this could be explained by the deposited MPs' resuspension in the 2017; J. K. H. Wong et al., 2020b). Therefore, greater particle flocculation
river banks. The authors also suggest that when the storm sewers net- and deposition will be observed in estuaries in comparison with other
work is not connected to WWTP, all kinds of pollutants directly flow aquatic environments. Modeling advances in aquatic systems and the
into the rivers through runoff (G. Wong et al., 2020a). They also re- MPs baseline data clarify the mechanisms influencing these particles'
ported an increased land-based number of MPs after heavy rainfall presence and distribution pathways in diverse aquatic environments.
events. Furthermore, the authors suggest 24 h lag period between the A study based on a literature review performed a hydrological model
rainfall and the MPs increased levels, corresponding to the time that to determine spherical MPs fate and transport (100 nm to 10 mm)
the rainwater takes to drag the particles from land into the storm sewers (Besseling et al., 2017). The authors assessed the advective transport ef-
and finally deposit them in the river (G. Wong et al., 2020a). Therefore, fect, homo- and hetero-aggregation, sedimentation-resuspension, poly-
studies about the rainfall events' influence on MPs dispersion are critical mer degradation, biofilm presence, and burial (Besseling et al., 2017).
considering rainfall spatiotemporal variations and that more frequent They found that river hydrodynamics affect MPs size distributions
and intense events are expected in the future (Westra et al., 2013). with consequences in their emission to the ocean. Characteristics such
Depending on precipitation patterns (G. Wong et al., 2020a), catch- as river width, depth, and flow rate could determine net sedimentation
ment soil characteristics (Nizzetto et al., 2016b), and river hydrodynam- and resuspension areas (Quik et al., 2015).
ics (Besseling et al., 2017), MPs retention as well as vertical distribution On the other hand, a study in the Thames River upgraded a mathe-
may vary significantly along with rivers (Lebreton et al., 2017). Studies matical model to assess catchment hydrology, soil erosion, and sedi-
in rivers registered temporal differences in MPs concentrations associ- ment budget effects on rivers' MPs fate (Nizzetto et al., 2016b). The
ated with seasonal rainfall differences and runoff (Moore et al., 2011; model assumed that physical controls on soil erosion and sediment
Yonkos et al., 2014). These results emphasize the role of runoff and transport are the same that control MPs' transport. According to their
the seasonality of freshwater contamination by MPs. Also, global runoff results, those particles with a size <0.2 mm will not be retained in
spatiotemporal patterns influence MPs distribution. A study found two streams, whereas larger particles with higher densities than water will
distinct plastic input peaks in rivers: between June and October from be retained in sediments, which could be remobilized under high flow
African, North, and Central American rivers and between November to periods. Furthermore, these authors concluded that those river sections
May from European, South American, and Australia-Pacific rivers experiencing low stream power are likely hotspots for MPs deposition
(Lebreton et al., 2017). According to the authors, rainfall and runoff pat- on sediments (Nizzetto et al., 2016b). Therefore, MPs storage in soils
terns for Asia are not as pronounced as for other continents due to the and river sediments should be considered temporary or permanent

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M.B. Alfonso, A.H. Arias, A.C. Ronda et al. Science of the Total Environment 799 (2021) 149447

sinks of relevance, contributing to the MPs' delay or prevention to reach recent study quantified the wet and dry MPs fallout suggesting that as
the marine environment. Similar results were found in a recent study in in the case of soil transport (Mahowald et al., 2014), those MPs with a
the Vaal River, Africa (Weideman et al., 2020). According to the authors, size <25 μm can be transported in a long-range or global scale distance
during low flow periods, MPs were more abundant in the river's lower (Brahney et al., 2020) and the most prominent MPs as fiber can be
reaches before the wet season flush. transported on a regional scale (10 to 1000 km) (Lawrence and Neff,
As it occurs in the ocean's subtropical convergence zones (van 2009). Moreover, if we consider that MPs densities are lower than
Sebille et al., 2015), internal freshwater currents could be responsible those of soil particles (0.65–1.8 g cm−3 vs. ~2.65 g cm−3), it can be ex-
for accumulating plastic particles. Previous studies in large lakes as the pected that MPs will be more transportable. Also, microfibers with
Laurentian Great lakes or Qinghai Lake found that plastic debris distri- higher surface area/volume ratios will increase dragging forces and re-
bution was affected by the lake currents (Hoffman and Hittinger, duce settling velocities (Brahney et al., 2020). Therefore, according to
2017; Xiong et al., 2018). Moreover, source inputs and wind direction these results, it is expected that large MPs and wet deposition will con-
could be responsible for MPs distribution in some small lakes (Imhof tribute less than dry deposition, highlighting the role of regional storms
et al., 2013; Free et al., 2014; Zhang et al., 2016). Finally, for estuarine in the local fallout of MPs and atmospheric patterns to a global scale dis-
systems, a recent study assessed the MPs distribution patterns in a persion (Brahney et al., 2020). Annual deposition maps show that
coastal upwelling environment, Ría de Vigo estuary (Spain). Using smaller road microplastic particles (diameter < 2.5 μm, PM 2.5) are dis-
water and sediment MPs field data during upwelling and downwelling persed more widely than larger ones (diameter < 10 μm, PM10). PM10
conditions and 2D-vertical modeling, the authors investigated the rela- road microplastics were deposited mainly close to the hotspot emission
tive importance of river discharge, wind-driven, and density-driven cir- regions (North America, Europe, and South-eastern Asia) (Evangeliou
culation (Díez-Minguito et al., 2020). According to their results, wind et al., 2020). Nevertheless, other studies proved that Saharan dust parti-
force was the leading MPs' mobilization/sedimentation driver, and cles of up to 450 μm traveled long trans-oceanic distances (van der Does
more significant for water circulation than the density-driven and et al., 2018). Therefore, more research is needed to understand the size
river flows circulation. The authors also observed that MPs' presence limits of SAMPs transport.
was higher in surface waters at the estuary's outer half during upwell- In the case of rivers, it was found that larger MPs traveled shorter
ing. The flush out of MPs to the sea was affected by wind-induced circu- distances, being registered mainly in the river upper reaches, whereas
lation in the water surface. Whereas, near the bottom, the effect of wind the smallest traveled longer distances, prevailing in the river's lower
landward and gravitational circulation produces maximum MPs con- reaches (Weideman et al., 2020). These results coincided with previous
centration inside the estuary (Díez-Minguito et al., 2020). Therefore, ac- mathematical models, showing that smaller MPs would not be retained
cording to their modeling results, MPs circulation pathways are in streams traveling with the river flow (Nizzetto et al., 2016b). In con-
dominated by winds in the outer part of estuarine environments and trast, it has been reported that larger particles are prone to be retained
by gravitational circulation in the internal area. Nevertheless, according in sediments (Nizzetto et al., 2016b). Nevertheless, in another study,
to Wolanski and Elliott (2015), MPs transport in lower rivers and estu- Besseling et al. (2017) observed heteroaggregates formation between
aries could differ among studies because of their differences in river suspended solids and MPs. The authors conclude that intermediate-
morphology and tidal activity, tidal currents, circulation, and estuary sized particles of about 5 mm will be less retained (18-25%) than the
geometry. smaller submicron size range particles as well as micro and
millimeter-sized MPs (Besseling et al., 2017). Also, Enders et al.
5. Considerations about MPs features: shape, size, and polymer (2015) found that MPs size affects the vertical dispersion in aquatic sys-
composition tems, with larger items being less affected by turbulent mixing. Finally,
in groundwater MPs migration, those larger particles were more prone
This ubiquitous contaminant's main features, as size ranges, shapes, to be retained in the soil than the smallest ones (Selvam et al., 2021).
textures, and density, influence MPs' behavior in the environment. Therefore, further research is needed to understand how MPs size af-
About their shape, fibers are the most cited MPs type in worldwide fects their dispersion in these aquatic environments.
studies (Table 1), followed by fragments, and those related to atmo- Finally, the most cited polymers were PE, PP, and PET in the different
spheric deposition are not the exception (Dris et al., 2018; Liu et al., continental MPs' reservoirs (Table 1). This has sense considering that
2019). A recent study found that fibers (60%) dominate the SAMPs in 89% of the historical plastic waste exports consist of only these three
the Pacific Ocean, also accompanied by fragments (31%), granules polymers (Brooks et al., 2018). MPs' polymer composition and density
(8%), and microbeads (5%) (Liu et al., 2019). Concerning the shape of greatly influence their distribution in the environment. Plastic density
SAMPs composition, it was observed that samples become less diverse ranges are wide (0.011 g cm−3 for PS foam to 2.3 g cm−3 for
as the distance from the coastline increases (Liu et al., 2019). Also, it polytetrafluoroethylene (PTFE)) (Chubarenko et al., 2016). Most
was reported that SAMPs numbers decreased at night, being fibers the manufactured MPs have buoyant properties, so they float in the surface
shape that most decreased because they are prone to the settlement layer or are temporarily suspended in the water column (Li et al.,
due to their density and size. Bullard et al. (2021) made a series of 2020a). Those MPs with higher density or which density increase by
wind tunnel experiments with microbeads and fibers at different con- biofouling presented higher sinking rate in the water column
centrations, using sand and soil as substrates. The authors demonstrated (Besseling et al., 2017). There are also neutral MPs suspended in the
that MPs were preferentially transported by wind instead of the sub- water column, showing that researchers should consider analyzing
strates and that fiber shape was more favored than microbeads. These their presence in the water column and not only on the surface to
results highlight the importance of MPs shape consideration in SAMPs avoid underestimation. In the case of atmospheric fallout, Liu et al.
transportation models (Bullard et al., 2021). Whereas in aquatic envi- (2019) found a high percentage of PET in SAMPs samples and that the
ronments, it was empirically demonstrated that microfibers presented PET and PE–PP proportion decreased at night compared with the day-
the lowest velocity, followed by sheets and fragments (Reisser et al., time. These results could be explained by their density and hygroscop-
2015). icity properties and higher relative humidity conditions during the
When it comes to MPs size, no matter the involved MPs pathway, night (Liu et al., 2019). In accordance with these results, Allen et al.
most studies coincided that those smaller MPs will travel longer dis- (2019) also found differences in SAMPs composition depending on cli-
tances than the larger ones. This affirmation was demonstrated for at- mate variability. The authors registered higher PS (1.05 g cm−3) con-
mospheric fallout, river flow, and even groundwater migration studies centrations when rain or snow events were low and higher amounts
(Mahowald et al., 2014; Nizzetto et al., 2016b; Brahney et al., 2020; of PE (0.96 g cm−3) when these events increased, according to the dif-
Evangeliou et al., 2020; Weideman et al., 2020; Selvam et al., 2021). A ferences in polymers densities (Allen et al., 2019).

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M.B. Alfonso, A.H. Arias, A.C. Ronda et al. Science of the Total Environment 799 (2021) 149447

Also, plastic items have presented different resistance and mecha- and meteorological variables and prioritize long-term monitoring. Con-
nism formation of MPs according to their polymer's composition tinental environments are affected by point and non-point plastic in-
(Efimova et al., 2018). In this manner, a study evaluated the degradation puts, so it is crucial to improve pollution sources assessments and
effect of beach sea wash with coarse bottoms on plastics and found that avoid enumerating general categories (plastic disposal, fishing activi-
the MPs number that finally ends in the oceans was expected to increase ties, laundry, among others). It is worth mentioning that most plastic
(Efimova et al., 2018). With an experimental study using common poly- pollution research efforts were made in China, North America, and
mers registered in ecosystems as LDPE (bags), PP (single-use table- Europe whereas, studies in misrepresented areas as South America
ware), and PS (PS foam trays and solid PS tableware), the authors and the Caribbean, Middle East, and Africa are still needed. In this mat-
found that solid PS generated more MPs items and mass (Efimova ter, the relationship between countries' economies, WWTP available
et al., 2018). In contrast, PP (0.86 g cm−3) was the most resistant technologies, and pollution regulations need special attention in the fu-
(Efimova et al., 2018). Therefore, the contribution to MPs pollution ture to abate this global problem. Also, laboratory experiments about
from PS SUP as trays, cups, and food containers is expected to be higher particles characteristics and behavior in the environment are needed.
in the future. This will contribute to improve sampling protocols and not underesti-
mate their presence in the environment.
6. Conclusions, knowledge gaps, and future challenges Supplementary data to this article can be found online at https://doi.
org/10.1016/j.scitotenv.2021.149447.
MPs are among the contaminants of emerging concern being ubiqui-
tous in different environments, from marine, freshwater, terrestrial to Declaration of competing interest
the atmosphere. We can conclude that freshwater systems were the
most studied continental MPs reservoirs, with rivers and estuaries dis- The authors declare that they have no known competing financial
charges as the main MPs' pollution contributors to marine systems. Fi- interests or personal relationships that could have appeared to influ-
bers prevailed in MPs samples from all the environments, with PE, PP, ence the work reported in this paper.
PET, and PS as the dominant polymers and decreasing sizes with in-
creasing distance from their sources. The atmospheric deposition also References
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