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Science of the Total Environment 835 (2022) 155426

Contents lists available at ScienceDirect

Science of the Total Environment


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

Atmospheric deposition of anthropogenic particles and microplastics in


south-central Ontario, Canada

Brittany Welsh a, , Julian Aherne a, Andrew M. Paterson b, Huaxia Yao b, Chris McConnell b
a
School of the Environment, Trent University, Peterborough, Ontario K9L 0G2, Canada
b
Ministry of the Environment, Conservation and Parks, Dorset Environmental Science Centre, Dorset, Ontario P0A 1E0, Canada

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

• Anthropogenic particles and microplastics


were ubiquitous across the study area.
• Particles were dominated by fibres with
blue and red being the most common col-
ours.
• Polyethylene terephthalate and polyam-
ide were the most abundant polymers.
• The average microplastic deposition rate
was 7 mp/m2/day (range 4–9 mp/m2/
day).

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

Editor: Jay Gan Microplastics are ubiquitous in the environment; however, few studies have examined their abundance in atmospheric
deposition in pristine environments, remote from anthropogenic emission sources. In the current study, atmospheric
Keywords: deposition samples were collected for 13 months (February 2019–March 2020) from four precipitation chemistry
Plastic monitoring stations located in Muskoka-Haliburton, south-central Ontario, Canada. Anthropogenic particles
Microfibres
(i.e., synthetic particles but not necessarily plastic) were observed at each station with an average deposition rate of
Precipitation
Air pollution
57 particles/m2/day (range from 32 to 73 particles/m2/day). Of the anthropogenic particles identified, 12% were plas-
Background region tic resulting in an average microplastic (mp) deposition rate of 7 mp/m2/day (range 4–9 mp/m2/day). Approximately
85% of the particles were fibres with fragments comprising only 15%. The most common particle colours were blue
and red with 50% of the fragments and 84% of fibres being one of these two colours. Raman spectroscopy determined
that polyamide and polyethylene terephthalate were the two most abundant polymers at 24% and 19%, respectively.
Across the four stations anthropogenic particle concentrations were significantly related to wind speed (rs = 0.32 to
0.62) and temperature (rs = −0.53 to −0.84), with a noticeable increase in particle concentration when wind shifted
from the west (average of 7.2 mp/L) to the south-east (average of 11.5 mp/L). Faster wind speed resulted in a larger
airshed source area, and the seasonal effect associated with changes in temperature and wind direction led to changes
in potential source regions that were contributing microplastics, such as the Greater Toronto Area (>200 km away).

1. Introduction 2018). Microplastics are plastic particles less than 5 mm in size that can
originate from primary and secondary sources (Sa et al., 2018). Primary
Microplastics are a growing global concern due to their ubiquity in the microplastics are manufactured to be microscopic in size, such as
environment (Cole et al., 2011; Taylor et al., 2016; Lambert and Wagner, microbeads that are used in cosmetic products, cleaning products, and
textiles (Cole et al., 2011; Li et al., 2018; Lambert and Wagner, 2018). In
⁎ Corresponding author. contrast, secondary microplastics are fragments that arise through the
E-mail address: brittanywelsh@trentu.ca (B. Welsh). breakdown and weathering of larger plastic pieces in the environment,

http://dx.doi.org/10.1016/j.scitotenv.2022.155426
Received 2 February 2022; Received in revised form 13 April 2022; Accepted 17 April 2022
Available online 22 April 2022

0048-9697/© 2022 Elsevier B.V. All rights reserved.


B. Welsh et al. Science of the Total Environment 835 (2022) 155426

through biological degradation, mechanical transformations, or UV radia- The objective of this study was to evaluate the abundance of anthropo-
tion (Cole et al., 2011; Driedger et al., 2015; Sa et al., 2018). Microplastic genic particles and microplastics in atmospheric deposition in relatively
particles can occur in a variety of different shapes, such as pellets, films, pristine locations in Muskoka-Haliburton, south-central Ontario, Canada.
foams, fragments, and fibres, which is largely dependent on the source of Further, the relationship between microplastics and meteorological vari-
the microplastics (Akdogan and Guven, 2019). Microfibres are small syn- ables was examined to evaluate the potential role of long-range atmo-
thetic fibres that vary in length, diameter, colour, and polymer type, and spheric transport.
are primarily released into the environment during textile production and
use, while secondary microfibres arise through the fragmentation of larger 2. Materials and methods
synthetic textiles (Akdogan and Guven, 2019; Henry et al., 2019). Common
synthetic polymers include nylon, polyester, and acrylic; particles comprised 2.1. Study area and sites
of cotton, wool or silk are not plastic but rather anthropogenic particles,
i.e., natural fibres containing anthropogenic (synthetic) dyes and chemical The Muskoka-Haliburton region is comprised of two adjacent regional
additives but not plastic (Carr, 2017; Rodríguez-Romeu et al., 2020). municipalities in south-central Ontario, Canada, the District Municipality
Microplastics may pose a serious risk to organisms due to their long res- of Muskoka, more commonly referred to as ‘Muskoka’, and Haliburton
idence time, tendency to cause physical harm via blockage and abrasion County (Fig. 1). The region, which is located approximately 2.5 h (200
when ingested, and potential to accumulate in food webs (Wright et al., km) north of Toronto, is commonly referred to as cottage country as it
2013; Sussarellu et al., 2016; Li et al., 2018; Kallenbach et al., 2022; sees more than 2.1 million tourists and visitors each year during the sum-
Gomes et al., 2021). Further, microplastics can adsorb and accumulate mer period. The region spans 8041 km2, has a year-round population of
toxic compounds, such as persistent organic pollutants, trace elements, 78,661 and contains more than 1200 lakes. The Muskoka-Haliburton
pharmaceuticals, and pathogens (Hirai et al., 2011; Mato et al., 2001; region has a humid continental climate with a 30-year annual precipitation
Rochman et al., 2014). As such, ingestion of microplastics can also cause average of 1008 mm, of which approximately 30% falls as snow (Yao et al.,
harmful effects such as carcinogenesis, endocrine disruption, reproductive 2009).
disruption and neurotoxicity (Wright et al., 2013; Sussarellu et al., 2016; The current study focused on four precipitation chemistry monitoring
Li et al., 2018; Kallenbach et al., 2022; Gomes et al., 2021). stations, two with duplicate collectors, Plastic Lake (PCP and PCP2),
Numerous studies have detected large quantities of microplastics in ma- Heney Lake (HYP2), Solitaire Lake (SE2P), and Paint Lake (PT1P and
rine environments (Collignon et al., 2012; Desforges et al., 2014), rivers PT3P) in the Muskoka-Haliburton region (Fig. 1; Table 1). These stations
and freshwater lakes (e.g., Eriksen et al., 2013; Yonkos et al., 2014; Mani are part of a long-term monitoring program operated by the Ministry of
et al., 2016), and more recently terrestrial environments (e.g., Scheurer the Environment, Conservation and Parks (MECP) at the Dorset Environ-
and Bigalke, 2018; Crossman et al., 2020). In contrast, only a handful of mental Science Centre, to assess the impacts of long-range atmospheric
studies have characterized microplastics and/or microfibres in precipitation. transport and deposition of pollutants on water quality (Dillon and Molot,
Recent studies have quantified the atmospheric deposition of microfibres in 2005; Girard et al., 2007; James et al., 2022). All of the stations are remote,
Paris, France (Dris et al., 2016), Nottingham, England (Stanton et al., i.e., more than 200 km from large urban or industrial centers and are lo-
2019), and coastal regions in Ireland (Roblin et al., 2020), and microplastic cated in an area with mixed deciduous and coniferous forest (Table SI-1).
deposition in Dongguan, China (Cai et al., 2017), Hamburg, Germany The duplicate collectors at Plastic Lake (PCP and PCP2, which are approxi-
(Klein and Fischer, 2019), Central London, England (Wright et al., 2020), mately 20 m apart) and the HYP2 collector have very minimal local anthro-
Gdynia, Poland (Szewc et al., 2021), protected areas in the United States pogenic activity; both PCP and PCP2 are located in a large clearing in the
(Brahney et al., 2020), the French Pyrenees (Allen et al., 2019), Shiraz and middle of a forest and are not easily accessible by vehicles or the general
Mount Derak, Iran (Abbasi and Turner, 2021), Ho Chi Ming City, Vietnam public, and HYP2 is located on the top of a hill in a cleared area. The collec-
(Truong et al., 2021), and Guangzhou, China (Huang et al., 2021). Atmo- tor at Solitaire Lake (SE2P) is located on the top of a hill adjacent to the
spheric deposition rates for microplastics in urbanized areas were reported Limberlost Forest and Wildlife Reserve, which is a private forest reserve
to range from 10 mp/m2/day (Gdynia, Poland) to 771 mp/m2/day (Central that contains 70 km of trails accessible to the public, and contains a few
London, England), and from 12 mp/m2/day (Mount Derak, Iran) to 365 campsites and cottages that can be rented during the summer. The collec-
mp/m2/day (French Pyrenees) in rural and remote regions. tors at Paint Lake (PT1P and PT3P) are located adjacent to the Ontario Min-
There is growing recognition that atmospheric deposition is an impor- istry of the Environment, Conservation and Parks' Dorset Environmental
tant vector for the transportation of microplastics (Dris et al., 2016; Cai Science Centre and may be influenced by the presence of people at the facil-
et al., 2017; Klein and Fischer, 2019; Stanton et al., 2019; Wright et al., ity (< 15 employees, up to 30 staff, students and partners in the summer
2020; Szewc et al., 2021), especially into remote regions far from emission months), parking lots and roads; however, it is still in a remote location.
sources (Allen et al., 2019; Brahney et al., 2020; Roblin et al., 2020). There
is evidence to suggest that microplastics can reach background or remote 2.2. Precipitation collection
regions through long-range atmospheric transport (Allen et al., 2019;
Brahney et al., 2020; Roblin et al., 2020; Allen et al., 2021; Zhang et al., Samples were collected by MECP from each of the precipitation chemis-
2021). Based on air mass trajectories, microplastics observed in a remote try monitoring stations for approximately 13 months commencing at the
mountain catchment in the French Pyrenees were estimated to have trav- end of February 2019 until the middle of March 2020, although the period
elled up to 95 km prior to deposition in the sparsely populated study region differed between stations (see Table 1). Samples were collected at irregular
(Allen et al., 2019). This is further supported by microplastic observations intervals ranging from 3 to 48 days; however, most samples were collected
in snow from remote locations in the Swiss Alps and Arctic, although an- at either weekly or biweekly intervals. Siting criteria and placement of col-
nual deposition rates in these locations were low, i.e., 1.4–66 mp/m2/ lectors followed standard protocols for precipitation chemistry monitoring
year (Bergmann et al., 2019). Similarly, observations from Pic du Midi sug- (WMO, 2018; EMEP, 2014). Bulk precipitation collectors were approxi-
gested free tropospheric microplastics transport across oceans and conti- mately 1.67 m above ground and comprised of a square 0.25 m2 collector
nents (Allen et al., 2021). Nonetheless, the number of observations of with a stainless-steel, Teflon-coated funnel leading into a 50 L polyethylene
microplastic deposition in pristine environments, remote from typical carboy lined with two clear plastic bags. An 80-μm Nitrex nylon mesh filter
point sources of pollution, is limited (e.g., Allen et al., 2019; Brahney was loosely inserted into the stainless-steel funnel to prevent contamination
et al., 2020; Roblin et al., 2020), with even fewer annual-scale studies from insects or other large objects. The wet-only precipitation collector
(Brahney et al., 2020; Roblin et al., 2020). Further, no studies have quanti- (PT3P) was a battery-operated sampler (Applied Earth Science Consul-
fied the abundance and type of microplastics in atmospheric deposition in tants), approximately 1.67 m above ground, comprised of a 0.0925 m2 col-
Canada. lector, which was activated by moisture and automatically opened during

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B. Welsh et al. Science of the Total Environment 835 (2022) 155426

Fig. 1. Location of the four precipitation chemistry monitoring stations (PCP and PCP2, HYP2, SE2P, PT1P and PT3P) in Muskoka-Haliburton, Ontario, Canada during Feb-
ruary 2019 to March 2020. Insets show (a) the location of the four stations in south-central Ontario, (b) location of the two collectors at Paint Lake, and (c) the location of the
two collectors at Plastic Lake.

periods of precipitation. When activated, the precipitation passed through graduated cylinder to determine the volume. Sample bottles were subse-
an 80-μm Nitrex nylon mesh filter and was collected in a carboy lined quently triple rinsed with either filtered B-pure™ or filtered DI water and
with two clear plastic bags. When there was sufficient volume in the precip- passed through the same filter paper as the original sample. The filter pa-
itation collectors, the bags were removed, zip-tied shut, and transported pers were immediately transferred to petri dishes, sealed, and stored for
back to the Dorset Environmental Science Centre. In the laboratory, while subsequent analysis.
wearing nitrile gloves, a corner of the plastic bag containing the precipita-
tion was rinsed with deionised (DI) water and cut with scissors that had 2.4. Particle identification
been placed in 5% hydrochloric acid and rinsed twice with DI water. A
sub-sample of the precipitation was poured into 500 mL PET jars and 1 L The filter papers were visually analyzed using a Leica EZ44 stereomicro-
Nalgene bottles that had been triple rinsed with filtered B-pure™, or filtered scope with an EZ4W0170 camera at 32× magnification for the presence of
DI water and triple rinsed with the precipitation that was just collected, and anthropogenic particles (i.e., synthetic particles but not necessarily plastic)
stored in the refrigerator in the dark until processed. following methods by Welsh et al. (2021). Each particle identified was
photographed and measured using image processing software (ImageJ;
2.3. Particle extraction URL: imagej.nih.gov/ij) and the type and colour of the particle was re-
corded. Particles were primarily identified down to a size of 50 μm but
Samples were vacuum filtered through 1.6 μm Fisherbrand™ G6 glass- smaller particles were also identified where possible. Particle size was esti-
fibre filter papers (4.25 cm diameter) and the filtrate was emptied into a mated by converting the number of pixels measured to a known length in

Table 1
Location (latitude and longitude) and annual precipitation of the four precipitation chemistry monitoring stations in the current study and the lake they are located near as
well as the type of precipitation collector used during the sampling period from February 2019 to March 2020.
Site ID Lake Precipitation Collector Latitude (decimal) Longitude (decimal) Annual Precipitation (mm) Sample Period
(dd/mm/yyyy)

PT1P Paint Bulk 45.224194 −78.933167 1033 01/03/2019–10/03/2020


PT3P Paint Wet-only 45.224417 −78.932861 1033 09/08/2019–13/01/2020
SE2P Solitaire Bulk 45.399111 −79.003194 1075 20/02/2019–25/02/2020
HYP2 Heney Bulk 45.130417 −79.097861 1112 20/02/2019–11/03/2020
PCP Plastic Bulk 45.181667 −78.824611 1081 11/04/2019–04/03/2020
PCP2 Plastic Bulk 45.181611 −78.824639 1081 11/04/2019–04/03/2020

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B. Welsh et al. Science of the Total Environment 835 (2022) 155426

millimetres. All non-fibres were referred to as fragments as they were dom- any remaining material, and triple rinsed again with filtered B-pure™ or
inated by fragments, with few to no films or foams identified. Of the anthro- DI water in between each sample. Finally, 100% cotton laboratory coats
pogenic particles that were identified, 20% were randomly selected and were worn when processing and analyzing the samples.
tested using a hot needle to determine the proportion that were plastic
(i.e., polymers with a petrochemical base). Following Welsh et al. (2021), 2.7. Data analysis
Roblin et al. (2020), and Loppi et al. (2021), a hot needle was pressed
against the edge of the selected particle and if the particle melted, it was Samples were analyzed by event (Table SI-2) and the number of anthro-
classified as plastic; approximately 50% of the particles identified as plastic pogenic particles observed for each sample/event was then pooled by sta-
were further tested for polymer type using Raman spectroscopy. tion over the study period. The concentration of anthropogenic particles
(particles/L) was calculated by dividing the total number of anthropogenic
2.5. Raman spectroscopy particles by the total sample volume (L) for each of the precipitation chem-
istry monitoring stations. Using the calculated concentration (particles/L),
Similar to Welsh et al. (2021) and Roblin et al. (2020), micro-Raman the annual precipitation volume (mm) measured at each station, and the
spectroscopy (WITec, operated by WITec Control) was used to analyze number of days sampled, the daily deposition (particles/m2/day) and the
the particles that were classified as plastic to characterize the type of plastic. annual deposition (particles/m2/year) was estimated for each of the sta-
Fibres were analyzed using 785 nm laser and fragments were analyzed tions (366 days as 2020 was a leap year). The daily microplastic (mp/m2/
using 532 nm laser at 100× objective and adjustable power (ranging day) and annual microplastic (mp/m2/year) deposition rates were calcu-
from 0 mW to approximately 85 mW). To confirm polymer identity, spectra lated by multiplying the anthropogenic particle deposition rate by the per-
were recorded in 0–1800/cm wavelength and analyzed through an open- cent of anthropogenic particles that melted during the hot needle test. A
access library (Open Specy; Fig. SI-1; Cowger et al., 2021). paired t-test was used to determine if there was a significant difference in
the concentration or deposition of anthropogenic particles between PT1P
2.6. Quality control and assurance (bulk collector) and PT3P (wet-only).
Meteorological data (i.e., temperature, relative humidity, precipitation
Precipitation bag blanks (n = 6) were collected in the field by pouring 8 volume, wind speed, and wind direction) were obtained from the nearby
L of filtered DI water into the bag and processing the sample in the same meteorological station at Muskoka Airport, approximately 50 km southwest
manner as precipitation samples; on inspection no microplastics were iden- of Dorset, Ontario. Temperature, precipitation, relative humidity and wind
tified in the precipitation blanks (Table 2). Similar to Welsh et al. (2021), speed were averaged for each sampling period by station (as sampling pe-
procedural open-air blanks, i.e., open petri dishes with filter papers, were riods differed by station). The average wind direction over each of the sam-
routinely deployed to determine potential contamination during the extrac- pling periods was calculated using a vector computation (WebMet; URL:
tion and analysis processes in the laboratory. The average potential www.webmet.com/met_monitoring/622.html). Associations between an-
microplastic contamination was less than one microplastic per observation thropogenic particle concentrations and counts, and meteorological vari-
period. Procedural B-pure™ and DI water blanks were also collected follow- ables, were evaluated using Spearman's Correlation as the data sets were
ing methods by Welsh et al. (2021). The average number of anthropogenic small and not normally distributed.
particles in DI water was 1.44 particles/L and 3.22 particles/L in B-pure™
water, therefore, all B-pure™ and DI water was vacuum filtered prior to 3. Results and discussion
use for rinsing and cleaning (Table 2).
Approximately eight microplastics were identified across all blanks: 3.1. Anthropogenic particle concentrations and composition
three were found in solutions prior to filtration (i.e., all solutions were fil-
tered prior to use); one was found in a microscope blank with an average In total, 2663 anthropogenic particles were observed across all four
exposure of 60.1 h; and four were found in open air blanks with an average sites, ranging from 134 particles at Plastic Lake (PCP2) to 1244 particles
exposure of 6.41 h. The field samples had an average exposure of 0.8 h dur- at Paint Lake (PT1P-bulk collector) (Table 3). The daily anthropogenic par-
ing the filtering process and 0.45 h during microscope analysis. Therefore, ticle deposition rate ranged from 32 particles/m2/day (PCP/PCP2) to 73
samples were not blank corrected as potential contamination was low. Al- particles/m2/day (PT1P) with an average of 57 particles/m2/day across
though some plastic equipment was used during the sample procedure, the four stations (20,704 particles/m2/year).
i.e., nitrile gloves were worn, the mesh was nylon, the sample bottles Paint Lake (bulk collector) had the highest deposition rate as it was
were comprised of polyethylene terephthalate, and the petri dishes were likely influenced by local anthropogenic activity, specifically from the pres-
comprised of polystyrene, potential contamination was limited. The ence of people at the Dorset Environmental Science Centre and nearby res-
nylon, polyethylene terephthalate, polystyrene and nitrile polymers later idential properties, its proximity to roads (both dirt and paved), and the
identified in the field samples were coloured indicating they did not origi- village of Dorset (4 km; Table SI-1). Similar to Paint Lake, the higher depo-
nate from analytical sources. Furthermore, less than 0.51% of particles sition rate observed at Heney Lake, despite being a more remote station,
identified in this study were clear. All equipment was also triple rinsed could be due to its close proximity to the town of Baysville (3 km;
with filtered B-pure™ or DI water prior to use and immediately covered in Table SI-1) as well as its location on a hill resulting in optimal exposure.
aluminium foil when not in use. The Buchner funnel was triple rinsed In contrast, Plastic Lake had the lowest daily particle deposition rate as it
with filtered B-pure™ or DI water, cleaned with a Kimwipe™ to remove is not easily accessible by the general public, and the collectors were located

Table 2
Average concentration of anthropogenic particles and microplastics (mp) in each of the blank samples collected and their coefficient of variation.
QA/QC Sample (liquid) Anthropogenic Concentration (particles/L) * Microplastic Concentration (mp/L) Coefficient of Variation (%)

Unfiltered B-Pure (n = 7) 3.22 0.19 61


Unfiltered Deionised (DI) water (n = 8) 1.44 0.09 90
Bag Blanks (n = 6) 7.75 0.00 65

QA/QC Sample (open-air) Anthropogenic Concentration (particles/h) * Microplastic Concentration (mp/h) Coefficient of Variation (%)
Filtering (n = 39) 1.19 0.07 167
Microscope (n = 6) 0.61 0.04 68

* The average concentration of particles in the liquid and air QA/QC samples have been normalized to MP L−1 and MP hr−1 respectively.

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B. Welsh et al. Science of the Total Environment 835 (2022) 155426

Table 3
The total number of anthropogenic particles, sample volume (L) and concentration of anthropogenic particles (particles/L) observed at the bulk precipitation collectors
(PT1P, SE2P, HYP2, PCP and PCP2) and wet-only collector (PT3P) as well as the annual precipitation (mm), number of days sampled, daily anthropogenic particle deposition
rate (particles/m2/day) and microplastics deposition (mp/m2/day) with the range in daily anthropogenic and microplastic deposition rates in brackets and the relative per-
cent difference (RPD) provided for the duplicate collectors at Plastic Lake.
Site ID Anthropogenic Volume Concentration Rainfall Days Anthropogenic Particle Microplastic
Particles (n) (L) (particles/L) (mm) deposition deposition
(particles/m2/day) (mp/m2/day)

PT1P 1127 44 26 1033 315 73 9


SE2P 360 24 15 1075 349 44 5
HYP2 602 27 22 1112 385 67 8
PCP / 338 31 11 1081 236–269 32 (26–38) 4 (3–5)
PCP2 RPD: 53%
Average 565 28 20 1076 57 7
PT3P 75 4.2 18 1033 78 51 6
(wet-only)

in a forest clearing. Given its remote setting and lack of obvious local observed in Iran and the plastic microfibre deposition rates observed in
sources, it is likely the observed particles were transported over distance Ireland (Table 4). The remaining 88% of anthropogenic particles that did
to the site. not melt during the hot needle test were likely composed of cellulose,
Anthropogenic particle deposition in the Muskoka-Haliburton region i.e., cotton or wool, but may contain toxic additives and dyes making
was primarily dominated by fibres (85%) with fragments comprising the re- them potentially as harmful as synthetic plastic fibres (Remy et al., 2015).
maining 15%. The dominance of fibres or fragments varies between studies
with Klein and Fischer (2019) and Allen et al. (2019) finding fragments to
3.3. Microplastic composition
be dominant, while Cai et al. (2017), Brahney et al. (2020), Wright et al.
(2020), Szewc et al. (2021), Abbasi and Turner (2021) and Huang et al.
Polyamide was the most common polymer identified at 24% followed
(2021) observed a high prevalence of fibres. This observed inconsistency
by polyethylene terephthalate at 19%. The fragments were mainly polyam-
between studies may be driven by analytical differences, e.g., studies that
ide (60%) followed by acrylonitrile butadiene (40%). The fibres were
detect microplastics down to smaller size classes (<50 μm) may be domi-
predominantly polyethylene terephthalate (25%) with polyamide, polypro-
nated by fragments (Henry et al., 2019; Brahney et al., 2020; Roblin
pylene and styrene isoprene copolymers also being identified (13% each).
et al., 2020; Wright et al., 2020; Szewc et al., 2021). Nonetheless, fibres
Polyethylene terephthalate and polyamide are two of the most common
tend to dominate atmospheric deposition in remote or background regions
plastic types used both as thermoplastics and in the textile industry. Poly-
as they can remain suspended in the atmosphere for longer and travel over
amide, also known as nylon, is commonly used in the textile industry but
longer distances to remote regions, depending on their size, wind trajectory
is also used in the automotive industry, such as car tires, as well as in fishing
and speed (Allen et al., 2019; Brahney et al., 2020; Loppi et al., 2021). Fi-
gear (Khosrovyan et al., 2020). Polyethylene terephthalate is widely used in
bres are also easier to detect during visual identification due to their large
the production of plastic bottles, fishing nets and food packaging, but also
size, potentially leading to their overestimation in samples (Klein and
in the production of synthetic fibres, specifically polyester (Stanica-
Fischer, 2019). The smaller portion of fragments identified in the current
Ezeanu and Matei, 2021; Jaffe et al., 2020). The polymer types observed
study is potentially due to the observation that fragments deposit closer
in the Muskoka-Haliburton region are similar to other studies with thermo-
to source (Szewc et al., 2021; Loppi et al., 2021).
plastic polymers being predominant (Table 4).
The average daily anthropogenic particle deposition rate in the
Muskoka-Haliburton region was 57 particles/m2/day with an annual depo-
sition rate of 20,704 particle/m2/year. Reported mean daily anthropogenic 3.4. Wet-only versus bulk deposition
particle deposition rates vary worldwide from 29 particles/m2/day in Ham-
burg, Germany, to 277 particles/m2/day in Dongguan City, China The observed daily bulk deposition of anthropogenic particles at Paint
(Table 4). The anthropogenic particle deposition rates observed in this Lake (PT1P: 73 particles/m2/day) was higher than the wet-only collector
study are generally consistent with other studies despite differences in sam- (PT3P: 51 particles/m2/day), although not statistically different. Nonethe-
pling periods, sample collection, and detection methods, e.g., daily fibre de- less, this suggests that the wet-only collector captured ~70% of the bulk
position rates in rural and remote sites in Ireland and daily particle collector with dry deposition making up approximately 30%, which is con-
deposition rates in both rural and urban sites in Hamburg, Germany sistent with Roblin et al. (2020) who also found that dry deposition made
(Klein and Fischer, 2019; Roblin et al., 2020; Table 4). up 30% of bulk anthropogenic microfibre deposition. Similarly, in Gydnia,
Poland, dry deposition comprised approximately 33% (Szewc et al., 2021).
3.2. Microplastic concentration Conversely, Brahney et al. (2020) found that more than 75% of the plastic
mass deposited in the western US national parks was due to dry deposition.
The hot needle test was conducted on a total of 541 particles (20% of Similarly, Abbasi and Turner (2021) found that wet deposition contributed
observations) of which 89% were fibres and 11% were fragments. Of the 5% and 7% of the total annual microplastic deposition at Shiraz and Mount
particles tested, 12% melted (11% of the fibres and 20% of the fragments Derak, Iran, respectively. Iran and the western United States receive low
that were tested) and were identified as plastic (i.e., synthetic polymers precipitation and thus are dominated by dry deposition, while the sites in
with a petrochemical base). The average deposition of plastic particles ob- Muskoka-Haliburton and Ireland receive >1000 mm of precipitation annu-
served across the four stations was 7 mp/m2/day with an average annual ally. Given the variation in deposition between duplicate bulk collectors
plastic deposition of 2485 mp/m2/year. The average plastic deposition (relative percent difference: 53%), the differences between bulk and wet-
rate was comprised of 5 mp/m2/day for fibres and 2 mp/m2/day for frag- only in this study are speculative, despite being consistent with the litera-
ments. This is lower than the plastic deposition rates observed in remote/ ture.
rural sites in protected areas in the United States (Brahney et al., 2020) At Paint Lake, the percent of fibres and fragments in the bulk deposition
and the French Pyrenees Mountain (Allen et al., 2019), which may be due collector and wet-only collector were nearly identical, with 86% identified
to differences in methodology, or size of detection (i.e., < 50 μm). Nonethe- as fibres and 14% as fragments in the bulk collector compared with 88% fi-
less, the average of the study sites was close to the plastic deposition rates bres and 12% fragments in the wet-only collector.

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B. Welsh et al. Science of the Total Environment 835 (2022) 155426

Table 4
Summary table outlining the study location, site type, number of sites used, monitoring period, type of collectors used, type of microplastics observed, size detection limit
(μm), mean daily anthropogenic particle deposition rate (particles/m2/day; includes both non-plastic synthetic and plastic pieces), the percentage or number of particles
further examined, the percentage of particles identified as plastic, the estimated plastic deposition rate (mp/m2/day), the main polymer types identified and the study source.
ns = not stated; PET = polyethylene terephthalate, PAN = polyacrylonitrile; PE = polyethylene; PP = polypropylene; PA = polyamide; PS = polystyrene; EVAC = eth-
ylene-vinyl acetate; PVC = polyvinyl chloride.
Location Site Type Number Monitoring Type of Observed Size Mean Deposition Examined Percent Plastic Polymer Source
of Sites Period Collector MP Types Detection (m−2 d−1) MPsa Plasticb Deposition
Limit (μm) (m−2 d−1)c

Paris, France Urban 2 12 months Bulk Fibres 50 S1: 110 ± 96 n = 24 29% S1: 31.9 PET, PA Dris et al., 2016
Sub-urban 6 months S2: 53 ± 38 S2: 15.37
Dongguan Urban 3 3 months Bulk Fibres, <200 S1: 277 ± 32 Fibres: 20% Foams, 36 (31–43) PE, PP, Cai et al., 2017
City, films, S2: 208 ± 3 Non-fibres: films, PS
China foams, S3: 198 ± 27 100% fragments:
fragments All: 228 ± 43 84.6%,
fibres: 23%
Nottingham, Urban 4 12 months Bulk Fibres ns SA: 130 n = 1100 2.3% 2 (1–3) ns Stanton et al.,
England SB: 68 2019
SC: 66
SD: 42
Hamburg, Rural 6 3 months Bulk Fibres, 63 DF: 109.4 ± n = 53 77% 212 PE, Klein and
Germany fragments 19.2 (median) EVAC, Fischer, 2019
OF: 76.5 ± 49.8 PET
Urban BO: 70.9 ± 31.6
HU: 51.2 ± 31.6
UC: 56.4 ± 43.6
W: 29.1 ± 14.9
All: 275
(median)d
Pyrenees Remote 1 5 months Bulk Fibres, <25 365 ± 69 n = 254 100% 365 ± 69 PS, PE, Allen et al.,
Mountains, fragments, PP 2019
France films
Central Urban 1 1 month Bulk Fibres, 20 ns Fibres: 5% 100% 771 ± 167 PAN, Wright et al.,
London, fragments, Non-fibres: PET, 2020
England films, 100% PA, PS,
foams, PP, PE
granules
Ireland Rural 4 12 months Wet-only Fibres 50 OP: 63 ± 25 10–15%e 15% 12 (9–15) PET, Roblin et al.,
JC: 70 ± 33 PAN, 2020
Remote VO: 77 ± 52 PE, PP
Bulk MH: 100 ± 52
All: 80f
National Remote 11 Fall 2017 Wet, dry Fibres, ≥5 ns n = 236 ns 132 ± 6 PET, Brahney et al.,
Parks and through the particles PA, PE, 2020
Wilderness summer PP,
Sites, USA 2019 PTFE
Gdynia, Urban 1 286 days Dry, Fibres, 5 ns n = 27 100% 10 ± 8 PET, Szewc et al.,
Poland bulk fragments, PE, PP, 2021
films PVC
Shiraz and Urban 2 1 year Dry, wet Fibres, 20 ns n = 32 100% 63.6 PP, PS, Abbasi and
Mount Remote particles 12.2 PE Turner, 2021
Derak, Iran
Ho Chi Minh Rural 3 1 year Dry, wet Fibres, 300 ns n = 35 97% CC: 256 PP, PE, Truong et al.,
City, Urban fragments D10: 374 PVC 2021
Vietnam Landfill PH: 230
Guangzhou, Urban 1 1 year Bulk Fibres, 12.5 114 ± 40 Fibres: n = Fibres: Fibres: 68 ± PET, Huang et al.,
China fragments, 77 78.7% 28 PAN, 2021
films, Non-fibrous: Non-fibrous: Non-fibrous: PP, PA,
microbeads n = 44 34.1% ns PS
Muskoka- Remote 4 13 months Wet-only Fibres, 20 PT3P: 51 20% (n = 12% 7 (4–9) PA, PET This study
Haliburton, Bulk particles PT1P: 73 541) (n = 65)g
Canada SE2P: 44
HYP2: 67
PCP: 38
PCP2: 26
Average: 57
a
The percentage or number of anthropogenic particles examined using the hot needle test, Raman spectroscopy and/or FT-IR.
b
The percent of anthropogenic particles that were tested and identified as plastic.
c
The estimated plastic deposition rate based on the percent of anthropogenic particles that were tested and identified as plastic and the mean deposition rate.
d
DF: Douglas fir forest; OF: open field; BO: beech/oak forest; W: Wilhelmsburg; UC: university; HU: Henstedt-Ulzburg.
e
Range for the sites but the average was 15% across all sites.
f
OP: Oak park; JC: Johnstown castle; VO: Valentia observatory; MH: Malin Head.
g
Approximately 50% of the particles identified as plastic were further tested for polymer type using Raman spectroscopy.

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B. Welsh et al. Science of the Total Environment 835 (2022) 155426

Fig. 2. Distribution in the length of (a) anthropogenic fibres and fragments combined, (b) anthropogenic fibres only, and (c) anthropogenic fragments only observed in
atmospheric deposition samples from the Muskoka-Haliburton region during February 2019 to March 2020. The black line represents the median, the box represents the
25th and 75th percentile and the whiskers represent 1.5 times the interquartile range.

3.5. Size deposition. Stanton et al. (2019) found that black-gray was the most com-
mon colour (47%) followed by blue (24%) while Huang et al. (2021)
Particle size in the Muskoka-Haliburton region exhibited a right skewed found white to be predominant (40%), followed by blue (29%) and red
distribution with the proportion of fibres and fragments decreasing as size (13%). Other studies that have reported on colour of microplastics ob-
increased (Fig. 2). Of the few particles that were identified down to a size served similar colours, but blue appears to be predominant (Zhang et al.,
range of 20–50 μm, one was a fibre and 69 were fragments. Fibre lengths 2020; Bergmann et al., 2019). Bright eye-catching colours such as red and
ranged from 20 μm to 4980 μm (mean: 770 μm; Table 5), however the ma- blue may be more easily recognized during visual identification and thus
jority of fibres (>55%) had a size less than 600 μm. Fragment size ranged overreported compared to other dull colours (Hidalgo-Ruz et al., 2012;
from 20 μm to 3480 μm (mean: 190 μm) with most fragments (>75%) hav- Dris et al., 2015; Zhang et al., 2020). Conversely, transparent or uncoloured
ing a size less than 200 μm. These results are very similar to Dris et al. microplastics may also be easily overlooked as they are harder to identify
(2016), Cai et al. (2017), Allen et al. (2019) and Wright et al. (2020), (Dris et al., 2015).
who found the majority of fibres to have a size less than 700 μm.
Previous studies in remote or rural regions (e.g., Pyrenees Mountains, 3.7. Meteorological relationships
Ireland, protected area of the USA, and Iran) have very similar fragment
and fibre sizes suggesting that smaller particles may be dominant in remote Only two of the meteorological variables, temperature and wind speed,
or rural sites, distant from urban or industrial centres due to long-range at- were significantly correlated with anthropogenic particle concentration or
mospheric transport (Allen et al., 2019; Brahney et al., 2020; Roblin et al., count (Table SI-4; Table SI-5). Temperature was negatively correlated
2020). Furthermore, the fibre sizes for this study fell within the size range with anthropogenic particle concentration (PT1P rs = −0.71, SE2P rs =
for regional transport (Brahney et al., 2020; Roblin et al., 2020). −0.84, HYP2 rs = −0.53, PCP2 rs = −0.65) and particle count (PT1P
-0.60, PT3P -0.75, SE2P -0.65, HYP2–0.43) and wind speed was positively
3.6. Colour correlated with anthropogenic particle concentration (PT1P 0.32, SE2P
0.57, HYP2 0.48, PCP2 0.62) and particle count (SE2P 0.57, HYP2 0.43).
A variety of different coloured anthropogenic particles were observed in Previous studies have generally found precipitation, wind speed and wind
this study with blue and red being the most common (Table SI-3). Of the direction to be important factors influencing the concentration of particles
fragments identified, 39% were blue and 11% were red, similarly, 53% of (Dris et al., 2016; Allen et al., 2019; Klein and Fischer, 2019; Roblin et al.,
fibres were blue and 32% were red. Green was also a very common colour 2020). Precipitation events, specifically the frequency or occurrence of
for fragments (37%) but was less common for fibres (<1%). The predomi- rainfall events has been reported to be correlated with particle concentra-
nant nature of blue fibres may suggest that the source of anthropogenic par- tions, rather than rainfall volume (Dris et al., 2016; Klein and Fischer,
ticles, especially fibres, is from textiles (clothing) as one study observed that 2019; Roblin et al., 2020). In the current study, anthropogenic particles
blue jeans and denim garments are worn by roughly 50% of the world's were observed in every sample from the wet-only collector but there was
population at any moment in time, with approximately 56,000 microfibres no significant relationship between rainfall volume and particle concentra-
being released per wash of one used pair of jeans (Athey et al., 2020). tions. This suggests that there is an association between particles and rain-
Stanton et al. (2019) and Huang et al. (2021) are the only other studies to fall events (i.e., washout) as the wet-only collector was only open during
report on the colour of microplastics or microfibres in atmospheric periods of precipitation, but that rainfall volume does not influence the
abundance of anthropogenic particles.
Table 5 The deposition of anthropogenic particles, especially in remote regions,
The mean and median anthropogenic particle size (μm) as well as the range (μm) depends on atmospheric transport and connection to source regions (Allen
and coefficient of variation (%) for particles observed in each of the meteorological et al., 2019; Roblin et al., 2020; Wright et al., 2020; Szewc et al., 2021).
stations. The summary values provided for particles fibres and fragments are across Wind direction and speed have been shown to influence microplastic abun-
all observations. dance and there is evidence to suggest that microplastics can travel long dis-
Site ID Anthropogenic Median Mean Range Coefficient of tances from source regions (Allen et al., 2019; Klein and Fischer, 2019;
Particles (n) (μm) (μm) (μm) Variation (%) Wright et al., 2020; Roblin et al., 2020; Szewc et al., 2021). In Ireland, po-
PT1P 1244 450 670 20–4810 101 tential source regions for microfibres were between 40 and 50 km away and
PT3P 75 360 750 20–4980 126 between 12 and 60 km away for particles and fibres in Central London,
SE2P 361 690 940 20–4980 89
England, based on a 5 m/s average wind speed (Roblin et al., 2020;
HYP2 646 440 700 20–4790 107
PCP 204 470 700 20–4440 94 Wright et al., 2020). In the French Pyrenees mountains, it was estimated
PCP2 134 410 700 40–3700 105 that the microplastics had travelled up to 95 km before being deposited,
Particles 2663 440 680 20–4980 105 and in Gydnia, Poland, the microplastics originated from sources greater
Fibres 2268 510 770 20–4980 95 than 100 km away (Allen et al., 2019; Szewc et al., 2021). In the current
Fragments 395 100 190 20–3480 162
study, there was a positive relationship between anthropogenic particles

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B. Welsh et al. Science of the Total Environment 835 (2022) 155426

and wind speed suggesting that faster wind speeds result in greater airshed 26,825 people. In the autumn, when the wind comes from the southeast
source area increasing the proportion of anthropogenic particles that travel and higher particle counts were observed, the likely source regions were Pe-
a greater distance. Preliminary estimates of atmospheric transport in the terborough (population: 85,456; distance: 110 km), Kingston (population:
current study (following Roblin et al., 2020 and Wright et al., 2020) ranged 176,467; distance 225 km), or the Greater Toronto Area (population: 6.4
from 85 to 350 km based on the average and maximum wind speeds (3.1 million; distance 200 km). While local sources may be important, the low-
and 12.5 m/s), a deposition velocity of 0.05 m/s for coarse particles >10 est deposition rates were observed during the summer when the greatest
μm (Roblin et al., 2020), and an atmospheric boundary height of 1400 m number of tourists visited the study area. This suggests that more distant re-
(Mariani et al., 2020). gional sources, were the dominant sources of microplastics in atmospheric
There was no correlation between anthropogenic particles and wind di- deposition.
rection but there was a noticeable change in wind direction with seasons
(Fig. 3). Wind direction primarily came from the west to northwest and 4. Conclusion
southeast over the study period with west winds dominating in the summer
(Fig. 3b) and southeast winds dominating in the autumn (Fig. 3c). In the Anthropogenic particles were observed in all deposition samples col-
winter and spring, the wind came equally from the northwest and southeast lected from four precipitation chemistry monitoring stations in Muskoka-
(Fig. 3a, d). The negative correlation with temperature and the noticeable Haliburton, south-central Ontario, Canada. Daily anthropogenic particle
change in wind direction with season suggests that there is a seasonal effect deposition ranged from 32 to 73 particles/m2/day with an average daily
with changes in wind direction resulting in changes in the source region for deposition of 57 particles/m2/day. Further, average daily microplastic de-
particles. During summer (June to August) average microplastic concentra- position was 7 mp/m2/day (4 to 9 mp/m2/day). Meteorological variables,
tion in rainfall was 7.2 mp/L, average temperature was 19 °C, wind speed i.e., temperature and wind speed, were significantly related to anthropo-
was 2.4 m/s, and wind direction was primarily from the west. In contrast, genic particle concentration and there was a noticeable change in particle
during autumn (September to November) average microplastic concentra- deposition with a shift in wind direction between seasons. This suggests
tion increased to 11.5 mp/L, while temperature dropped to 7.95 °C, that long-range transport from populated regions in the south, such as the
windspeed increased to 2.9 m/s, and wind direction shifted to primarily Greater Toronto Area (> 200 km away), contributed to the observed depo-
south-east. The likely source region in the summer, when lower particle sition of microplastics at the study sites. The atmosphere is an important
counts were observed and the wind came from the west, was the Town of vector for the transport of microplastics, especially to remote or back-
Huntsville (25–35 km; Table SI-1), which has a seasonal population of ground regions distant from typically point sources.

Fig. 3. Wind roses showing wind speed and direction from (a) March 2019 to May 2019, (b) June 2019 to August 2019, (c) September 2019 to November 2019, and
(d) December 2019 to February 2020 for Muskoka-Haliburton, Canada from a nearby meteorological station at the Muskoka Airport.

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B. Welsh et al. Science of the Total Environment 835 (2022) 155426

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