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Science of the Total Environment xxx (xxxx) xxx

Contents lists available at ScienceDirect

Science of the Total Environment


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

The distribution and characterisation of microplastics in air, surface water


and sediment within a major river system
Imogen E. Napper a, c, *, Anju Baroth b, Aaron C. Barrett c, Sunanda Bhola b, Gawsia
W. Chowdhury d, e, Bede F.R. Davies f, Emily M. Duncan g, Sumit Kumar b, Sarah E. Nelms g,
Md. Nazmul Hasan Niloy d, e, Bushra Nishat h, Taylor Maddalene i, j, Natalie Smith a, l, Richard
C. Thompson a, c, Heather Koldewey g, k
a
International Marine Litter Research Unit, University of Plymouth, UK
b
Wildlife Institute of India, Dehradun, Uttarakhand, India
c
School of Biological and Marine Sciences, University of Plymouth, UK
d
Department of Zoology, University of Dhaka, Dhaka 1000, Bangladesh
e
WildTeam, 69/1 New Circular Road, Malibagh, Dhaka 1217, Bangladesh
f
Nantes Université, Institut des Substances et Organismes de la Mer, ISOMer, UR2160, Nantes, F-44000, France
g
Centre for Ecology and Conservation, University of Exeter, Penryn Campus, UK
h
Isabella Foundation, Dhaka, Bangladesh
i
National Geographic Society, Washington, DC, USA
j
University of Georgia, Athens, GA, USA
k
Zoological Society of London, London, UK
l
Plymouth Marine Laboratory, UK

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

• Microplastics were investigated in


water, sediment, and air in a major river
system for the first time.
• For water and sediment there was an
increase of microplastics from source to
sea.
• Higher population densities correlated
with increased microplastic abundance
in Air and Water.
• It is predicted a large proportion of
denser microplastics settle in sediment.
• Rayon was the dominant polymer and
blue fibres were the dominant colour
and shape.

* Corresponding author at: International Marine Litter Research Unit, University of Plymouth, UK.
E-mail address: [email protected] (I.E. Napper).

https://doi.org/10.1016/j.scitotenv.2023.166640
Received 23 May 2023; Received in revised form 17 August 2023; Accepted 26 August 2023
Available online 28 August 2023
0048-9697/© 2023 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).

Please cite this article as: Imogen E. Napper et al., Science of the Total Environment, https://doi.org/10.1016/j.scitotenv.2023.166640
I.E. Napper et al. Science of the Total Environment xxx (xxxx) xxx

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

Editor: Yolanda Pico, Ph.D. Rivers are key pathways for the transfer of microplastics (MP) to marine environments. However, there are
considerable uncertainties about the amount of microplastics transported by rivers to the ocean; this results in
Keywords: inaccuracies in our understanding of microplastic quantity and transport by freshwater systems. Additionally, it
Microplastic has been suggested that rivers may represent long-term sinks, with microplastics accumulating in sediment due
Fibres
to their high density or other biological, chemical, and physical factors. The atmosphere is also an important
Freshwater
pathway by which airborne microplastics may enter aquatic habitats. Here, we compare for first time micro­
Water
Air plastics type and concentration in these key environmental mediums (air, water and sediment) along a major
Sediment river (Ganges), from sea to source to understand 1) the abundance, 2) the spatial distribution, and 3) charac­
teristics. Mean microplastic abundance settling from the atmosphere was 41.12 MP m2 day− 1; while concen­
trations in sediment were 57.00 MP kg− 1 and in water were 0.05 MP L− 1. Across all sites and environmental
mediums, rayon (synthetically altered cellulose) was the dominant polymer (54–82 %), followed by acrylic
(6–23 %) and polyester (9–17 %). Fibres were the dominant shape (95–99 %) and blue was the most common
colour (48–79 %). Across water and sediment environmental mediums, the number of microplastics per sample
increased from the source of the Ganges to the sea. Additionally, higher population densities correlated with
increased microplastic abundance for air and water samples. We suggest that clothing is likely to be the
prominent source of microplastics to the river system, influenced by atmospheric deposition, wastewater and
direct input (e.g. handwashing of clothes in the Ganges), especially in high density population areas. However,
we suggest that subsequent microplastic release to the marine environment is strongly influenced by polymer
type and shape, with a large proportion of denser microplastics settling in sediment prior to the river discharging
to the ocean.

1. Introduction different environmental compartments of an ecosystem (surface water,


water column, sediment and sea floor sediments). Additionally, there
Plastic debris is persistent and pervasive throughout the environ­ are discrepancies between the amount of microplastics supposedly
ment and has been reported from the deepest parts of the ocean to the exported by rivers to the ocean and the microplastic stocks accumulating
tops of the highest and most remote mountains (Allen et al., 2019; at the ocean surface has triggered the idea of a “missing” ocean plastic
Napper et al., 2020; Woodall et al., 2014). Plastics in the microplastic sink (Cózar et al., 2014; Thompson et al., 2004).
size range (<5 mm) are an environmental pollutant of particular public Recent research indicates the presence of large amounts of micro­
and scientific concern (Paul et al., 2020; Thompson et al., 2004) and plastics in the surface water of rivers (Li et al., 2020a; Napper et al.,
have been widely reported in the environment; from soil to aquatic 2021). Previous research by Napper et al. (2021) estimated that the
systems (e.g. ocean, rivers, shorelines and lakes) (Auta et al., 2017; Ganges river system, with the combined flows of the Brahmaputra and
Biginagwa et al., 2016; Horton et al., 2017b; Napper et al., 2021; Prata Meghna rivers (GBM), could release up to 1–3 billion (109) microplastics
et al., 2020; Thompson et al., 2004; Woodall et al., 2014). into the Bay of Bengal (north-eastern portion of the Indian Ocean) every
The marine environment is believed to be a major sink for micro­ day. Additionally, Miller et al. (2017) estimated that the Hudson River’s
plastics, with an estimated 1.5 Mt. entering the ocean annually (Boucher watershed drainage area could contribute an average 300 million
and Friot, 2017) and the majority being transported from land (Siegfried anthropogenic microplastic fibres into the Atlantic Ocean per day. Such
et al., 2017). Riverine transport is a key pathway that transfers micro­ research provides the first step in understanding how major rivers may
plastics from land to marine environments (Eerkes-Medrano et al., 2015; contribute to oceanic microplastic loads. However, research suggests
Napper et al., 2021; Schmidt et al., 2017; Seo and Park, 2020; Wagner that rivers do not solely function as pure conduits for plastics travelling
et al., 2014; Weideman et al., 2020). Due to their small size, micro­ to the ocean, but also represent long-term sinks, with some microplastics
plastics have the potential to be ingested by a wide range of marine being buried in streambeds and floodplain sediments (Bläsing and
species; from microscopic zooplankton to large vertebrate predators Amelung, 2018; Ding and Mao, 2019; Peng et al., 2018; Rodrigues et al.,
(Aytan et al., 2022; Botterell et al., 2019; Moore et al., 2022; Nelms 2018).
et al., 2019). They can also cause negative impacts to marine species Sediment has been described as the ‘final settling tank’ for micro­
biological processes such as decreased mobility, reduced feeding and plastics (Nizzetto et al., 2016). Microplastics can accumulate in sedi­
growth, and reduced body condition (Critchell and Hoogenboom, 2018; ment due to their high density or other biological, chemical, and
de Sá et al., 2015; Lo and Chan, 2018; Messinetti et al., 2018). Subse­ physical factors (Li et al., 2020b). For example, biofouling (Lobelle and
quently, the worsening of microplastic pollution in the ocean and rivers Cunliffe, 2011), mineral adsorption (Corcoran et al., 2015), incorpora­
has received substantial attention across various fields (Horton et al., tion of microplastics into faecal pellets (Cole et al., 2016) and marine
2017b; Jambeck et al., 2015; Lebreton et al., 2017; Napper et al., 2021; aggregates (Long et al., 2015) can decrease the buoyancy of plastics,
Thompson et al., 2004). facilitating their movement into bottom sediment (Rodrigues et al.,
Freshwater systems are estimated to release up to 265,000 Mt. of 2018). Microplastics concentrations have been observed in the Ciwa­
plastic into coastal environments annually (Lebreton et al., 2017; Mai lengke River (Majalaya, Indonesia) with an average abundance of 30.3
et al., 2020; Schmidt et al., 2017; Wagner et al., 2014). Sources may ± 15.9 microplastics/kg, whereas higher concentrations have been
include leakage from wastewater treatment plants (WWTPs) (Kay et al., found in river sediments within Shanghai (China) urban districts at 802
2018), atmospheric pollution (Allen et al., 2019; De Falco et al., 2020; ± 594 microplastics/kg (Peng et al., 2018). Additionally, microplastics
Dris et al., 2015), road runoff (Horton et al., 2017a; Knight et al., 2020), in the sediment may be released by disturbance at the water-sediment
industry (Lechner and Ramler, 2015), and degradation of larger items of interface (Ji et al., 2021), allowing them to migrate upward into the
mismanaged and openly dumped plastic waste (Barnes et al., 2009; main body of water.
Schmidt et al., 2017; Schwarz et al., 2019). However, despite scientific The atmosphere is another important pathway for plastics to enter
interest in the sources and distribution of environmental microplastic, different environments by which suspended particulates can be trans­
which represents one of the most studied fields globally (Aretoulaki ported regionally and even on a global scale (Allen et al., 2019;
et al., 2020), there are gaps regarding microplastic fluxes within the Camarero et al., 2017; Dris et al., 2016). Subsequently, airborne

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microplastics may enter freshwater via deposition from the atmosphere plastic pollution from major Asian rivers (Blettler et al., 2018; Chowd­
(Napper et al., 2023). Atmospheric deposition rates for microplastics hury et al., 2021). It was hypothesized that the majority of microplastics
(predominately fibres) have been studied in urban areas which range would be microfibres, and concentrations would increase from source to
from 10 m2 day− 1 (Gdynia, Poland; Szewc et al., 2021) to 771 m2 day− 1 sea due to the movement and accumulation of freshwater for both water
(Central London, England; Wright et al., 2020) and for remote regions and sediment samples but would be correlated with population density
from 12 m2 day− 1 (Mount Derak, Iran; Abbasi and Turner, 2021) to 365 for atmospheric samples.
m2 day− 1 (French Pyrenees; Allen et al., 2019).
Although there is good understanding of the accumulation of 2. Methodology
microplastics in aquatic environments, there is less clarity on the
different environmental pathways, transportation, and underlying cau­ 2.1. Study area
ses, which presents a major barrier to implementing solutions (Galloway
et al., 2020; Napper et al., 2020). Due to this, microplastics were The Ganges River is a major river system and has a transboundary
examined within the medium of air (via atmospheric deposition), water, river basin which is distributed between five countries; India, China,
and sediment along a mainstream river (the Ganges, flowing through Nepal, Bhutan and Bangladesh. The river originates from the Gangotri
India and Bangladesh), from sea to source. Within the different envi­ glacier in the Himalayas (India) at an elevation of nearly 7010 m and
ronmental mediums, this study aims to understand 1) the abundance, 2) traverses a length of about 2575 km before it flows south-east, trans­
the spatial distribution, and 3) characteristics of microplastic from forming into distributaries and ultimately flowing into the Bay of Bengal
source to sea within a major river system. (Bangladesh) (Singh and Singh, 2019; Whitehead, 2018). Throughout
The River Ganges was selected as a case study to better understand the Ganges River, both large and small tributaries join, such as the
and document the characteristics and flow of plastics in a major river Brahmaputra River, which joins in Bangladesh as the Padma and further
system. A large population live by the river and the characteristics of the down the combined discharge joins the Meghna river at Chandpur
cities and communities along the river is diverse. Additionally, the (Pangare et al., 2021). The total annual Ganga-Brahmaputra-Meghna
Ganges has been identified to have a substantial amount of plastic (GBM) river basin inflow into Bangladesh from India is 1110 km3
pollution (Napper et al., 2021; Nelms et al., 2020; Youngblood et al., (FAO, 2012). >138,700 m3/s of water flows into the Bay of Bengal
2022). Furthermore, there are limited studies and empirical field data on during flooding (especially in the monsoon season) through a single

Fig. 1. Sampling locations along the Ganges River.

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outlet of the GBM river in Bangladesh. This is the largest in the world for polypropylene bag for transportation The sample bags containing the
a single outlet to the sea and exceeds even that of the Amazon discharge sediment were then not opened again until in a dedicated laboratory for
by about 1.5 times (Parua, 2001). During pre-monsoon (March to May) microplastics analysis.
water levels are often at the lowest, with discharge in all the rivers Within the laboratory, microplastics were separated from the sedi­
starting to rise due to glacier melt by end of May. The Ganges river flows ment using the methodology and custom-made sediment-Microplastic
only notably increase after the monsoon starts (Pangare et al., 2021). Isolation (SMI) unit as detailed in Coppock et al. (2017); including
The river is also of high religious, cultural, socio-economic and cleaning, purging and priming the SMI. On each occasion, a dry (50 g)
ecological significance and sustains over 655 million people, many of sample, clean magnetic stir bar and 700 mL of ZnCl2 were added to the
whom live below the poverty line (Rahman et al., 2020; Sharma et al., purged SMI unit. ZnCl2 (1.5 g cm− 3) was chosen as the floatation me­
2010; Singh and Singh, 2019). dium as has been deemed to have the best efficiency (Coppock et al.,
2017). A nylon mesh (pore size 30 μm) was used and split over multiple
2.2. Site selection meshes (if high quantities of organic material present) to capture any
separated microplastics.
Within this study, 10 sites in India and Bangladesh were selected
along the length of the mainstream river to represent the whole length of 2.3.3. Atmospheric deposition sampling
the Ganges (Fig. 1). Three sites were located in Bangladesh: Bhola (L1), Microplastics within the air were sampled by atmospheric deposi­
Chandpur (L2), Rajbari (L3). India included the other seven sampling tion; microplastics that had been transported by the atmospheric envi­
sites: Sahibganj (L4), Patna (L5), Varanasi (L6), Kannauj (L7), Anup­ ronment and settled at ground level. Atmospheric deposition samples
shahar (L8), Rishikesh (L9) and Harsil (L10). The number signifies the were collected at ground level from riverbanks adjacent to the main
site’s position along the river, with L1 being closest to the ocean and L10 body of freshwater. A plastic funnel (13 cm diameter) was placed for 24
closest to the river source; the position number will be used predomi­ h, after which, each funnel was flushed with ~200 mL of DI water to
nately in lieu of the sampling site name throughout this paper. Further capture any atmospheric fallout on the funnel surface in a collection
information on site selection is reported in (Napper et al., 2021). bottle. On completion, the deionised water containing any atmospheric
Considering the large size and international transboundary nature of the deposition was poured through a nylon mesh (pore size 30 μm). Each
Ganges River, it was logistically difficult to choose >10 representative mesh was subjected to the same methodology as the water samples
sites and perform sampling. (Section 2.3.1) for transportation.

2.3. Sampling method 2.4. Laboratory analysis

Three different environmental mediums were collected from the The nylon mesh acquired from sampling each environment medium,
Ganges River and within its vicinity: water, sediment, and air (from and subsequent foil packaging, was examined for microplastics using a
atmospheric deposition) samples. The samples were collected during the light microscope (S9E - Leica) and information on the type of particle (i.
pre-monsoon season (May 2019 – June 2019). At each sampling site, a 5 e., fragment or fibre), dimensions (length and diameter) and colour was
km stretch of river was selected and samples were collected from three recorded. Visual analysis to classify suspected particles as natural or
points within it at 2.5 km intervals (0, 2.5 and 5 km). Replicate samples synthetic was based on methodology by Greaves and Saville, 1995
were collected on two consecutive days (n = 6 per site). Contamination (Stanton et al., 2019). Suspected microplastics (defined in this study as
control measures for all environmental mediums were applied either having length or diameter < 5 mm) were then analysed with
throughout the sample collection and transport process (see Section Fourier transform infrared spectroscopy (FT − IR) in transmission mode
2.5). Once collected, all samples were transported to either labs within with a Hyperion 1000 microscope coupled to a Vertex 70 spectrometer
the University of Dhaka (Bangladesh), the Wildlife Institute of India (Bruker). Any spectra were recorded with 32 scans in the region of
(India), or University of Plymouth (United Kingdom) for laboratory 4000–600 cm− 1. The spectra obtained were compared against a spectral
analysis. database of synthetic polymers (BPAD polymer and synthetic fibres
ATR). Rayon, as a synthetically altered cellulosic material, was included
2.3.1. Water sampling in this analysis to understand its proportion and similarities against
The water sampling method is outlined in Napper et al. (2021) which other plastic materials. It is reported as a common polymer type for
involved pumping 30 L water from 0.5 m below the river surface and microplastics in both freshwater and marine samples (Lindeque et al.,
then immediately filtering through a nylon mesh (pore size 330 μm). 2020; Nan et al., 2020; Park et al., 2020., Napper et al., 2023).
This pore size was chosen to mitigate additional organic matter clogging
the mesh apertures but was subsequently larger than both microplastic 2.5. Contamination control and quality control
screening in sediment and air. However, as the mean microplastic
lengths within sediment and air exceed a mean of >300 μm, it was Several steps were taken to mitigate potential contamination; before
assumed that mesh pore size was not a limitation (sediment and air mesh fieldwork each nylon mesh was inspected for contamination using a
pore size was 30 μm). After sampling, each nylon mesh filter was microscope (S9E - Leica), with any particles being removed before being
immediately double wrapped in foil and then placed in separate clear wrapped in two layers of clean foil, prior to and after sampling. For
polypropylene bags for transportation for further analysis. For water atmospheric deposition and sediment sampling, the equipment was
samples taken within tidal sections of the river (sites L1-L3), samples rinsed thoroughly with filtered DI water (30 μm nylon mesh) immedi­
were collected on an ebbing tide to ensure microplastics within the ately before deployment. Further contamination control for the water
outflowing river water were not those brought inshore from the Bay of sampling is outlined in Napper et al. (2021). Additionally, to account for
Bengal. potential airborne microplastic contamination from team members, a
damp (300 μm filtered DI water) filter paper (Whatman 47 mm diam­
2.3.2. Sediment sampling eter, 0.45 μm glass fibre filter) was placed nearby while samples were
River sediment was collected by either a Van Veen Grab (> 1 m water collected in an open petri dish; this was included for one replicate
depth) or stainless-steel spoon (< 1 m water depth). Sediment was taken sample from each environment medium at each site. The petri dishes
~1–3 m away from exposed riverbank. After collection, the sediment were kept open for the duration of the sampling so that the blanks and
was immediately placed into a plastic foil bag which was sealed using a samples were exposed to the same levels of airborne contamination. In
polyethylene cable tie. The foil bag was placed into a clear total, the procedural controls (air blanks) (n = 30) had an average of

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0.16 ± 0.08 MP filter− 1; (mean ± S.E.). For sediment samples, 1000 m− 2 ) across the different mediums (air, water and sediment) and
contamination from the foil and polypropylene bags used would have size was further log transformed. Both variables were then centered and
resulted in silver or clear coloured fragments, but the majority of scaled: y′i,j =
yi,j − yj
(yi,j ) is the log transformed size or abundance for
σ yj
microplastics reported were fibres (<5 % as fragments) and typically
every rep i for each medium j),
blue in colour (overall <10 % silver or clear). Overall, it was considered
that there was minimal contamination and no further contamination
3. Results
controls were necessary.
During all laboratory analysis, all steps were conducted in a dedi­
3.1. Abundance
cated clean room for microplastic work, which had limited access and
procedural blanks for each sample (n = 30) and had an average of 0.10
In total, 396 microplastic particles were identified across all envi­
± 0.06 MP filter− 1. Cotton laboratory coats and clothes were worn to
ronmental mediums; air (n = 131) sediment (n = 171) and water (n =
reduce contamination from synthetic textiles. All laboratory ware used
94). Across water and sediment environmental mediums, the number of
was made of glass or stainless steel and thoroughly rinsed with filtered
microplastics per sample increased with distance from the source of the
(1.6 μm) Milli-Q water before use.
Ganges (L10) to the sea (Fig. 2); as might be expected, this pattern was
not evident in the air samples. Additionally, both air and water showed a
2.6. Data analysis peak at L6, with another peak for water at L3, which typically reflected
higher areas of population density (Fig. 3). Mean microplastic abun­
Changes in response variables (microplastic count per sample and dance (mean ± S.E.) was 41.12 ± 3.99 MP m2 day− 1 in air. There was
microplastic length) were assessed with General Linear Models (GLMs) also 57.00 ± 5.27 MP kg− 1 in sediment and 0.05 ± 0.01 MP L− 1 in
for each environment medium (air, sediment and water) within the R water. With rayon removed from analysis, this abundance was 14.10 ±
computer programming language (R Core Team, 2019). Response met­ 7.03 MP m2 day− 1 in air, 10.30 ± 5.79 MP kg− 1 in sediment and 0.02 ±
rics were modelled as a function of Location (L1, L2, L3, L4, L5, L6, L7,
L8, L9 & L10); microplastic counts per sample exhibited a Poisson dis­
tribution, microplastic length exhibited a Gamma distribution, and both
polymer type and colour exhibited Binomial Distributions. The most
parsimonious models were selected by sequential removal of terms and
pairwise Akaike Information Criterion (AIC) comparison. To provide
pairwise comparison between locations, factor order manipulation was
carried out. Due to the different units, and different methods of collec­
tion for each environment medium (e.g. the differences between water
(300 um), sediment (30 um) and air (30 um) mesh pore size), there will
be no direct comparison of data but a discussion of similar trends. Non-
metric multidimensional scaling (MDS) was used to visualize relation­
ships between polymers and colours across locations and environmental
mediums; STRESS values were all below 0.16 which indicated that the
patterns in MDS were a good fit.

2.7. Population density

Population data for each of the sites were sourced from LandScan
(2019)™ High Resolution Global Population Data Set (copyrighted by
UT-Battelle, LLC, operator of Oak Ridge National Laboratory). Land­
Scan’s ambient population count incorporates census data and remote
sensing imagery analysis techniques, effectively providing a distribution
of where people go in a 24-h period. LandScan was chosen over other
commonly used datasets (e.g., Gridded population datasets such as
Gridded Population of the World (GPW), Global Human Settlement
Population Grid (GHS-POP) and WorldPop plus population counts from
statistical population records such as census and/or yearbooks). This
was due to a comparative study by Yin et al. (2021) who reported that
LandScan performed the best for spatial fineness and estimated errors.
Additionally, this methodology allowed for consistency across all sam­
pling locations for population estimation. However, it should be noted
that when analysing high population density and rapid population
growth areas, there are potential larger errors when using gridded
population datasets. Using ArcGIS Pro software (Esri), a 1 km2 circle
outline was placed over the center coordinates of each study site and
LandScan provided ambient population count per raster cell at
approximately 1 km spatial resolution. ImageJ (Fiji, 1.53c) was then
used to calculate the percentage cover of each population density range
Fig. 2. A - Microplastic abundance across locations and environmental me­
within the 1 km circle area. diums (sediment, water & air) (n = 6 per site). Symbols show abundances, solid
To assess change in abundance and size across environmental me­ lines show model estimates and shading model standard error. Dashed line
diums plus population density, a linear regression was used. Both vari­ represents microplastic proportions without rayon. B- Calculations of the
ables (abundance and size) were modelled as a function of the fourth average population (1000 people per 1km2. Density range within a 1 km2
root transformed population density within a 1 km radius (fourth root diameter circle at each sampling site. Data sources from Landscan 2019.

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Fig. 3. Proportional Contribution of Microplastic Polymer Mediums per Sample across Locations and Environmental Mediums (sediment, water & air) (n = 6
per site).

0.01 MP L− 1 in water. In terms of microplastic shapes, the majority of different environmental mediums, the mean size of microplastic was:
microplastics were fibres: 95 % fibres and 5 % fragments in air; 99 % 1320 ± 294 μm in air; 1650 ± 243 μm in sediment; and 1920 ± 454 μm
fibres and 1 % fragments in sediment and 96 % fibres and 4 % fragments in water. The longest sizes were seen at L5 in air (5670 ± 1490 μm) and
in water. L8 for water (5450 ± 1750 μm) (Fig. 4). The shortest mean length
overall was 1020 ± 180 μm within sediment. Such sizes exceed the
3.2. Polymer type largest mesh size (300 μm for water), and therefore there is more con­
fidence in their comparability. Microplastic size seems to become more
Of the 396 microplastics found in total across all environmental consistent nearer the sea, which may be due to a higher abundance of
mediums, FT-IR spectroscopy revealed that rayon was the most microplastics being found which could reduce the variability.
frequently recorded polymer but there were differences in abundance In total across all environmental mediums, the most dominant colour
throughout. Air and sediment mediums were similar; with rayon being found was blue (68 %), followed by red (11 %), and black and clear
the most abundant (66 % and 82 %, respectively). This was followed by (both 5 %). All other colours were below 5 %. Air (48 % & 21 %) and
polyester (17 %) and acrylic (10 %) for air, then polyester (10 %) and sediment (79 % & 21 %) both had blue and red as the dominant colours.
acrylic (6 %) for sediment. For water samples, rayon was still the Air had the greatest diversity in colours overall, additionally having
dominant polymer (54 %), followed by acrylic (23 %) and polyester and green and clear coloured plastics (both at 9 %). In water, the most
polyvinyl chloride (PVC) (both 9 %). All other polymers recorded were dominant colour found was also blue (74 %), followed by black (12 %),
below 5 % (Fig. 3). Focusing on abundance estimates removing rayon and red (5 %). All other colours were below 5 % (Fig. 5). No statistical
from the analysis, all other plastic mediums were consistent from source relationship was found between polymers and colours across locations
to sea, apart from water which was found to increase (Fig. 2). and environmental mediums (S1 Fig. 2).

3.3. Microplastic length and colour 3.4. Population density effects

Microplastic length was relatively similar across environmental The concentration of population density was compared against both
mediums, and GLM analysis showed that there were no significant microplastic abundance and the length of microplastics. Microplastic
changes in length along the Ganges (S1 Table 1, Fig. 4). Within the abundance increased significantly with higher population densities in
air and water but not in sediment (Fig. 6a, p < 0.05). However, popu­
lation density and environmental medium had no effect on the length of
microplastics (Fig. 6b, p < 0.05).

4. Discussion

While a number of studies have reported microplastics in freshwater


environments (Dris et al., 2018a; Phuong et al., 2022; Stanton et al.,
2019; Wagner et al., 2014; Yang et al., 2021), this study presents a novel
comparison throughout a whole major river system for three known
environmental mediums (water, sediment, and air) which are known to
contain microplastics. To the best of our knowledge, there is no research
which compares microplastics within these different environmental
mediums (river water, river sediment, and atmospheric deposition).
Fig. 4. Microplastic Length across Locations and Environmental Mediums
(sediment, water & air) (n = 6 per site). Symbols show lengths, solid lines show
average lengths from model estimates and shading model standard error.

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Fig. 5. Proportional Contribution of Microplastic Colours per Sample across Locations and Environmental Mediums (sediment, water & air).

4.1. Abundances of microplastics in different environmental mediums

Collectively, our results showed that microplastics were present


throughout the Ganges River system. However, each environment me­
dium showed a different pattern in terms of abundance. Microplastics in
air were found to be variable and strongly influenced by population.
Microplastics in sediment were found to progressively increase along the
river water course. Water had an intermediate variability affected by
population and perhaps by the volume of water.
Population density and environmental medium had no effect on the
length of microplastics which suggests similar sources of microplastics
throughout all mediums. Additionally, a clear observation is that the
vast majority of microplastics were fibres (>95 %). Microplastic fibres
can originate from textiles and can be mobilised by the wearing of
textiles during use in the home or outdoor settings resulting in atmo­
spheric deposition (Cai et al., 2017, 2021; De Falco et al., 2020), or from
the mechanical fragmentation of textiles during drying and laundering
(Geyer et al., 2022; Kapp and Miller, 2020; Napper and Thompson,
2016; O’Brien et al., 2020). It has been estimated that for polyester
clothing, one person could emit approximately 2.98 × 108 microfibres
per year to water by mechanical washing, and 1.03 × 109 microfibres
per year to the atmosphere by wearing polyester garments (De Falco
et al., 2020). Additionally, many communities use the Ganges fresh­
water for handwashing garments, often directly in the river (DuPont,
2013). The contribution of handwashing to microplastic pollution is not
well studied and will be more complex to solve than the current con­
siderations of application of filters to washing machines. It is important
to understand this better in the context of the Global South.
As such, it is expected that the abundance of microplastics would be
positively correlated with the degree of urbanization and population
density and places involving frequent human activities or near sewage
outlets. This study reports that microplastic abundance significantly
increased with higher population densities in air and water but not in
sediment. For air samples, Varanasi (L6) had the highest quantities of
microplastics settling from atmospheric deposition (75.3 ± 15.4 MP
m− 2 day− 1) and the largest population (population density estimated
between 4929 and 179,833 per km2); this may be due to the site being of
strong religious and heritage significance and higher quantity of tran­
Fig. 6. Change in abundance (a) and length (b) with population density across sient population including tourists from all across the globe. Whereas
environmental medium (sediment, water & air).
Rajbari (L3) had the lowest quantity of atmospheric microplastic (22 ±
8.31 MP m− 2 day− 1) and the 4th smallest population (population den­
sity estimated between 484 and 2413).

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A study by Napper et al. (2023) also had similar results, where they referred to as viscose), is derived from cellulose and modified chemically
tested atmospheric deposition in both urban and rural environments; for the manufacture of a wide range of products. Worldwide, polyester
they report that urban environments had an average deposition rate of has the highest market share of around 54 % of total global fibre pro­
123.2 ± 30.8 MP m− 2 day− 1, whereas rural environments had a third of duction, whereas manmade cellulosics fibres (MMCFs) (of which rayon
the amount at an average deposition rate of 40.1 ± 10 MP m− 2 day− 1. constitutes ~80 %) has 6 %. Rayon is often removed when classifying
Additionally, Varanasi (L6) also had the highest colour and polymer microplastics from environmental samples since cellulose and rayon
variety (joint with L7 and L10, respectively), likely due to clothing have almost identical FTIR spectra (Lusher et al., 2014; Napper et al.,
having a variety of colours and material types. Multiple microplastic 2023; Peeken et al., 2018), and a proportion of natural fibres may be
colours were observed in our study, but blue microfibres were the most mistaken for extruded textile fibres (Stanton et al., 2019).
predominant in all environment mediums and may be due to the colour However, rayon was decided to be included in analysis as India is the
blue being extensively used in synthetic clothes worldwide (Gago et al., world’s second largest producer and exporter of viscose fibre after China
2018). (accounting for about 11 % of the global rayon fibre production market;
Microplastics within water samples were also found to peak at Var­ Changing Markets, 2017) and proportions largely followed the same
anasi (L6). It has been stated that many urban areas located in the abundance patterns compared with the other plastic types reported
catchment of the Ganges generate vast quantities of wastewater; a major (Fig. 2). The potential high quantities of rayon may relate to previous
portion of which ultimately reaches the river untreated or partially reports of industrial effluent from producers being discharged into
treated through the natural drainage system (typically from Rishikesh Ganges River delta (Sinha and Khan, 2010). Additionally, a greater
(L9) onwards) (Dutta et al., 2020). Synthetic microfibres may be at high proportion of manmade cellulosics (such as rayon) is used for clothing
concentrations in wastewater due to laundry wastewater emissions (50–80 %) compared to polyester (30–60 %) (Changing Markets, 2017).
(Vardar et al., 2021; Xu et al., 2019; Yang et al., 2019) or urban surface Taking that into consideration, Zambrano et al. (2019) has previously
runoff (with plastic microfibres being the main contributor from atmo­ reported that rayon releases significantly more microfibres during
spheric deposition) (Dris et al., 2018b; Treilles et al., 2021; Werbowski washing than polyester fabrics as the cellulose-based fibres swell in the
et al., 2021). Varanasi is also one of seven holy cities in India and over water environment.
60,000 people gather daily for holy ritual bathing in the River (Kumar Rayon was the most abundant in sediment (82 %) followed by
et al., 2012). Due to Varnasi’s high population density, lack of efficient polyester and acrylic (10 % & 6 %, respectively). However, in compar­
sewage system at time of testing and mass participation in holy bathing, ison for water samples, rayon was still the dominant polymer (54 %), but
it is suspected that the peak in microplastic fibres likely accumulate from the medium had quadruple amounts of acrylic (23 %). This is likely due
these factors. to plastic density, where rayon has the highest density (1.52 g/cm3) and
However, unlike air samples, water samples had an additional peak acrylic has the least (1.10 g/cm3) (Morton and Hearle, 2008). Previ­
of microplastic at Rajbari, Bangladesh (L3). It has previously been re­ ously, Nizzetto et al. (2016) revealed that microplastics that have den­
ported that factors such as land use, infrastructure and socioeconomics, sities higher than water (1.00 g/cm3) could be retained in the sediment
as well as local site-level variables (e.g., vegetation height, site type) are as they are more likely to sink within the water column. Additionally,
more strongly correlated with plastic in the environment than popula­ previous research has reported a large proportion of microplastics in
tion density (Schuyler et al., 2021). Nelms et al. (2020) found that sediment suggesting that sediment was the main sink within a coastal
Rajbari was one of three sampling locations, from nine riverbank sur­ area (Ding et al., 2019) and continental shelf (Kukkola et al., 2022).
veys along the length of the Ganges river, where discarding macroplastic Subsequently, it is likely that a large majority of rayon in freshwater
fishing gear into the environment was the most common end-of-life gear sinks to the sediment whilst being transported by water flow. This may
outcome (50 %) (Nelms et al., 2020). Nelms et al. (2020), also reported lead to a gradual accumulation overtime which is shown in this study
that the three most common polymer mediums found for fishing gear (Fig. 2). Other less dense synthetic microplastics are likely to continue in
was nylon, polyethylene and polypropylene, but this was not reflected in the main body of water.
this study. Furthermore, Mendrik et al. (2023) reported that non-buoyant
At the time of sampling, Rajbari had no sewerage system and solid microplastic settling is influenced by a combination of biofilm growth,
waste was reported to be dumped in open dumping areas (~2 km away water salinity and suspended clay concentrations typically seen across
from the Padma River; a distributary of Ganges in Bangladesh) (LGED, fluvial to marine environments. Results indicate that biofilms signifi­
2016). Interestingly, this was also shown in Youngblood et al. (2022), cantly increased settling velocity of three different polymer types of non-
who reported that there were significantly higher quantities of littered buoyant microplastics (fragments and fibres, size range 0.02–4.94 mm)
items along the Ganges River in low populations compared with than by up to 130 % and significant increases in settling velocity were
those with mid to high populations, and it is likely that discrepancy in observable within hours. However, preliminary experiments that
access to waste management is a driving factor. Additionally, according included buoyant microplastics (polystyrene (PS), polypropylene (PP)
to Hafiz et al. (2017), in Bangladesh there is no effective waste man­ and high-density polyethylene (HDPE)) showed that the majority of
agement system, no proper recycling unit, and the single-use food these particles remained buoyant even after biofouling (Mendrik et al.,
packaging system is increasing. 2023).
Microplastics within sediment were found to steadily increase
throughout the Ganges river course from source to sea, which is likely 4.3. Microplastics in riverine systems
due to the gradual accumulation of different polymer types and re­
ductions in buoyancy. Nizzetto et al. (2016) reported that microplastics Previous microplastics research has focused on different environ­
that have densities higher than water could be retained in the sediment; mental mediums in riverine systems across the world, but with a
but high flow periods could remobilise this pool, meaning sediments in particular focus on either surface water, sediment or combined. How­
low flow river segments are likely hotspots for deposition of micro­ ever, there is a lack in understanding the proportion of atmospheric
plastics (Section 4.2). deposition as a source of microplastics into a river basin. In this study the
abundance of microplastic from atmospheric deposition around the
4.2. Prominent polymer types Ganges river system was recorded at 41 m2 day− 1. When comparing
different sources of microplastic, microplastics transported via air ap­
Although no relationship was found between polymers and colours pears to be a dominant pathway. For example, Sun et al. (2022) reported
across locations and environmental mediums, rayon was found to from their study that the total quantity of microplastics deposited in the
dominate the polymer type throughout (54–82 %). Rayon (commonly urban environment could reach 1.7–12 times of those discharged from

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treated wastewater. Among them, they predict that 10 % would directly 3,350,000 MP/m3) (Scherer et al., 2020). Additionally, for atmospheric
deposit to urban waters in the studied city region, while the others may deposition, we report that the Ganges river system had a mean of 41 MP
also enter the urban waters through runoff (the area of lakes and rivers m− 2 day− 1 which is less than that reported in Dongguan city (China;
accounts for 10 % of the total area of Shanghai). Additionally, Napper 175–313 MP m2 day− 1) (Cai et al., 2017), Yantai (China; 115–602 m2
et al. (2023) found atmospheric deposition of microfibres at an average day− 1) (Zhou et al., 2017), Paris (France; 118 m2 day− 1 (Dris et al.,
rate of 81.6 fibres m2 day− 1 across urban and rural areas. When 2015), Hamburg (Germany; 275 particles m2 day− 1) (Klein and Fischer,
compared against treated wastewater effluent (0.03 synthetic fibres 2019), while greater than that reported in Nottingham (UK; 0–31 fibres
L− 1), where they predict ~20,000–500,000 microfibres could be dis­ m2 day− 1) (Stanton et al., 2019). The shape, density and other features
charged per day from the Wastewater Treatment Plants studied, atmo­ can contibute to the transport of microplastics in the atmosphere, such
spheric deposition of synthetic microfibres appeared the most as the distance travelled and wet or dry depositions. Further, factors
prominent, releasing fibres at a rate of several orders of magnitude such as weathering, speed and direction of wind play an important role
greater than via treated wastewater effluent. This suggests that air in movement of microplastics from source to sinks (such as rivers and
quality management for microplastics may be more effective than the oceans).
wastewater management. However, there needs to be further research to This study has demonstrated that investigating microplastics in three
identify the main sources and subsequent potential methods to reduce key environmental mediums (water, sediment and air), can help further
such microplastic atmospheric deposition. identify potential sources through a more detailed understanding of
For sediment and water microplastics, our findings differ from other overall sinks, transport mechanisms and trends across a river system.
freshwater studies within the Ganges. Singh et al. (2021) completed Across water and sediment environmental mediums, the number of
research in early 2019 within the lower section of the Ganges River microplastics per sample increased with distance from the source of the
between Ballia and Diamond Harbour; within this study, the location Ganges (L10) to the sea (Fig. 2); as might be expected, this pattern was
represents locations around L4 – L5 but a different route through con­ not evident in the air samples. However, we report that for air and water
fluences to the Bay of Bengal through India. They report microplasitcs in samples, microplastic abundance significantly increased with higher
the ranges of 17 to 36 MP kg− 1 in sediments and 380–684 MP/1000 m3 population densities. As such, we demonstrate that microplastic emis­
(0.38–0.68 MP L− 1) in water at five different locations. There were also sion from freshwater into marine environments may be reduced due to
vast differences in microplastic characteristics; they reported that the particles sinking and accumulating in sediments. Additionally, we report
majority of microplastics were white in colour and films in shape. This that clothing is likely to be a prominent source of microplastics to a river
may be due to only recording for a proportion of the whole river, sea­ system, largely influenced by atmospheric deposition in high density
sonal/local variation or the sampling/laboratory technique. Subse­ population areas but also through lack of waste management facilities
quently, to understand the spatial and characteristic trends of (including effective wastewater treatment). Future research should
microplastics in a highly complex and dynamic nature of these major obtain a higher quantity of sample sizes to further confirm trends,
river systems, a repeated comprehensive and basin-wide approach is continue to investigate how such trends may fluctuate over time with
required to recognise trends arising both from natural environmental seasonal differences, and how results change with the implementation of
conditions and human-environment interactions. This includes under­ solutions.
standing sinks and accumulation of microplastics throughout a fresh­
water system. CRediT authorship contribution statement
The variety in field and laboratory methodologies makes comparing
quantities and characteristics of microplastics found in different envi­ Imogen E. Napper: Conceptualization, Methodology, Investigation,
ronmental mediums difficult. For example, freshwater microplastic Formal analysis, Data curation, Writing – original draft, Writing – re­
sampling techniques have included driftnets (Lechner et al., 2014), view & editing. Anju Baroth: Conceptualization, Methodology, Inves­
plankton net trawling (Scherer et al., 2020), water samplers (Fan et al., tigation, Writing – review & editing, Supervision. Aaron C. Barrett:
2019) and collection of water via a bucket and then filtering (Tee et al., Conceptualization, Methodology, Investigation, Writing – review &
2020). The quantity of samples may also have an impact and it should be editing. Sunanda Bhola: Conceptualization, Methodology, Investiga­
noted that within this study, a relatively low number of microplastics tion, Writing – review & editing. Gawsia W. Chowdhury: Conceptu­
were identified considering the number of samples taken (overall 396 alization, Methodology, Investigation, Writing – review & editing,
microplastic particles were identified from 10 sampling sites; n = 6 Supervision. Bede F.R. Davies: Investigation, Formal analysis, Data
replicates per site). Further, different minimum size limitations for mesh curation, Writing – review & editing. Emily M. Duncan: Conceptuali­
filtering may also be chosen. Therefore, to be able to compare locations, zation, Methodology, Investigation, Writing – review & editing. Sumit
there needs to be an agreement on and standardised approach to: 1) Kumar: Conceptualization, Methodology, Investigation, Writing – re­
applied field and laboratory techniques (including quantity of samples); view & editing. Sarah E. Nelms: Conceptualization, Methodology,
2) microplastic size range limits and 3) consensus on characteristic Investigation, Writing – review & editing. Nazmul Hasan Niloy:
definitions. There also needs to be further research at other locations Investigation, Writing – review & editing. Bushra Nishat: Investigation,
that compare microplastic across prominent environmental mediums Writing – review & editing. Taylor Maddalene: Conceptualization,
(air, water, sediment); as our research has shown, this helps to identify Methodology, Investigation, Writing – review & editing. Natalie Smith:
accumulation and distribution patterns, especially when observed Investigation, Formal analysis, Data curation, Writing – review & edit­
against population density. ing. Richard C. Thompson: Conceptualization, Methodology, Writing –
Considering the above limitations and differences, it is nevertheless review & editing, Supervision. Heather Koldewey: Conceptualization,
important to mention that microplastic concentration has been reported Methodology, Investigation, Writing – review & editing, Supervision.
higher in other large river systems; where we report the Ganges to have a
mean of 0.05 MP L− 1 in surface water. Such rivers include the Yangtze Declaration of competing interest
(China; 104 MP L− 1) (Fan et al., 2019), Seine and Marne Rivers (France;
106 MP L− 1) (Dris et al., 2015), Sungai Dungun River (Malaysia; 40–300 The authors declare the following financial interests/personal re­
MP L− 1) (Tee et al., 2020) and Elbe River (Germany; 6 MP L− 1) (Scherer lationships which may be considered as potential competing interests:
et al., 2020). Likewise, this was also found to be similar in the sediment Imogen Napper reports financial support was provided by National
component; in the Ganges we report microplastic concentration at a Geographic Society.
mean of 57 MP kg− 1, which is similar to the Dafeng River (China; 9.4 to
50.3 MP kg− 1 (Liu et al., 202) but lower than the Elbe River (Germany;

9
I.E. Napper et al. Science of the Total Environment xxx (xxxx) xxx

Data availability Duarte, C.M., 2014. Plastic debris in the open ocean. Proc. Natl. Acad. Sci. U. S. A.
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