pubs.acs.

org/journal/estlcu Letter

Temporal Archive of Atmospheric Microplastic Deposition

Presented in Ombrotrophic Peat
D. Allen,* S. Allen, G. Le Roux, A. Simonneau, D. Galop, and V. R. Phoenix
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ABSTRACT: Ombrotrophic peatlandfed solely from atmospheric

deposition of nutrients and precipitationprovide unique archives of
atmospheric pollution and have been used to illustrate trends and
changes in atmospheric trace element composition from the recent
Downloaded via 180.249.165.215 on February 7, 2024 at 06:00:37 (UTC).

decadal to the Holocene period. With the acknowledgment of

atmosphere plastic pollution, analysis of ombrotrophic peat presents
an opportunity to characterize the historical atmospheric microplastic
pollution prevalence. Ombrotrophic peatland is often located in
comparatively pristine mountainous and boreal areas, acting as
sentinels of environmental change. In this paired site study, a
Sphagnum ombrotrophic peat record is used for the first time to
identify the trend of atmospheric microplastic pollution. This high
altitude, remote location ombrotrophic peat archive pilot study identifies microplastic presence in the atmospheric pollution record,
increasing from <5(±1) particles/m2/day in the 1960s to 178(±72) particles/m2/day in 2015−2020 in a trend similar to the
European plastic production and waste management. Compared to this catchment’s lake sediment archive, the ombrotrophic peat
core appears to be effective in collecting and representing atmospheric microplastic deposition in this remote catchment, collecting
microplastic particles that are predominantly ≤20 μm. This study suggests that peat records may be a useful tool in assessing the past
quantities and trends of atmospheric microplastic.

■ INTRODUCTION
Microplastic (MP) particles are 5 mm−1 μm “synthetic solid
variation in MP quantities, both relative to the sample location
and over the historic timeline.10,13,15 This suggests that marine
particle[s] or polymer matri[cies]”.1,2 Since the creation of and freshwater MP deposition is not consistent and may be
Bakelite (1907), commercialization of PVC (1930s), and use influenced by availability, location, and environmental
of nylon fibers (1938)1,3,4 plastic creation, waste and conditions.
mismanagement has increased relentlessly. In 2019, 368 Sea ice cores from both the Arctic and Antarctica illustrate
million metric tonnes (Mt) was produced globally,5 with an historical MP to depths greater than 1 m.16,17 Sea ice collects
estimated 32% of the municipal waste mismanaged and MP from both the marine and atmospheric environments,
potentially lost to the environment (in 2016).6 This has often illustrating high uptake of MP from the surrounding
resulted in a predicted 3-fold increase in plastic waste entering seawater.16−19 Due to the remote location of some ice sample
the environment by 2040 (∼80 Mt, business as usual sites, it is suggested that atmospheric transport is a significant
scenario).7,8 This increase in plastic waste lost to the MP vector.20
environment over past decades has been quantified in Alternatively, assessment of the long-term plankton trawl
environmental archives of sediment (both freshwater lake records in the North Atlantic and adjacent seas illustrates that
and marine sediments), soil, and ice but has not previously since the 1950s there has been a consistently increasing trend
been reported in peat.9 in marine plastic litter. The most significant increase was seen
Marine sediments are the most commonly analyzed archives, in the 1990s, with the greatest marine plastic litter recorded in
with studies evidencing historical marine MP deposition in plankton nets occurring between 2000 and 2009.21 These data
Arctic, Baltic, Mediterranean, North seas, Atlantic and Pacific
ocean sediments.10 Mangrove sediments are areas of high
marine deposition and have illustrated an exponential increase Received: August 28, 2021
in MP deposition since the 1950s.11,12 Within urban lakes, Revised: October 18, 2021
similar exponential trends have been found, showing the most Accepted: October 20, 2021
significant increase in plastic deposition to occur in the most Published: October 25, 2021
recent decades (1980−present).13,14 Urban freshwater and
marine sediment archives illustrate a notable amount of

© 2021 American Chemical Society https://doi.org/10.1021/acs.estlett.1c00697

954 Environ. Sci. Technol. Lett. 2021, 8, 954−960
Environmental Science & Technology Letters pubs.acs.org/journal/estlcu Letter

Figure 1. Microplastic content represented in the peat (a) and lake (b) cores collected from the Arbu Catchment. The MP quantities are
represented as deposition rates1 for time periods relevant to collected subsamples of the cores and in units comparable to previously published
environmental MP rates. All nonfibrous MP are classified as fragments. While peat samples were available to create 5-year time step analysis back to
2000 and 20-year time steps back to 1940, lake samples were constrained by sample volume availability for samples dated 1940−1970, and
therefore, only the 1970−2015 samples were analyzed (alongside pre-1900 dates field process blanks). Error bars represent the standard deviation
for the sample set. It is noted that the peat core results are actually net accumulation rates of MP illustrating the MP deposited and potentially lost
through re-entrainment, but for the purposes of this paper, they are described as deposition.

sets all illustrate the increasing prevalence of MP in the previously been used to quantitatively characterize historical
environment (sea, sediment, soil), and it is logical to MP trends, while lake archives are well established in
hypothesize a similar occurrence in an atmospheric archive. identification of past trends in catchment MP pollution. To
Ombrotrophic peat has been used to illustrate changes in “logic check” the MP results found in the peat core, the results
atmospheric composition and deposition of anthropogenic were compared with MP quantified in the Lake Arbu core (N
pollutants over the past centuries.22,23 Ombrotrophic peat = 1). The lake collects runoff and erosion from the total
collects and retains atmospheric dust, particles, and pollutants, catchment as well as direct atmospheric MP deposition and is
providing dated historical records of past humans influ- therefore more representative of the total catchment
ence,9,24,25 such as mining, urbanization, and industrial atmospheric MP deposition in contrast to the peat, which
activities (e.g., lead, fly ash, antimony, copper26−29), illustrating only represents deposition specifically onto the peat surface.
trends over the industrialization era.
The lake core was collected during a previous campaign
Disaggregating purely atmospheric pollutants from other
(2014) using a UWITEC corer from a floating platform
transport pathways (e.g., runoff, erosion, seawater, other
(sub)surface influences) in sea ice, soil, or sediment records (subsampled core analysis following the same MP methods as
is difficult, and thus, defining solely the atmospheric influence implemented for peat analysis, detailed in the SI). Archive
is difficult. Ombrotrophic Sphagnum peatlands are unique as samples were dated using 210Pb and 14C radiocarbon dating
they receive pollutants, nutrients, and water solely from the techniques,30−32 and age depth models are created to date all
atmosphere. Thus, despite inconsistent growth rates, bio- subsamples (CLAM, CRS33,34) (SI).
turbation from plant roots, and potentially incomplete μRaman analysis was undertaken using a Horiba Scientific
deposition retention,9 peat may provide a unique insight into Xplora Plus, using a 785 nm laser 50−3200 cm−1, 1.5 cm−1
the history of atmospheric MP pollution. resolution, 0.5 μm confocal imaging accuracy with an X−Y

■
motorized stage.35,36 Approximately 30% of the filter surface
MATERIALS AND METHODS was analyzed, collecting a minimum of 10 acquisitions of 15 s
using a maximum of 25% power (filter) (1200 grating mm−1,
The pilot study field location is a small remote catchment in
50 μm slit, modified as necessary to achieve effective spectra
the central Pyrenees. The Arbu catchment is 1.6 km2
clarity). LOD/LOQ for this analysis was set to 5 μm. MP size
(42°48′18″ N, 1°26′15″ E), at an elevation of 1940 m
a.m.s.l (Figure S1). The site has low local hiking traffic, which and shape were characterized using Nile red fluorescence
does not traverse near the peatland, but it is acknowledged that microscopy37−39 and FIJI software.
local hikers may be a minor contributing factor to plastic in the For both peat and lake samples, field blanks (negative
catchment. The catchment has a lake at its base and an controls) were created by randomly selecting subsamples from
ombrotrophic peat area on the western elevation. A Wardenaar the bottom of the cores (dated pre-1900). Blank samples were
peat core (N = 1) was collected from the peat site during a processed following the (H2O2 organic digestion and ZnCl2
field campaign in 2017, subsampled (∼1 cm deep sections) in density separation, SI) peat/lake sample preparation protocol
the laboratory, and analyzed using μRaman spectroscopy prior to filtration onto 0.2 μm pore, 25 mm diameter
following standard methods (detailed methods description in aluminum oxide filters. All sample preparation and analysis
the SI). Ombrotrophic peat (hereafter “peat”) has not were completed in a controlled laboratory following rigorous
955 https://doi.org/10.1021/acs.estlett.1c00697
Environ. Sci. Technol. Lett. 2021, 8, 954−960
Environmental Science & Technology Letters pubs.acs.org/journal/estlcu Letter

Figure 2. Microplastic particle size distribution for peat and lake samples (Figure 2a, b). The black line represents the mean particle size within the
overall sample, and the gray shading is representative of the first−third quartile range of particle sizes. The particle size distribution results are
disaggregated into fibers and fragments in Figures S3 and S5. The insets illustrate the proportion of smaller particles (MPs <20 μm) throughout the
samples relative to the sample age dating. Polymer composition of samples, relative to the age depth are in Figure 2c and d and Figure S4).

protocols to mitigate contamination. Peat and lake samples MP findings (Tables S1 and S2). This declines to a deposition
were all blank corrected (SI). rate of less than 600 MP/m2/year prior to 2005 (equivalent to

■ RESULTS AND DISCUSSION

Microplastic Particle Counts. The greatest quantity of
≤900 MP/kg), with lower MP found in samples dated pre-
1990s (<140 MP/m2/year, <300 MP/kg). The proportion of
fiber MP was relatively consistent throughout the lake samples
MP was found in the top section of the single peat core, (8%−24%). The greater comparative peat surface fiber counts
presenting a deposition rate of 178 (±79) MP/m2/day (Figure may be a result of effective vegetation capture of fibers (and
1a). The quantity of MP decreased with depth, with negligible particles) by peat and the potential for fibers to move more
MP found in the 1940−1960 dated samples (1−2 MP/sample, slowly or get detained in the catchment vegetation and soils
≤1 MP/m2/day). The change in the rate of MP deposition was prior to runoff conveyance to the lake. The overall difference
greatest in the top sample (2015−2020) and 1980−2000 between peat and lake MP counts may also be due to the
sample (deposition rate increase of >70 MP/m2/day). The evolution of vegetation cover (1990−2020 increased shrub and
proportion of MP fibers was greatest in the top peat sample heathland, increasing the filtration role by vegetation). MPs
(>30% of the total MPs), decreasing to ≤20% in the 1960− may also float on the lake surface, discharging downstream,
1980 samples. The decrease may be due directly to resulting in only a proportion of catchment MP deposited in
atmospheric concentration and deposition or in situ particle lake sediment.
degradation (UV, chemical or mechanical forces) of particles Microplastic Particle Size Distribution. Peat MP size
caught in the peat (sub)surface, acknowledging the uncertainty distribution shows greater than 50% of particles identified as
due to taphonomic processes.9 ≤30 μm (Figure 2). This concurs with the atmospheric
Lake samples from the single lake core illustrated a similar deposition MP size distribution from direct atmospheric
decline in MP numbers with depth. The uppermost samples sampling for the adjacent catchment in the Pyrenees36
(2010−2015) present a deposition rate of 7.2 (±1.6) MP/m2/ (>50% MP particles <20 μm). The overall prevalence of
day (2620 (±577) MP/m2/year), equivalent to 2800 (±616) ≤30 μm MP suggests atmospheric deposition to primarily be
MP/kg (dry weight). These values are comparable to MP smaller MP particles, reflective of the remote location. The
found in Arctic (≤6695 MP/kg),40 Tibetan Plateau (8−563 proportion of MP less than 20 μm shows a slightly increasing
MP/m2),41 and remote Swiss mountain lake sediments (100− trend since 1980 (SI), potentially due to an increase in
1300 MP/m2)42 and lower than published urban lake sediment creation/emission of smaller MP directly into the atmosphere
956 https://doi.org/10.1021/acs.estlett.1c00697
Environ. Sci. Technol. Lett. 2021, 8, 954−960
Environmental Science & Technology Letters pubs.acs.org/journal/estlcu Letter

Figure 3. Comparison of peat and lake archive results with Europe and management trends. The global plastic production trend has been provided
for supporting context to the European production trend. The EU and global trend data are compiled from published plastic statistics.7,47 Global
production is indicated in gray, while European (EU) production is indicated in orange. EU collected waste is identified in brown, discarded
(landfill) waste in green, incinerated waste in blue, and recycled plastic waste in yellow. The peat and lake archive results are presented as black
dotted lines (average MP/m2/day) with the first−third quartile range shaded in light gray.

from human activities (e.g., laundry (dryer) emissions, commercialization of low cost plastic personal devices and
ineffective incineration, agricultural practices43−45) or/and an homecare products.46
increase in macroplastic waste loss to the environment that has The lake samples follow a similar decreasing trend in
degraded over time (in situ or in transport) resulting in individual polymer prevalence and sample complexity with
increased MP and an increase in atmospheric transport. depth to that found in the peat archive. PS and PP indicate a
MP fragments (nonfibrous particles) follow the overall localized increase in prevalence during 1990−1995, while PE
sample size distribution (Figure 2, Figures S3 and S5) with and PET show a consistently declining trend with depth. In
pre-1980 samples showing a greater proportion of larger general, the peat and lake archives illustrate an increasing
fragments (>20 μm) than recent (top) samples (MP fragments quantity of all plastic polymer types over time and a complexity
less than 20 μm decline from 50% to 35% during 2020−1980) in their composition.
(SI). Microplastic fibers are generally between 20 and 200 μm Past Trends of Atmospheric MP Deposition. Overall,
in length with a predominant fiber length of 100−150 μm the findings suggest peat to be an effective atmospheric MP
(Figure S3). deposition collector, illustrating a MP deposition rate (MP/
The lake core MP samples present a similar particle size m2/day) at a moderate interval (∼5 to 10 year time steps).
distribution trend to peat. The proportion of less than 20 μm Similar to lake archives, peat representation will fluctuate in
MPs shows little variation prior to 1995, an increase in smaller resolution according to the availability of precipitation, growth
(<20 μm) particles post 1995, but a decrease in the top sample nutrients, and climatic and environmental conditions. Peat
(2010−2015). This water−sediment interface difference may growth and atmospheric MP deposition retention appears to
be a pre- and postburial difference. It may alternatively be due be great enough to support atmospheric archive analysis of
to a decrease in catchment influx of the smaller MP particles in recent historic MP. Unlike passive or active field atmospheric
surface runoff during this period (influenced by catchment sampling (e.g., collection via deposition collectors or pumped
vegetation change, increased shrub and heathland potentially filters), it is acknowledged that an unknown proportion of
detaining surface runoff MP), precipitation (e.g., fewer, less atmospheric deposition may be resuspended, and taphonomic
intense or shorter duration runoff events), and other processes may influence the accumulation record,9 resulting in
meteorological conditions (e.g., lower average wind speed or an under/overestimation of atmospheric deposition. This
planetary boundary layer). study confirms the effectiveness of ombrotrophic peat as a
Plastic Types. Polypropylene (PP), polyethylene tereph- MP atmospheric deposition archive providing a unique record
thalate (PET), polyethylene (PE), polystyrene (PS), and of past atmospheric MP deposition.
polyvinyl chloride(PVC) are the most abundant in the peat Acknowledging this single site pilot study, a comparative EU
core samples (Figure 3), generally following the European plastic trend assessment is used to tentatively expand on MP
demand relative to polymer type.7 PE, PET, PP, and PVC trends. Lake MP show a rapid MP increase post 2000,
show a general decreasing trend with depth, illustrating a following plastic production trends. While MP generally
relatively consistent increase in the atmospheric deposition of increased from 1960 onward, the late 1990s MP lake
these polymers over time consistent with the increasing deposition dip appears to coincide with plateauing of the
production and use of plastic. The sample MPs are composed discarded plastic waste stream (rather than sediment
of a complex mixture of polymer types, with ethylene vinyl accumulation rate) and commencement of increased recycling
acetate (EVA), polycarbonate (PC), acrylonitrile butadiene and incineration/energy recovery waste processes.
styrene (ABS), and other plastics occurring in the post 1980 Peat MP results show a similar increasing MP trend and a
samples. This concurs with the post 1980s development and MP deposition dip between 2005 and 2010 coinciding with the
commercialization of high performance plastics and the recession (2007−2009) (less disposable income potentially
957 https://doi.org/10.1021/acs.estlett.1c00697
Environ. Sci. Technol. Lett. 2021, 8, 954−960
Environmental Science & Technology Letters

■
pubs.acs.org/journal/estlcu Letter

resulting in lower single use plastic waste). This dip also AUTHOR INFORMATION
coincides with the increase in EU collected waste plastic Corresponding Author
(∼3%) compared to the generally consistent increase in waste
D. Allen − Department of Civil and Environmental
plastic collection and the drop in EU production. The MP dip
Engineering, University of Strathclyde, Glasgow G11XJ,
in the 2005−2010 period also occurs alongside the start of the Scotland; Laboratoire écologie fonctionnelle et environnement,
decrease in landfill (discarded) plastic waste in Europe Université de Toulouse, Toulouse 31062, France;
(occurring from ∼2006 onward to the present). Interestingly, orcid.org/0000-0002-4038-9394; Email: deonie.allen@
this dip is not seen in the lake archive, and this may be due to strath.ac.uk
the lake MP being predominantly resultant from atmospheric
deposition on the catchment which is then transported to the Authors
lake via surface runoff over vegetation and soil. The lag S. Allen − Laboratoire écologie fonctionnelle et environnement,
between atmospheric deposition and lake MP settling may Université de Toulouse, Toulouse 31062, France; School of
result in a decrease in lake archive sensitivity (relative to time Geography, Earth and Environmental Sciences, University of
resolution), resulting in a smoother trend in the lake sediment Birmingham, Birmingham B15 2TT, England; Department
archive (at this location and with this lake sediment deposition of Earth and Environmental Sciences, Dalhousie University,
rate) compared to the atmospheric peat archive. The Halifax, NS B3H 4R2, Canada
comparable peat MP, EU production, and waste trends G. Le Roux − Laboratoire écologie fonctionnelle et
tentatively suggest atmospheric MP concentration responds environnement, Université de Toulouse, Toulouse 31062,
relatively quickly to changes in atmospheric MP emissions France; orcid.org/0000-0002-1579-0178
(primary and secondary) even where there is no significant A. Simonneau − ISTO, Université d’Orléans, 45100 Orléans,
local source (e.g., remote mountain sites). These comparisons France
of MP and EU plastic trends maybe an overinterpretation and D. Galop − GEODE, Université Toulouse Jean Jaurès,
require further investigation, but if atmospheric MP concen- Toulouse 31062, France; LabEx DRIIHM, OHM Pyrénées
trations are found to respond quickly to decreased MP Haut Vicdessos, Paris 75000, France
emissions, then management methods to help decrease V. R. Phoenix − Department of Civil and Environmental
atmospheric MP emissions could have a relatively immediate Engineering, University of Strathclyde, Glasgow G11XJ,
beneficial impact on MP pollution of the atmosphere and Scotland
environment. Complete contact information is available at:
Both the pilot study and single core archive records of MP https://pubs.acs.org/10.1021/acs.estlett.1c00697
show some correspondence with European waste management,
specifically the landfill/discarded plastic waste management Notes
that was predominant in the early plastic pollution era (pre- The authors declare no competing financial interest.

■
1995), the overall economic health (recession periods), and
the quantity of plastic produced (especially in the EU), with a
ACKNOWLEDGMENTS
stronger comparison seen in the peat samples than the lake
samples. While this is a pilot study, early results suggest MP The authors acknowledge the Leverhulme Trust through
peat monitoring may be sensitive enough to indicate Grant ECF-2019-306 and Carnegie Trust (RIG009318), IGI
atmospheric MP response to policy initiatives or global funding through the University of Birmingham, OFI fellow-
increases in certain polymer use. Further ombrotrophic peat ship, Belmont-Forum MSC- ANR-15-MASC-0001-P3 and
archive analysis is needed for a variety of locations (urban to ANR JCJC TRAM (ANR-15-CE01-0008), Observatoire
remote) to consolidate these results and provide a spatially Hommes-Milieux Pyrénées Haut VicdessosLabEx DRIIHM
comprehensive history of atmospheric MP composition and ANR-11-LABX0010, and INTERREG VA Spain-France-
deposition. Andorra (POCTEFA 2014-2020) (REPLIM project, Ref.

■
EFA056/15). The research leading to these results has also
received support through the People Programme (Marie Curie
ASSOCIATED CONTENT Actions) of the European Union’s Seventh Framework
*
sı Supporting Information Programme (FP7/2007-2013) under REA Grant Agreement
The Supporting Information is available free of charge at No. PCOFUND-GA-2013-609102, the PRESTIGE pro-
https://pubs.acs.org/doi/10.1021/acs.estlett.1c00697. gramme coordinated by Campus France. The authors
acknowledge that this work was carried out in the CMAC
Figure S1: contextualized site map, detailed method- National Facility, housed within the University of Strathclyde’s
ology, commentary on peat, and a comparative sediment Technology and Innovation Centre, who are funded with a
MP particle count with current published research. UKRPIF (UK Research Partnership Institute Fund) capital
Tables (S1 and S2) of published sediment MP particle award, SFC ref H13054, from the Higher Education Funding
counts per mass of sediment and per m2 of sampled Council for England (HEFCE).

■
surface area. Figure S2: age date model information for
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