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Science of the Total Environment 738 (2020) 139901

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Science of the Total Environment

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

Influential factors on microplastics occurrence in river sediments


Beibei He a, Buddhi Wijesiri a, Godwin A. Ayoko a, Prasanna Egodawatta a,
Llew Rintoul b, Ashantha Goonetilleke a,⁎
a
Science and Engineering Faculty, Queensland University of Technology (QUT), P.O. Box 2434, Brisbane, QLD 4001, Australia
b
Institute for Further Environments, Queensland University of Technology (QUT), P.O. Box 14 2434, Brisbane, QLD 4001, Australia

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

• Role of catchment and sediment charac-


teristics in microplastics in river sedi-
ments
• Bayesian Networks modelling to evalu-
ate microplastics occurrence in river
sediments
• Land use, population exert greater im-
pact on microplastics type not concen-
tration
• Clay particles influence microplastics
concentration in river sediments

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

Article history: Rivers are regarded as sinks and pathways of plastic pollutants from terrestrial environments to various other
Received 14 April 2020 aquatic systems such as lakes and oceans. Although extensive research has been conducted in recent years on
Received in revised form 31 May 2020 microplastic pollution in river sediments, knowledge on the relationships between potential influential factors
Accepted 31 May 2020
such as catchment characteristics and sediment properties, and microplastics occurrence in river sediments, is
Available online 02 June 2020
still considered an under-researched area. This study evaluated the influence of land use, population, and sedi-
Editor: Damia Barcelo ment particle size on the presence of microplastics abundance and types. Based on a Bayesian Network modelling
approach to characterise the correlations between influencing factors and microplastics occurrence, it was evi-
Keywords: dent that microplastics type had a positive correlation with different land use types and population. Catchment
Microplastics characteristics were found to play a more important role in influencing microplastics type than microplastics
Catchment characteristics concentration. A statistically significant positive relationship was observed between microplastics concentration
Sediment properties and clay particles which suggested that the occurrence of microplastics in sediments can be impacted by the
River sediments presence of clay particles.
© 2020 Elsevier B.V. All rights reserved.

1. Introduction

Microplastic pollution has been reported across various aquatic sys-


tems worldwide including lakes (Anderson et al., 2016; Boucher et al.,
⁎ Corresponding author. 2019; Xiong et al., 2018), rivers (He et al., 2020a, 2020b; Yan et al.,
E-mail addresses: beibei.he@hdr.qut.edu.au (B. He),
b.mahappukankanamalage@qut.edu.au (B. Wijesiri), g.ayoko@qut.edu.au (G.A. Ayoko),
2019), ponds (Bordos et al., 2019), estuaries (Ramírez-Álvarez et al.,
p.egodawatta@qut.edu.au (P. Egodawatta), l.rintoul@qut.edu.au (L. Rintoul), 2020; Richard et al., 2019) and oceans (Avio et al., 2015; Li et al.,
a.goonetilleke@qut.edu.au (A. Goonetilleke). 2016) in recent years. Past studies confirm that river sediments act

https://doi.org/10.1016/j.scitotenv.2020.139901
0048-9697/© 2020 Elsevier B.V. All rights reserved.
2 B. He et al. / Science of the Total Environment 738 (2020) 139901

not only as sinks for microplastics retention, but also as a medium for and even deposited in sediments (Ballent et al., 2012). Sedimentary
microplastics transportation along rivers to oceans (Andrady, 2011; microplastics could be either transported together with sediments, or
Avio et al., 2017). Despite the fact that extensive research has been un- resuspended and transported by hydraulic forces (Ballent et al., 2016).
dertaken on the abundance, spatial distribution patterns, sources of or- Such vertical and horizontal movements suggest that sediment particles
igin, and potential adverse impacts of microplastics (Horton and Dixon, can serve as carriers of microplastics (Horton and Dixon, 2018). This re-
2018; Wright et al., 2013), there is limited understanding of the role of sults in various distribution patterns of microplastics together with sed-
catchment characteristics and sediment properties on the distribution iment particle transportation behaviour. However, such combined
of different types of microplastics in river sediments. effects of catchment characteristics and sediment properties on
Past studies on microplastic pollution date back to 2004 with reports microplastics presence has not been investigated in-depth so far,
of the presence of small plastic particles in the marine environment which constrains the assessment of environmental risk of microplastic
(Thompson et al., 2004). Since then, the concentrations of different pollutants in aquatic environments.
microplastic debris, fragments, films and pellets in aquatic environ- This paper provides insights into the relationships among land use,
ments have been identified (Dris et al., 2015; Velzeboer et al., 2014). population, sediment properties, and microplastics. The outcomes of
As typical and widely used materials which play a prominent role in var- this study will enhance the knowledge base on how these influential
ious aspects of daily necessities, plastic pollutants such as polyethylene factors contribute to the occurrence and transportation of microplastics
(PE) and polypropylene (PP), which are the most widely used polymers in river sediments. Such understanding will guide environmental risk
in single-used packaging materials (Geyer et al., 2017), plastic bags management and critical decision-making relating to source tracking,
(Eerkes-Medrano et al., 2015), personal care products (Fendall and and transportation monitoring of microplastic pollutants in river
Sewell, 2009), textiles (Browne et al., 2011), are considered to be systems.
strongly associated with population and urbanisation characteristics
(Gatidou et al., 2019; Lechner et al., 2014; Nel et al., 2017; Peng et al., 2. Materials and methods
2018; Yan et al., 2019; Yonkos et al., 2014). Terrestrial anthropogenic
activities are thus considered as the main source which releases plastics 2.1. Study area and sample collection
to aquatic environments (Horton and Dixon, 2018), via wastewater dis-
charge, sewer system leaks, stormwater runoff, and prevailing wind This study was conducted in the Brisbane River, Queensland,
(Anderson et al., 2016; Eriksen et al., 2013). Abundance of microplastics Australia. Brisbane River is the longest river in Southeast Queensland,
in lakes, rivers, estuaries, and beaches worldwide have been docu- travels 344 km from Mount Stanley, flows through Brisbane City and
mented in highly populated areas or areas with intensive anthropogenic into Moreton Bay, and enters the Pacific Ocean (Straughan, 1972). Trib-
activities (Horton et al., 2017). Such studies include, Canada (Anderson utaries and creeks discharge into the Brisbane River, including Six Mile,
et al., 2016), China (Peng et al., 2018; Xiong et al., 2019; Yan et al., 2019), Goodna, Woogaroo and Bulimba Creek. Brisbane River catchment has
Italy (Fischer et al., 2016), Germany (Klein et al., 2015), Portugal wet summers and dry winters. The catchment encompasses various
(Rodrigues et al., 2018), and UK (Vaughan et al., 2017). land use types and urbanisation levels including agricultural (AGR),
Microplastic particles can float in water bodies due to their low den- commercial (COM), industrial (IND), natural (NAT), and residential
sity after being discharged into aquatic environments. However, after (RES) land uses.
microorganisms accumulation (Lagarde et al., 2016), microplastics on Fig. 1 shows the selected twenty-two sampling points from up-
the water surface can be drawn down into the deep water column stream (S1-S3) to middle stream (S4–S11) and downstream (S12–

Fig. 1. Sampling locations along the Brisbane River.


B. He et al. / Science of the Total Environment 738 (2020) 139901 3

S22) which covered different land uses along the Brisbane River, analysis using mean centering and standardising to eliminate the influ-
namely, S1–S3 mostly natural land (forest), S4–S12 moderately resi- ence of different variable scales. The data analysis was performed using
dential and natural land area, S13–S18 highly urbanised and commer- IBM SPSS Statistics 25.0 and Origin 2019.
cial area, S19–S22 highly industrialised and marina area. Sediment
samples on the surface layer (0–3 cm) from the centre of the river 2.3.2. Bayesian networks (BNs) modelling
were collected using a Ponar Stainless-steel Grab Sampler, in December Followed by qualitative PCA, a quantitative analysis was undertaken
(summer) 2017 and March (autumn), June (winter), and September using BNs modelling (Wijesiri et al., 2019) to further investigate how
(spring) 2018, respectively. Accordingly, a total of eighty-eight sedi- catchment characteristics and sediment properties influence the total
ment samples were collected. All the collected sediment samples were concentration of microplastics in sediments along the Brisbane River.
stored in pre-labelled 250 mL glass jars, transported on ice to the labo- Fig. 2 depicts the BNs model that describes the microplastics concentra-
ratory and stored below −20 °C until further analysis. Sample handling tions based on the influence of catchment characteristics, population,
was done in accordance with Australia/New Zealand Standards. and sediment properties. Further details on BNs modelling can be
The geographic location of each sampling site was recorded by GPS found in the Supplementary Information.
(Garmin Etrex 10 GPS). Catchment characteristics data such as different
land use areas at each sampling site was obtained from Queensland Spa- 3. Results
tial Catalogue website, and data manipulation was performed using
ArcGIS software. Resident population (POP) in the selected river section 3.1. Variability of microplastics distribution in river sediments
associated with each sampling site in Brisbane River catchment was ob-
tained from census data reported by the Queensland Government Fig. 3 shows the spatial distribution patterns of microplastics in river
Statistician's Office (Liu et al., 2017). sediments for the four different sampling episodes. High microplastic
concentrations were observed at the beginning of the summer season
2.2. Laboratory analyses and data generation (December), decreased in the late summer period (March) with the ex-
ception of site 4 (which is attributed to the fragmentation of large plas-
Pre-experimental study was done using NaCl with density of tic items). In the following winter season from June to September, an
1.2 g/mL, NaI solution with density of 1.5 g/mL, and ZnCl2 1.6 g/mL to increasing pattern of microplastic concentrations was observed. Addi-
extract virgin microplastic particles. Optimum separating results was tionally, as observed in Fig. 3, the hotspots of microplastic concentra-
obtained using the ZnCl2 extraction method. Therefore, in this study, tions (S4, S10–S12, S15, S20) were found to be associated with
microplastics in the collected sediment samples were extracted using different land uses including residential, industrial, commercial and nat-
ZnCl2 solution with a density of 1.6 g/mL, and then filtered by vacuum ural (forest) land.
filtration (MF Membrane Filters, 0.45 μm HA). After extraction, all The percentage of each microplastics type is given in Fig. 4, and an
suspected particles on the filter were further identified by Fourier increasing pattern of microplastics types can be observed from S1 to
Transform Infrared Spectroscopy (Nicolet iS50 FT-IR) instrument at S22. Polyethylene (PE) was the primary plastic type in upstream sites
4 cm-1 resolution and 64 scans. In this step, the spectra-matching rate which encompass natural land. Residential lands are abundant in the
of the tested particles was compared with polymer spectra database midstream area, where PE was the dominant microplastic type,
to obtain accurate results of the suspected particle types. Polymer parti- followed by polyamide (PA) and polypropylene (PP). Most microplastic
cles account for 90% of all the materials remaining on the filters. All types were observed in the downstream area, which consists of a range
identified microplastic particles were then photographed using a Leica of land uses including residential, commercial, and industrial.
M125 Metallographer, and weighed using an Analytical XSE 105DU an-
alytical balance with an accuracy of 0.01 mg (He et al., 2020a, 2020b). To 3.2. Relationships between microplastics and influential factors
avoid false negative and/or positive results for microplastic extraction,
various measures such as pre-experiments, laboratory blanks and Land use type and population were initially investigated to assess
non-plastic tools were used as part of the quality control and quality as- how these factors are correlated in terms of microplastics concentration
surance procedures. and type. The resulting PCA biplot is shown in Fig. 5. Microplastics con-
Malvern Mastersizer 3000 analyser, which utilises a laser diffraction centration was observed to have no correlations with some land uses
technique to measure particles sizes ranging from 0.01 μm to 3.5 μm
based on percentage volume distribution of particles, was used to deter-
mine the particle size distribution of the sediment samples. Appropriate
sediment sample quantity was added to the dispersion unit of the
Malvern Mastersizer 3000 instrument to obtain an obscuration value
of around 7% as recommended in the user manual. The volume-based
particle size distribution of the collected sediment samples for each
sampling site was derived accordingly. For quality control and quality
assurance purposes, laboratory blanks and a minimum of 10% of all sam-
ple replicates were analysed.

2.3. Data analysis

2.3.1. Statistical analysis


The data set of microplastics concentration and microplastics type
was initially analysed using descriptive statistical methods to under-
stand the spatial distribution patterns of microplastics in river sedi-
ments. Multivariate statistical technique, namely, principal component
analysis (PCA) was then applied to investigate the relationships
among land uses, population, sediment properties and microplastics oc-
currence. To avoid the influence of different variable scales on the out- Fig. 2. Graphical representation of Bayesian Networks (BNs) model of microplastics
comes, the original data set was pre-processed prior to the PCA concentration in sediments.
4 B. He et al. / Science of the Total Environment 738 (2020) 139901

Fig. 3. Spatial distribution of microplastics in Brisbane River sediments.

(natural and agriculture), and weak inverse correlations with the others ranges, namely, clay (b0.002 mm), silt (0.002–0.063 mm), fine sand
land uses (commercial, residential, and industrial) and population. (0.063–0.20 mm), sand (0.20–0.63 mm), and coarse sand (N0.63 mm)
However, microplastics type shows a strong positive correlation with to investigate the influence of particle sizes of sediments on
different land use types and population. microplastics presence. The data on each sediment particle size of
Based on the significance associated with particle size distribution, each sampling site can be found in Fig. S2 in the Supplementary Infor-
collected sediment samples were characterised for five different size mation. Fig. 6 shows the resulting PCA biplot of microplastics

Fig. 4. Spatial variation of different microplastic types in Brisbane River sediments.


B. He et al. / Science of the Total Environment 738 (2020) 139901 5

uses, which is evident from the strong positive relationship observed


(conditional regression coefficient – 5.074, 4.052, and 3.817, see
Table 1). In terms of sediment particles, a statistically significant positive
relationship (conditional regression coefficient – 2.402, p-value b0.01)
is observed between microplastics concentration and clay particles. In-
terestingly, coefficient index of the relationship between microplastics
concentration and sediment particle sizes decreases with the increasing
particle sizes (see Table 1).

4. Discussion

4.1. Influence of catchment characteristics on microplastics occurrence

Studies on microplastic pollution, both in the water column and sed-


iments suggest that microplastic concentration and type are strongly
linked to urbanisation (Ballent et al., 2016; Eriksen et al., 2013). How-
ever, our results indicate that land use and population have a relatively
greater impact on microplastics type rather than microplastics concen-
tration. This could be explained by the role of hydrologic conditions
such as water flow velocity in regulating microplastics distribution pat-
Fig. 5. PCA biplots of microplastics and catchment characteristics. (Note: AGR – terns after being discharged to rivers (Carson et al., 2013). Microplastics
agricultural land use, COM – commercial land use, IND – industrial land use, NAT – accumulation in aquatic environments has been reported as linearly re-
natural land use, RES – residential land use, POP – population). lated to seasonal precipitation events (Carson et al., 2013). The climatic
condition of Brisbane River catchment is sub-tropical with distinct wet
summer and dry winter seasons. The intensive storm events during
concentration related to various sediment particle sizes. According to summer are expected to result in more frequent transportation and
Fig. 6, clay particles show a relatively stronger correlation with mobilisation of microplastics together with sediments. Consequently,
microplastics concentration, as the angle between microplastics and lower accumulation of microplastics can be expected in the summer
clay particles is more acute compared to the other vectors. season in Brisbane River sediments, especially at the end of the summer
season (March) (Fig. 3).
Moreover, the downstream section of rivers is expected to have
3.3. Interdependencies among microplastics, catchment characteristics and
higher concentration of microplastic pollutants due to the transport of
sediment properties
microplastics by water flow (Ballent et al., 2016). However, the spatial
distributions of microplastics concentration along Brisbane River did
Table 1 gives the estimated BNs model parameters that describe the
not show a consistent pattern of increase or decrease for the four differ-
relationships among microplastics, land uses, population, and sediment
ent sampling episodes (see Fig. 3). The pattern of spatial variation of the
properties. The performance of the BNs model was deemed satisfactory
hotspots of microplastics indicates that not all microplastics are likely to
as evident from the results of the overall model F-test (p-value b0.01,
be transported from upstream to downstream (He et al., 2020a, 2020b).
see Table 1) and Fig. 7. As evident from Table 1, microplastics concentra-
It is evident that there is a statistically significant negative relationship
tion shows a statistically significant negative relationship (conditional
between microplastics concentration and industrial land use (see
regression coefficient – −10.267, p-value b0.05) with industrial land
Table 1), as the industrial area is in the downstream part of the Brisbane
use. While highly related to commercial, natural, and agriculture land
River catchment, namely, from SP 19 to SP 22. Since part of the
microplastics load can be retained in the upstream sediments through
deposition due to the changes in hydrodynamic forces, it is thus a lesser
amount of microplastics that would be accumulated in the downstream
area (Besseling et al., 2017). Consequently, understanding the differ-
ences in the concentration and type of microplastics could thus be sug-
gested as an approach to source tracking of microplastic pollutants
(Duis and Coors, 2016; Horton and Dixon, 2018).
Brisbane River is subjected to diverse sources of terrestrial pollution
inputs. Although S1-S3 in the upstream section is mostly natural land,
plastics that are carried from the upstream can make a considerable
contribution to microplastic pollutants at the sampling sites. PE is the
dominant microplastic type in upstream sediments as shown in Fig. 4.
This can be caused by the wide use of PE products (Blettler et al.,
2018; Horton and Dixon, 2018), which accounts for 70% of all
microplastic pollutants in Brisbane River sediments (He et al., 2020a,
2020b). Residential land is the main land use in the midstream area.
Plastics originating from daily usage, such as microbeads from cosmetics
products (Napper et al., 2015), nylon fibres from clothes (Browne et al.,
2011), are commonly discharged to waterways via sewage effluent and
sewer system leakages (Browne et al., 2010). Additionally, runoff con-
taining microplastics from a variety of domestic waste sources can be
transported to water bodies (Gatidou et al., 2019). PE, PP, and PA in
Fig. 6. PCA biplots of microplastics and sediment properties. (Note: CL – clay content, CO – downstream sites could either originate from upstream transportation
coarse particle content, FI – fine particle content, SA – sand content, SI – silt content). or inputs from downstream sites while other microplastic types such
6 B. He et al. / Science of the Total Environment 738 (2020) 139901

Table 1
Estimated conditional regression coefficients for the Bayesian Networks (BNs) model of microplastics concentration as a function of catchment characteristics and sediment properties
(Gaussian distribution, log transformed data). Note: AGR – agricultural land use, COM – commercial land use, IND – industrial land use, NAT – natural land use, RES – residential land
use, POP – population, CL – clay content, CO – coarse particle content, FI – fine particle content, SA – sand content, SI – silt content.

Response variable Predictor variables

Catchment characteristics Sediment properties


Population (POP) Standard deviation of residuals
Microplastic AGR COM IND NAT RES CL CO FI SA SI
3.817 5.074 -10.267* 4.502 −0.751 1.215 2.402** 0.480 4.698 1.828 4.007 0.353

Conditional density: Microplastic | AGR + CL + CO + COM + FI + IND + NAT + POP + RES + SA + SI.
Leave-one-out cross validation.
Significance codes: ** 0.01 * 0.05.
Overall model p-value (F-test): 0.00543 (b0.01).

Fig. 7. Performance of the Bayesian Networks (BNs) model for total concentration of microplastics: (a) Observed vs Predicted; (b) Residuals.

as polyethylene terephthalate (PET), and polyvinylidene fluoride Richard et al., 2019), enhance the degradation of large plastic fragment
(PVDF) in sediments can be primarily attributed to industrial effluent into smaller plastic debris (da Costa et al., 2016) and lead to changes in
or stormwater runoff from the surrounding industrial areas (Nizzetto the settling velocities and settling processes of microplastics (Kowalski
et al., 2016). et al., 2016). Consequently, the interaction and adsorption between set-
According to the study by Carr et al. (2016), most current wastewa- tled microplastics and sediment particles are likely to be changed. How-
ter treatment plants though effective at removing a high percentage of ever, due to the very limited number of published studies and the lack of
microplastics, are not able to fully remove microplastics from the waste- comprehensive data sets on the interactions between the distribution
water stream. Additionally, due to the differing density of various and transport of microplastics and other potential influential factors
microplastics materials which could be either the result of manufactur- (such as flow velocity, wind, and sediment clays), further in-depth in-
ing properties or biofilm accumulation (Wu et al., 2017; Zettler et al., vestigations are needed to derive a detailed understanding of the depo-
2013), the sedimentation and resuspension processes can vary for dif- sition and transportation mechanics between different sediment
ferent microplastic types. Therefore, further research is needed to eval- particle types and microplastics.
uate the transportation and deposition characteristics under different
hydrodynamic conditions of flow.
5. Conclusions

4.2. Influence of sediment properties on microplastics transport Despite the fact that microplastics pollution in aquatic environments
is increasingly being detected worldwide, there is lack of understanding
The occurrence of microplastics in sediments can be impacted by the regarding the influential factors in relation to microplastics occurrence
sinking/floating behaviour of different sediment particles due to the and prevalence in river environments. The research outcomes highlight
mechanical forces between clays and microplastic particles the correlations among the factors that potentially influence
(Chubarenko et al., 2020). The positive relationships between microplastics occurrence. Land use was observed to be highly correlated
microplastics concentration and clay fraction found in this study suggest with microplastic types, while weakly correlated with microplastics
that the deposited microplastics are expected to have similar dynamics concentration. This suggests that land use is the major contributor to
as clay sediment particles in relation to the transport processes. How- microplastics type rather than to microplastics concentration. There-
ever, Li et al. (2019), showed that there is limited influence of small fore, prudent land use planning and management can reduce the inputs
suspended particles (b10 μm) on the microplastics settling process. of specific types of microplastics, especially polymers which are
This can be explained by the different degradation levels of the surveyed manufactured using highly hazardous chemical compounds. Addition-
microplastics. Once released into the aquatic environment, the interac- ally, the study outcomes have identified the decreased coefficient
tions between plastics and bio/abiotic factors (such as the presence of index between microplastics abundance and sediment particles with in-
microorganisms, UV radiation) are expected to weaken the molecular creased sediment grain size. The outcomes indicate that finer the sedi-
structure and alter the density of plastics (Chubarenko et al., 2020; ment clays, the more abundant are microplastics. The study outcomes
B. He et al. / Science of the Total Environment 738 (2020) 139901 7

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Pollut., 114490 https://doi.org/10.1016/j.envpol.2020.114490.
Supplementary data to this article can be found online at https://doi. He, B., Goonetilleke, A., Ayoko, G.A., Rintoul, L., 2020b. Abundance, distribution patterns,
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