Coupling of Microplastic Contamination in Organisms and The Environment Evidence From The Tidal Flat Ecosystem of Hangzhou Bay, China
Coupling of Microplastic Contamination in Organisms and The Environment Evidence From The Tidal Flat Ecosystem of Hangzhou Bay, China
Research Article
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
A R T I C L E I N F O A B S T R A C T
Editor: Joao Pinto da Costa Microplastics are a new type of contaminant, widely defined as fragmented plastics with the longest dimension or
diameter less than 5 mm, that are widely distributed, difficult to degrade, and easily adsorb other pollutants.
Keywords: Estuaries are key habitats where terrestrial microplastics flow in water runoff and import into the ocean. The
Microplastics ubiquitous use of plastics has resulted in a massive amount of plastic waste that is released and accumulated in
Hangzhou Bay
bay ecosystems, posing serious ecological impacts. The study of microplastic contamination in Hangzhou Bay,
Tidal flats
the estuary of the Qiantang River, has important theoretical value in ecology and environmental science.
Organisms
Coupling Microplastic contamination in the tidal flats and organisms of Hangzhou Bay is serious and microplastic char
Spatial statistics acteristics (type, size, and polymer type) in organisms were significantly correlated with those in the environ
mental media. Spatial autocorrelation was found in the abundance of microplastics in marine and tidal flat
sediments of Hangzhou Bay, China, but no spatial autocorrelation was found in the sediment environment as a
whole. The microplastic abundance in each organism in this study was not statistically correlated by weight or by
individual count with its corresponding trophic level (P = 0.239 > 0.05; P = 0.492 > 0.05, respectively). Our
study suggests a coupling relationship of microplastic contamination between organisms and the environment
Abbreviations: PP, Polypropylene; ABS, Acrylonitrile-Butadiene-Styrene; AA, Acrylic Acid; CP, Cellophane; CA, Cellulose Acetate; LDPE, Low-Density Poly
ethylene; HDPE, High-Density Polyethylene; PS, Polystyrene; PP+PE, Polypropylene+Polyethylene; PPC, Polypropylene Copolymer; PAA, Poly(Acrylic acid); PET,
Polyethylene Terephthalate; PVT, Polyvinyltoluene; PMP, Polymethylpentene; PVC, Polyvinyl Chloride; PU, Polyetherurethane; PA, Polyamide; PI, Polyimide; PE,
Polyethylene; PL, Polyester; HEC, Hydroxyethyl Cellulose; RY, Rayon; CE, Cellulose; μ-FTIR, μ-Fourier Transform Infrared Spectroscopy.
* Corresponding authors.
E-mail addresses: [email protected] (H. Chen), [email protected] (B. Jin), [email protected] (J. Lu).
https://doi.org/10.1016/j.jhazmat.2023.131838
Received 31 March 2023; Received in revised form 9 June 2023; Accepted 10 June 2023
Available online 12 June 2023
0304-3894/© 2023 Elsevier B.V. All rights reserved.
X. Cai et al. Journal of Hazardous Materials 457 (2023) 131838
and can provide essential data and a scientific foundation for the study of microplastics pollution in Hangzhou
Bay, as well as provide important evidence for the ecological and health risk assessment of microplastics.
1. Introduction may be less harmful than previously thought [7]. A correlation between
microplastic community composition in different habitats was also
Marine plastic litter has become an ecological pollution problem of observed to gradually weaken with the increase in point source distance
global concern due to the large and increasing threat it poses to marine [18]. Several experimental laboratory-based studies have been con
and coastal tidal flat ecosystems. After being exposed to long-term ducted but do not fully reflect the true field ecosystem and may have
physical, chemical, and biological processes in the marine environ limited applicability to the natural environment, due to crucial differ
ment, plastic litter is eventually broken down into plastics with ences between the characteristics of microplastics in fish in a laboratory
maximum diameters less than 5 mm, known as “microplastics”. The environment and the natural environment [17,19]. However, there are
fragmentation of large, individual plastic items leads to the creation of studies that suggest that the trophic level of fish is one factor that in
millions of microplastics, which are thought to be the direct source of fluences microplastic uptake in fish [20]. In contrast, another study
most of plastic debris in the ocean today [1]. The emergence of micro found no microplastic accumulation in the food web [21]. Microplastics
plastics in the environment may pose an ecological threat to human in mangrove habitats appear to transfer between different trophic levels
existence. and are bioamplified in successive trophic levels [22]. However, a
More than 80% of marine plastic waste comes from land [2]. The different study suggested that the microplastic pollution in benthic or
developed economies of coastal areas, along with the large populations ganisms is not affected by the changes of biological habitat or trophic
close to the coastline, generate land-based sources of plastic waste that level [23]. Therefore, by collecting wild aquatic organisms from natural
enter the marine ecosystem directly or indirectly through sewage sys habitats of estuaries and testing whether the microplastic content in
tems, rivers, the atmosphere, and human activities (tourism and aqua them is related to the microplastic content deposited in the environment
culture) [3]. Estuaries are key areas where terrestrial microplastics flow of the same site based on their trophic levels, the sources and entry
with water runoff and import into the ocean [4,5]. The process of flow routes of microplastics in estuaries can be identified. In turn, these re
diffusion in estuarine habitats is complex, and is further complicated by sults may inform the local protection of marine fisheries.
the influence of tides, waves, coastal currents, estuarine topography, Hangzhou Bay is an offshore tidal flat ecosystem in China. It is an
and evolution. Therefore, the special geographical environment of urban estuary of Qiantang River that is also affected by runoff from the Yangtze
estuarine habitats increases the possibility of microplastic deposition River. Here, sediment and organic particles carried by the rivers interact
and accumulation, leading to high microplastic load in estuarine habi with ocean currents of the Pacific Ocean to form one of the world’s
tats. The high load of microplastics in estuarine habitats is not only largest fisheries — the Zhoushan fishery. The aims of this study are: 1) to
manifested in environmental media, but also in the organisms that examine the microplastic pollution in organisms in the estuary
inhabit estuarine ecosystems, such as the sandworms of Haeju Bay and ecosystem of Hangzhou Bay and analyze its spatial correlation with
its intertidal zone in North Korea, the Xiangshan Harbor and its farmed environmental microplastic pollution; 2) to explore the relationship
fish in China, the Cienfuegos Bay and its local Perna viridis in Cuba, and between microplastic pollution and trophic level of marine economic
the Terengganu estuary and its zooplankton in Malaysia [6–9]. Typical species of Hangzhou Bay and whether there is a biomagnification of
indicator organisms, such as sand worms, also actively ingest micro microplastics; 3) to quantify the load of microplastics in marine species
plastics and the degree of microplastic pollution in their bodies can of commercial interest located in the coastal ecosystem of Hangzhou Bay
reflect the degree of microplastic pollution in habitats overall, such as and assess the risk of microplastic accumulation in humans through
tidal flats and estuarines where microplastic pollution is high [9]. consumption of marine food products.
Gulf estuaries are highly productive ecosystems with a large amount
of nutrient turnover. Upstream deposition of man-made products 2. Study area and methods
transport large amounts of organic debris, which usually accumulate in
coastal and off-shore fisheries around the mouth of bays, such as 2.1. Overview of the study area
Newfoundland fishery in Canada and Zhoushan fishery in China. These
ecosystems bring together a great diversity of aquatic species that are Hangzhou Bay, located in the northeastern part of China’s Zhejiang
freshwater, marine, and those that migrate between both bodies of province, has the largest tidal difference of any bay along the coast of
water. The aquatic products of these systems (e.g., shellfish, crabs, China, and is one of the eight largest estuaries in China. It contains a
shrimp, fish, seaweed) are important sources of food for humans. Bay typical coastal wetland ecosystem with a tidal flat area of about 550 km2
estuary areas are not only an economically developed areas, but also and is listed as an important wetland in China. Hangzhou Bay is rich in
ecologically vulnerable zones that are crucial to sustainable develop nutrients, fertile water, bait organisms, and hydrological environment,
ment [10]. Identifying microplastic contamination in aquatic life in and has many large fishing grounds, rich fishery products, and a
coastal regions is particularly important to analyze the threat of developed fishery economy. Hangzhou Bay is also an important
microplastics to human health. Understanding how microplastics affect stepping-stone along the migration route of East Asian migratory birds,
estuarine life is therefore of interest not only to biologists, but increas and a large number of wetland water birds inhabit this location [24].
ingly to policy makers and environmental managers. In recent decades, China’s economic and social development has put
Most studies across the globe have reported the presence of micro tremendous pressure on the coastal waters around Hangzhou Bay due to
plastics in freshwater, coastal environments, and organisms [11–16], pollution. As early as 2003, the Zhejiang provincial government
but few studies have focused on the relationship between marine sedi included the six cities along the coast into the Hangzhou Bay area, which
ments, organisms, and microplastic contamination in the surrounding now account for 79.80% of Zhejiang’s total economic output. Hangzhou
tidal flats. Similarly, few studies have attempted to track the fate of Bay is located in a highly urbanized area of eastern China that includes a
microplastics and mixed contaminants through the complex marine food variety of industries (e.g., chemical, dyeing, and food factories) and
web using environmentally relevant concentrations to identify the true hydroelectric power plants [24]. The Hangzhou Bay region has experi
level of risk [17]. One study indicated that microplastic pollution in enced increased urbanization, industrialization, and agricultural devel
cultured marine economic species in Xiangshan Bay of China was related opment. These human and economic activities have resulted in the
to trophic level changes, but microplastic impacts on commercial species import of large amounts of harmful pollutants into Hangzhou Bay [25],
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X. Cai et al. Journal of Hazardous Materials 457 (2023) 131838
leading to the continued deterioration of environmental quality in the Boleophthalmus pectinirostris, Uroteuthis edulis, Harpadon nehereus, Pam
region [26]. pus argenteus, Larimichthys polyactis; Table S1) were thawed (− 20 ◦ C),
washed, and drained. Samples of similar size were selected, body lengths
2.2. Sample collection and weight were measured, carapaces shellfish were removed, and the
weight was again measured. Tissue digestion was performed using a
Employing a grid sampling method, a grab sampler (Van Veen, mixture of 150 mL 10% KOH solution and 50 mL 30% H2O2. The
Hydro-Bios, Germany) was used to collected 5 cm of surface depth digestion was performed in an oscillatory incubator at 60 ◦ C and
marine sediment at stations M 1–13 in the summer of July 2020 (see 135 rpm/min for at least 24 h until the biological tissue is completely
Fig. 1). Tidal flat sediment samples at 5 cm surface depth were collected digested where the solution appeared clear. Sediment samples were
at stations T 1–5 in the summer of July 2021 using a shovel, and the processed in a similar manner.
samples were stored in an aluminum box (see Fig. 1). Processed samples were observed with a stereomicroscope (SteREO
Several organism samples were caught directly in the tidal flats of Discovery V8 Zeiss, Carl Zeiss Microimaging Gmbh, Germany) and
Hangzhou Bay in July 2021 and several samples of organisms from suspected microplastics were identified, photographed (OPLENIC, C33,
Hangzhou Bay were caught by local fishermen in October 2021. The OPLENIC, America), and counted. The type and color of the micro
legends and specific information about the organism samples are shown plastics were categorized and the dimensions were measured using
in Annex Table S1 and Fig. S1. ZenLite software (Carl Zeiss Microimaging Gmbh, Germany). The
chemical components of all suspected microplastics were identified by
Fourier-transform infrared spectroscopy (Nicolet iN10, ThermoFisher
2.3. Extraction and identification of microplastics Scientific, US). Scans were performed 64 times using a 150 µm
× 150 µm aperture at 8 cm− 1 resolution in liquid nitrogen-cooled
Three sediment parallel samples were taken from each site and the transmission mode, and measured spectra were recorded in the
sediment samples (about 160 g) were placed in a 60 ◦ C oven to dry to 650–4000 cm− 1 aperture range. Spectra were compared with the
constant weight. Saturated 300 mL NaCl solution (at least 400 g of NaCl organic ensemble spectral library to verify the polymer type. Consid
was added into 1 L Milli-Q water at 40 ◦ C. The solution was stirred until ering the very small number of microplastic samples at some sites, a
the NaCl was precipitated. After cooling at room temperature, the NaCl matching degree of more than 65% was identified as corresponding to
crystals were resolved to determine the saturated NaCl solution) was known polymers.
added for flotation and stirred well to cause the plastic sample float on
the liquid surface. After standing for at least 2 h, supernatant was
transferred to another beaker and the above steps were repeated 3 times 2.4. Statistical methods
for each sample to improve the plastic recovery rate⋅H2O2 solution
(30%, 150 mL) was added to digest the organic matter and after The microplastic abundances, sizes, types, and chemical composi
standing at room temperature for 24 h, the digested solution was filtered tions in the sediment and organism samples were characterized based on
with a vacuum filtration device and additionally filtered through a glass the experimental results. Sediment microplastic abundance was calcu
fiber membrane (GF/F, pore size 0.7 µm, diameter 47 mm). Filter lated by weight as items/kg (dw). The microplastic abundance of or
membranes were dried at 60 ◦ C. ganisms was calculated by weight as items/g (ww) and by number of
A total of 13 organism samples (Bullacta exarata, Cerithidea largillierti, individuals as items/individual. The microplastic size was counted every
Mactra veneriformis, Sinonovacula constricta, Exopalaemon modestus, 1000 µm. The microplastic types were divided into six categories: fibers,
Chinomantes dehaani, Scylla serrata, Portunus trituberculatus, fragments, lines, films, foams, and pellets.
Fig. 1. Map of Hangzhou Bay, showing the sediment sampling locations. Different colors represent different types of land use. ▴: Sampling location; M: Marine; T:
Tidal flat.
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X. Cai et al. Journal of Hazardous Materials 457 (2023) 131838
The method for obtaining the trophic level and specific values can be the same as those of other groups but without experimental samples. All
found in Table S1. Sampling maps were plotted using ArcGIS 10.6, and solutions used in the experiment were filtered through glass fiber
all resulting maps were completed using Origin 2021 software. One-way membranes for later use. No microplastics were found on the glass fiber
analyses of variance, independent sample t-tests, and bivariate correla filter of the blank control group. All glassware and dissection vessels
tion analyses were performed on the experimental results using SPSS were rinsed three times with filtered Milli-Q water. The utensils used for
19.0 software to test for differences (ANOVA) or correlations (data sample collection and all the tools and containers during the experiment
normally distributed: Pearson correlation analysis; non-normal distri were made of metal or glass. Experimenters wore cotton lab coats and
bution: Spearman rank correlation coefficient) among the data groups. cotton gloves to reduce microplastic pollution in the air while per
The term spatial autocorrelation refers to the presence of systematic forming field sampling and laboratory work. Samples are stored sepa
spatial variation in a mapped variable. Where adjacent observations rately and sealed to prevent any post-collection contamination.
have similar data values, the map shows positive spatial autocorrelation.
Where adjacent observations tend to have very contrasting values, then 3. Results
the map shows negative spatial autocorrelation. A semi-variogram
analysis of the spatial distribution of microplastic abundance (using a 3.1. Characteristics of microplastic contamination in sediments of
pure nugget effect model with random variation and distribution of Hangzhou Bay
microplastic abundance was performed on microplastic abundance data
from two environmental media) was conducted and semi-variogram As shown in Table 1, the overall microplastic abundance in sedi
plotting was completed using GS+ Version 9 [27]. ments of Hangzhou Bay ranged from 3.32 to 35.12 items/kg, with an
average abundance of 16.85 items/kg. Microplastic types were primar
2.5. Quality control ily fibers and fragments, black or blue in color, the majority of which
were less than 2000 µm; PP was the main polymer collected. The main
Three procedural blank control groups were set up in the experiment, polymers in the marine sediments were PL, CE, and RY, which did not
and all the experimental steps of the blank control group were exactly match the main polymers of the overall sediments. The microplastic
Table 1
Microplastic contamination in sediments in various environmental media.
Area Range of abundance (items/kg) Average abundance (items/kg) Main types Main colors Main size scale (μm) Main polymers
Marine 3.32–26.15 13.16 ± 1.82 Fiber (92.16) Black (52.94) 1–1000 (64.71) PL (29.41)
1001–2000 (31.37) CE (25.49)
RY (23.53)
M1 0.00–9.07 5.88 ± 2.94 Fiber (100.00) Black (100) 1–1000 (100.00) CE (50.00)
RY (50.00)
M2 9.17–30.14 19.19 ± 6.07 Fiber (100.00) Black (66.67) 1–1000 (100.00) RY (33.33)
M3 0.00–25.67 8.56 ± 8.56 Fiber (100.00) Blue (50.00) 1–1000 (100.00) PS (50.00)
White (50.00) RY (50.00)
M4 0.00–23.68 11.23 ± 6.86 Fiber (100.00) Black (75.00) 1001–2000 (50.00) CE (50.00)
PP (50.00)
M5 9.31–34.03 20.12 ± 7.30 Fiber (100.00) Blue (40.00) 1–1000 (60.00) PL (40.00)
Transparency (40.00) 1001–2000 (40.00) CE (40.00)
M6 0.00–18.50 9.00 ± 5.35 Fiber (100.00) Black (66.67) 1–1000 (33.33) CE (33.33)
1001–2000 (33.33) CA (33.33)
2001–3000 (33.33) RY (33.33)
M7 0.00–9.95 3.32 ± 3.32 Fiber (100.00) White (100.00) 1–1000 (100.00) PS (100.00)
M8 9.45–30.94 21.28 ± 6.30 Fiber (83.33) Black (66.67) 1–1000 (33.33) PL (50.00)
1001–2000 (66.67) CE (33.33)
M9 0.00–10.57 6.44 ± 3.26 Fiber (100.00) Blue (50.00) 1–1000 (50.00) PL (50.00)
White (50.00) 1001–2000 (50.00) RY (50.00)
M10 11.13–48.82 26.15 ± 11.53 Fiber (75.00) Black (62.50) 1–1000 (87.50) PL (37.50)
PS (25.00)
M11 10.93–25.72 15.96 ± 4.88 Fiber (100.00) Black (75.00) 1–1000 (50.00) PS (75.00)
1001–2000 (50.00)
M12 0.00–9.53 6.25 ± 3.12 Fiber (100.00) Red (50.00) 1–1000 (50.00) CE (100.00)
Transparency (50.00) 1001–2000 (50.00)
M13 9.32–25.66 17.71 ± 4.72 Fiber (83.33) Black (50.00) 1–1000 (66.67) PL (33.33)
White (33.33) 1001–2000 (33.33) RY (33.33)
Tidal flat 7.92–35.12 18.63 ± 2.62 Fiber (52.17) Black (25.00) 1–1000 (44.89) PP (38.07)
Fragment (29.55) Blue (25.00) 1001–2000 (31.25)
Green (22.16)
T1 2.75–32.00 9.43 ± 4.60 Fiber (68.42) Black (36.84) 1–1000 31.58) PP (31.58)
Transparency (31.58) 1001–2000 (52.63) PET (21.05)
T2 2.12–16.82 7.92 ± 4.52 Fiber (100.00) Blue (30.00) 1–1000 (40.00) PP (70.00)
Black (40.00) 1001–2000 (30.00)
T3 4.39–28.70 14.13 ± 3.27 Fiber (68.75) Blue (37.50) 1–1000 (40.63) PP (18.75)
Black (28.13) 1001–2000 (37.50) CE (18.75)
RY (18.75)
T4 11.43–34.65 21.19 ± 3.20 Fiber (40.48) Green (47.62) 1–1000 (60.47) PP (54.76)
Fragment (38.10) 1001–2000 (28.57)
T5 22.52–52.08 35.12 ± 5.18 Fiber (41.10) Blue (23.29) 1–1000 (41.10) PP (42.47)
Fragment (39.73) Black (26.03) 1001–2000 (24.66)
2001–3000 (20.55)
Total 3.32–35.12 16.85 ± 1.92 Fiber (61.23) Black (31.28) 1–1000 (49.34) PP (30.40)
Fragment (23.35) Blue (21.15) 1001–2000 (31.28)
Note: The value in brackets is the percentage of each factor in the total number (%).
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X. Cai et al. Journal of Hazardous Materials 457 (2023) 131838
characteristics of other marine or tidal flat sediments were similar to microplastic found was fiber, the main colors were black and blue, the
those of the overall sediments. The legend, abundance, and character most common sizes ere less than 2000 µm, and the main polymers were
istics of microplastics are shown in Annex Figs. S2–4 and 6. RY, CE, and PL. The characteristics of microplastics in marine or tidal
flat organisms were similar to those in the overall sediments. The
abundances and characteristics of microplastics are shown in Annex
3.2. Spatial distribution of microplastics in the sediments of Hangzhou
Figs. S5–6.
Bay
The correlation analysis of microplastic abundance performed for
each organism and its corresponding trophic level revealed no signifi
The results of a semi-variance analysis indicated that no spatial
cant correlation between microplastic abundance and changes in the
distribution pattern was observed in the microplastic abundance from
trophic level of organisms. This result was true when the analysis was
the overall sediments of Hangzhou Bay. However, in the variation model
applied by both the soft tissue weight and individual counts
of microplastic abundance in marine sediments, which used a spherical
(P = 0.239 > 0.05; P = 0.492 > 0.05) (see Fig. 3).
model with spatial dependence, several regions had extremely low or
high microplastic abundance (see Fig. 2a). The variation model of
3.4. Correlation of microplastic characteristics between sediments and
microplastic abundance used for tidal flat sediments was a Gaussian
organisms in Hangzhou Bay
model with spatial dependence; in this model, the microplastic abun
dance was high in the eastern tidal flat section (outlet), but low in the
In all microplastics in sediments and organisms, all microplastic in
western tidal flat section (inlet) (see Fig. 2b). Annex Fig. S7 shows the
dicators, except for color, were correlated in the same environment
semi-variance model of microplastic abundance.
(Fig. 4). Sediments were significantly correlated with microplastic type
within organisms in both the tidal flats and in the overall environment
3.3. Characteristics of microplastic contamination in organisms in (P = 0.041 < 0.05; P = 0.041 < 0.05). However, the polymer types in
Hangzhou Bay the marine and tidal flat environments were significantly and highly
correlated with microplastic polymer types in organisms (P = 0.010 <
Table 2 summarizes the overall microplastic abundance in organisms 0.05; P = 0.001 < 0.01, respectively). Regardless of the environment,
in Hangzhou Bay, which ranged from 0.04 to 2.71 items/g and from 0.08 size was highly significantly correlated within both sediments and or
to 2.50 items/individual, with average abundances of 0.70 items/g and ganisms (P = 0.001 < 0.01; P = 0.005 < 0.01; P = 0.001 < 0.01). A
0.92 items/individual, respectively. The most common type of relationship between the microplastic characteristics (type, size, and
polymer type) in the organism and those in the environmental media
was confirmed.
4. Discussion
The type, color, and size of microplastics change over time due to the
physical, chemical, and biological effects of microplastics in the envi
ronment. The sources of microplastics in the natural environment
cannot be traced by fluorescent labeling. Only the polymer type of
microplastics remains the same over time; therefore, polymer type is the
best indicator for microplastic source inference or destination analysis.
In total, 17 different microplastic polymer types were detected in
sediments and 11 were detected in organisms. Excluding the over
lapping polymer types, 21 different microplastic types were detected in
sediments and organisms combined (Table S2). A comparison of the
proportion of microplastic polymer types in sediments and organisms
from the same environment (marine, tidal flats, and overall environ
ment) revealed a significant correlation between microplastics in or
ganisms and those in sediments in marine and tidal flat environments.
Likewise, the types of microplastic polymers and number of microplastic
samples indicate that the main polymer types and number of samples in
sediments and organisms from the same environment are consistent,
excluding the singleton (those only occurring once) polymers. Thus,
polymer type is the best tracer of the source and transfer of microplastics
in the natural environment among the various characteristics of
microplastics.
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X. Cai et al. Journal of Hazardous Materials 457 (2023) 131838
Table 2
Microplastic contamination in organisms in various environmental media.
Source Range of abundance Average abundance Main types Main colors Main size scale Main
(μm) polymers
items/g items/ items/g items/
individual individual
Marine 0.04–2.71 0.08–2.50 0.62 0.91 ± 0.37 Fiber (98.04) Black (54.90) 1–1000 (54.90) PL (33.33)
± 0.42 Blue (25.49) 1001–2000 (27.45) CE (21.57)
Exopalaemon modestus 0.00–20.00 0.00–3.00 2.71 0.50 ± 0.29 Fiber (83.33) Black (33.33) 1–1000 (66.67) PL (33.33)
± 1.88 Blue (50.00) PET (33.33)
Portunus trituberculatus 0.00–0.42 0.00–1.00 0.04 0.08 ± 0.08 Fiber Blue (100.00) 1–1000 (100.00) PVT (100.00)
± 0.04 (100.00)
Uroteuthis edulis 0.00–0.20 0.00–3.00 0.06 1.33 ± 0.49 Fiber Blue (50.00) 1–1000 (50.00) CE (37.50)
± 0.03 (100.00) 1001–2000 (37.50) PET (37.50)
Harpadon nehereus 0.00–2.06 0.00–3.00 0.51 1.50 ± 0.56 Fiber Black (4.44) 1–1000 (44.44) PL (44.44)
± 0.32 (100.00) Grey (33.33) 1001–2000 (33.33) PET (33.33)
Pampus argenteus 0.00–0.46 0.00–4.00 0.22 2.50 ± 0.56 Fiber Black (80.00) 1–1000 (66.67) CE (26.67)
± 0.09 (100.00) 1001–2000 (26.67) PET (40.00)
Larimichthys polyactis 0.00–0.45 0.00–4.00 0.19 2.00 ± 0.58 Fiber Black (66.67) 1–1000 (41.67) PL (25.00)
± 0.07 (100.00) 1001–2000 (25.00) PET (41.67)
2001–3000 (25.00)
Tidal flat 0.08–1.89 0.33–1.67 0.60 0.83 ± 0.16 Fiber (97.83) Black (41.30) 1–1000 (54.35) RY (45.65)
± 0.23 Blue (43.48) 1001–2000 (34.78) CE (26.09)
Bullacta exarata 0.00–4.17 0.00–4.00 0.70 0.83 ± 0.27 Fiber (93.33) Blue (53.33) 1–1000 (40.00) RY (33.33)
± 0.29 1001–2000 (46.67) CE (46.67)
Cerithidea largillierti 0.00–1.93 0.00–5.00 0.70 1.67 ± 0.80 Fiber Black (50.00) 1–1000 (60.00) RY (90.00)
± 0.32 (100.00) Blue (50.00) 1001–2000 (30.00)
Mactra veneriformis 0.00–1.11 0.00–3.00 0.30 0.83 ± 0.48 Fiber Black (40.00) 1–1000 (80.00) PET (40.00)
± 0.18 (100.00) Blue (40.00) CE (40.00)
Sinonovacula constricta 0.00–0.22 0.00–2.00 0.08 0.67 ± 0.33 Fiber Black (75.00) 1–1000 (25.00) RY (25.00)
± 0.04 (100.00) 1001–2000 (25.00) PET (25.00)
Chinomantes dehaani 0.00–1.09 0.00–2.00 0.28 0.50 ± 0.34 Fiber Black (33.33) 1–1000 (100.00) RY (33.33)
± 0.19 (100.00) Grey (33.33) PET (33.33)
Transparency
(33.33)
Scylla serrata 0.00–1.01 0.00–1.00 0.24 0.33 ± 0.17 Fiber Black (67.67) 1–1000 (66.67) RY (33.33)
± 0.14 (100.00) CE (33.33)
Boleophthalmus 0.00–8.00 0.00–2.00 1.89 1.00 ± 0.37 Fiber Black (33.33) 1–1000 (50.00) RY (50.00)
pectinirostris ± 1.28 (100.00) Blue (50.00) 1001–2000 (50.00) CE (33.33)
Total 0.04–2.71 0.08–2.50 0.70 0.92 ± 0.12 Fiber (97.94) Black (48.45) 1–1000 (54.64) RY (27.84)
± 0.24 Blue (34.02) 1001–2000 (30.93) CE (23.71)
PL (20.62)
Note: The value in brackets is the percentage of each factor in the total number (%).
discrepancy is because Chongming Island is part of Shanghai. Although standardization in microplastic research to facilitate more accurate
both sites are estuaries along the East China Sea, Chongming Island has comparisons and to improve our understanding of the true extent of
more industrial plants and a greater amount of ship traffic, resulting in a microplastic contamination.
greater number microplastics entering the ocean and thus depositing in The microplastic abundances in two bivalves in this study were
the sediments. The average microplastic abundance in the marine sed similar to those measured in Crassostrea gigas and Mytilus edulis (see
iments of Hangzhou Bay was lower than that measured in other bays and Table 4), and the microplastic abundance by weight was significantly
estuaries (see Table 3). The average microplastic abundance in the tidal higher in the Palaemon modestus than those in other similar shrimp
flat sediments of Hangzhou Bay was lower than that in the tidal flat species. Daniel et al. suggested that the microplastic abundance of Por
sediments of other bays (see Table 3). The microplastic abundance in the tunus pelagicus in the distant sea was the same as that of Portunus tritu
tidal flat sediments of the bay may be closely related to the microplastic berculatus in this study; both had very low values [46]. The microplastic
abundance in marine sediments (Table 3). abundance by weight was extremely low for all mollusks, and the
In interpreting the results of this study, it is essential to consider the microplastic abundance by individual was greater, probably due to the
influence of methodological choices on observed microplastic abun large specific surface area and body weight of mollusks. Similar to other
dance. Specifically, the use of different floating solutions and sampling fishes, the microplastic abundance by individual was greater than the
depths across studies can introduce variability that might confound abundance by weight for the four species in this study.
comparisons. For instance, different floating solutions, such as NaI, The Xiangshan Bay studied by Wu et al. is close to Hangzhou Bay, but
ZnCl2, and Saturated NaCl, have varying densities, which could poten the marine organisms studied are all commercially important species
tially affect the buoyancy of microplastics and therefore the detection cultured in aquaculture factories in Xiangshan Bay [7], and all the
efficiency [42,43]. Moreover, sediment sampling depths, which ranged commercially important marine species studied here were native spe
from 1 cm to 30 cm in the cited studies, might influence microplastic cies. Because of the frequent interference of human activities, artificial
abundance estimates due to potential stratification of microplastics breeding organisms can be regarded as having great differences
within sediment layers [44,45]. In shallow sampling depths (e.g., 1 cm), compared with those in natural environment. The results of Wu et al.
microplastics might be overrepresented due to their potential to be showed that microplastic bioaccumulation was more likely to occur in
preferentially deposited on the surface layers through low-density or aquaculture organisms than in organisms in natural environments,
secondary microplastics from the degradation of larger plastic debris which is consistent with the observation that there was no significant
[44]. On the other hand, deeper sediment layers (e.g., 30 cm) may correlation between microplastic abundance and trophic level in natural
contain older microplastics, which have been buried over time [45]. The aquatic economic species in this study.
heterogeneity of methods used across studies underscores the need for There are many large bay areas around the world, such as the New
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X. Cai et al. Journal of Hazardous Materials 457 (2023) 131838
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X. Cai et al. Journal of Hazardous Materials 457 (2023) 131838
Table 3
Characteristics of microplastic contamination in sediments in several offshore areas in China.
Study area Abundance (items/ Main Main Sample depth Sampling instrument Flotation solution References
kg) polymer type (cm)
Marine sediment
Xiangshan Bay, China 73.94 ± 30.43 RY, PP, PA Fiber 5 Van Veen garb Saturated NaCl [7]
sampler
Yangtze Estuary, China 121.00 ± 9.00 RY, PL, AA Fiber 5–10 / Saturated NaCl [28]
Bohai Sea offshore, China 171.80 ± 55.40 RY, PE, PET Fiber / Stainless steel box Saturated NaCl [30]
sampler
Northern Yellow Sea offshore, China 123.60 ± 71.60 RY, PE, PET Fiber / Stainless steel box Saturated NaCl [30]
sampler
Southern Yellow Sea offshore, China 72.00 ± 27.20 RY, PE, PET Fiber / Stainless steel box Saturated NaCl [30]
sampler
Haizhou Bay, China 330.00 ± 260.00 RY, PET, PP Fiber / Grapple bucket Saturated NaCl [31]
Hangzhou Bay, China 13.16 ± 1.82 PL, CE, RY Fiber 5 Van Veen garb Saturated NaCl This study
sampler
Chao Phraya River Estuary, Thailand 39.00 ± 14.00 PE, PP / / Van Veen garb NaI [32]
sampler
Tampa Bay, America 280.00 ± 290.00 / Fiber / Van Dorn sampler NaI [33]
Belgian coast, Belgium 390.00 PP, PA Fiber / Van Veen garb Concentrated saline [34]
sampler solution
Tidal flat sediment
Beach sand of South China Sea, China 5014.00–8714.00 HDPE, PET, Fiber 1 Watch glass Saturated NaCl [35]
PE
Beach sand of Northeastern coast of 6080.00 HDPE, PET, Fiber 1 Watch glass Saturated NaCl [35]
Beibu Gulf, China PE
Beach sand of Bohai Sea, China 102.90–163.30 PE, LDPE, Fragment 2–20 Metal ring Saturated NaCl [36]
HDPE
Tidal zone of Haizhou Bay, China 490.00 ± 170.00 PE, PET, PS Fiber 30 Quantitative sampling Saturated NaCl [9]
frame
Beaches of Xiamen Bay, China 148.27 PE, PS Fragment 2–3 Stainless steel1 shovel Saturated NaCl [37]
Tidal flat of Zhanjiang Bay, China 61.00–989.00 items/ PP Fragment 2 / Saturated NaCl [38]
m2
Hangzhou Bay, China 18.63 ± 2.62 PET, PL, Fiber 5 Stainless steel1 shovel Saturated NaCl This study
PP+PE
Kayamkulam estuary, India 433.30 PP Fiber / Van Veen garb ZnCl2 [39]
sampler
Vitória bay estuarine system, Brazil 0–126.67 / Fiber / Van Veen garb Saturated NaCl [40]
sampler
Gulf of Thailand, Thailand 150.40 ± 86.20 RY, PL Fiber 5 Stainless steel box Saturated NaCl [41]
sampler
conduct full coverage of solid waste classification, collection, and subjected to physical, chemical, and biological effects that will gradually
transportation to improve the utilization rate of resources and develop degrade them resulting in microplastics smaller than 2 mm accumu
low-impact treatment methods and standardized management pro lating in the Hangzhou Bay.
tocols, which results in the relative low abundance of debris and film in The distribution of microplastics in both marine and tidal flat sedi
sediments of Hangzhou Bay. Regardless, many polymer fibers are too ments in Hangzhou Bay is spatially dependent. Among benthic sampling
small to be completely filtered and recycled, leading to RY, CE, and PL sites, M10, M8, and M5 sites are far from the coast and microplastics
sediment accumulation, which become the main polymer components of easily deposit under the action of Lagrange circulation and the net water
Hangzhou Bay microplastic pollution. transport field [59,60], which increases the concentration of micro
Microplastics were detected in many of the organisms that we plastics significantly. In contrast, although the sites of M1, M3, M7, and
examined that are also commonly consumed by people. Although most M12 are close to the coast, due to the effect of tides and the channel
microplastics are removed through gutting inedible internal organs and dredging of Hangzhou Bay in the shipping channel, microplastics are not
cleaning, microplastics are still present in the remaining edible flesh. easily deposited and the concentration of microplastics is reduced. The
This consumption includes the microplastics and their adsorbed chem concentration of microplastics in tidal flat sediments increased slightly
icals and the resulting marine food safety issues and risks to human from T1 to T2, and then gradually increased to T5 (Fig. S4). On con
health require further study. struction land, T4 and T5 experienced a gradual increase of micro
plastics due to the intensity of human activities, resulting in a very high
concentration.
4.4. Characteristics of microplastic pollution in tidal flat ecosystem of In this study, microplastic pollution was detected in all organisms in
Hangzhou Bay Hangzhou Bay. Per weight, E. modestus and B. pectinirostris had the
highest abundance of microplastics (Fig. S5), both of which are
The overall abundance of microplastics in the sediments of Hang omnivorous animals and prefer to inhabit estuarine shoals [61]. Inci
zhou Bay ranged from 3.32 to 35.12 items/kg, but the main types (fiber), dentally, the shoal sediments of Hangzhou Bay had a higher abundance
colors (black), and sizes (1–1000 μm, 1001–2000 μm) of microplastics of microplastics than those of marine sediments. When counted by in
were consistent in all environmental media. The predominant type was dividuals, the abundance of microplastics in P. argenteus and L. poly
fiber, was is consistent with the results of sediment microplastic pollu actis were the highest recorded (Fig. S5). Compared with other
tion in other bays or estuaries around the world (see Table 3). The area organisms in this study, these two species had the highest trophic level
of Hangzhou Bay is large and after entering the marine environment, and largest body sizes. Furthermore, the adults feed on low-trophic or
microplastics can be transported for a long distances due to ocean cur ganisms such as jellyfish, benthic animals, and small fish [61], leading to
rents and winds. In the process of transportation, microplastics are also
8
X. Cai et al. Journal of Hazardous Materials 457 (2023) 131838
Table 4
Characteristics of microplastic contamination in several marine organisms.
Species Site Abundance Main Type References
Bivalve, Snail
Ostrea denselamellosa Xiangshan Bay 0.31 ± 0.10 1.67 ± 0.44 Fiber [7]
Sinonovacula constricta Xiangshan Bay 0.21 ± 0.05 1.80 ± 0.34 Fiber [7]
Mytilus edulis A mussel farm in Germany 0.36 ± 0.07 / / [47]
Crassostrea gigas Purchase from supermarket 0.47 ± 0.16 / / [47]
Modiolus modiolus Coast of Scotland 0.086 ± 0.031 3.50 ± 1.29 Fiber [48]
Bullacta exarata Hangzhou Bay 0.70 ± 0.29 0.83 ± 0.27 Fiber This study
Cerithidea largillierti Hangzhou Bay 0.70 ± 0.32 1.67 ± 0.80 Fiber This study
Mactra veneriformis Hangzhou Bay 0.30 ± 0.18 0.83 ± 0.48 Fiber This study
Sinonovacula constricta Hangzhou Bay 0.08 ± 0.04 0.67 ± 0.33 Fiber This study
Shrimp
Parapenaeopsis hardwickii Xiangshan Bay 0.25 ± 0.08 0.95 ± 0.28 Fiber [7]
Lysmata vittata Xiangshan Bay / 0.30 ± 0.50 Fiber [49]
Exopalaemon modestus Hangzhou Bay 2.71 ± 1.88 0.50 ± 0.29 Fiber This study
Crab
Portunus pelagicus fishing harbors of India 0.003 ± 0.01 0.14 ± 0.44 Fragment [46]
Coastal sea crab Zhoushan 2.37 ± 0.41 / Fiber [50]
Chinomantes dehaani Hangzhou Bay 0.28 ± 0.19 0.50 ± 0.34 Fiber This study
Scylla serrata Hangzhou Bay 0.24 ± 0.14 0.33 ± 0.17 Fiber This study
Portunus trituberculatus Hangzhou Bay 0.04 ± 0.04 0.08 ± 0.08 Fiber This study
Mollusc
Sepia officinalis Marine station, Portugal / 39.00 Fiber [51]
Uroteuthis (Photololigo) duvaucelii fishing harbors of Kerala, India 0.008 ± 0.02 0.18 ± 0.48 Fragment [46]
Dosidicus gigas The coast of Peru 0.625 5.950 Fiber [52]
Uroteuthis edulis Hangzhou Bay 0.06 ± 0.03 1.33 ± 0.49 Fiber This study
Fish
Konosirus punctatus Xiangshan Bay 0.044 ± 0.025 2.1 ± 0.38 Fiber [7]
Larimichthys crocea Xiangshan Bay 0.008 ± 0.006 1.80 ± 0.42 Fiber [7]
Myctophum aurolanternatum North Pacific / 6.00 ± 8.99 Fragment [53]
Central Gyre
Cololabis saira North Pacific / 3.20 ± 3.05 Fragment [53]
Central Gyre
Planktivorous fish Tokyo Bay / 2.30 ± 2.50 Fragment [54]
Boleophthalmus pectinirostris Hangzhou Bay 1.89 ± 1.28 1.00 ± 0.37 Fiber This study
Harpadon nehereus Hangzhou Bay 0.51 ± 0.32 1.50 ± 0.56 Fiber This study
Pampus argenteus Hangzhou Bay 0.22 ± 0.09 2.50 ± 0.56 Fiber This study
Larimichthys polyactis Hangzhou Bay 0.19 ± 0.07 2.00 ± 0.58 Fiber This study
microplastic bioaccumulation. Hypothetically, microplastics pass Exopalaemon modestus are shrimp, Chinomantes dehaani, Scylla serrata,
through the food web and accumulate in higher level trophic organisms. and Portunus trituberculatus are crabs, Bullacta exarata, Cerithidea largil
However, we observed no significant correlation between the abun lierti, Mactra veneriformis, Sinonovacula constricta and Uroteuthis edulis
dance of microplastics in organisms and trophic level (Fig. 3). This un are mollusks. Based on the results of this study, it can be inferred that in
expected finding may be related to the large species differences among 2020, the total amount of these five types of marine economic species
organisms in this study. In the future, more similar species groupings caught in Zhejiang province could accumulate about 2.23 G t of
should be selected for analysis. microplastic particles. Thus, the potential risks to human health caused
by microplastic pollution of marine organisms cannot be ignored.
4.5. Risk prediction of microplastic pollution in marine organisms in
Hangzhou Bay 3. Outlook and conclusion
In 2020, China’s total marine fishery output reached 10.94 M t, This study confirmed the existence of high microplastic pollution in
among which Zhejiang province, where Hangzhou Bay is located, had a marine sediments, tidal flat sediments, and 13 commercially important
marine fishery output of 2.57 M t, ranking first in China [62]. China is species in the Hangzhou Bay. However, the marine ecosystem of
bordered by the Bohai Sea, the Yellow Sea, the East China Sea, and the Hangzhou Bay is not only composed of sediments and organisms, and
South China Sea. Hangzhou Bay is the mouth of the Yangtze River the 13 aquatic economic species cannot fully represent the marine or
entrance into the East China Sea. The total output of marine fisheries in ganisms and complex food web of Hangzhou Bay. As such, the existing
2020 in the East China Sea was 3.81 M t, while Zhejiang’s marine research results have not been able to provide a detailed answer to the
fishery output in the East China Sea was 2.39 M t, the largest in China. In various microplastics pollution problems in the marine ecosystem of
2020, aquatic products in Zhejiang province were exported as a total of Hangzhou Bay and its marine organisms. Future studies should be
172.76 M USD and 0.44 M t, mostly to the United States, the European further conducted considering the following aspects: (1) How micro
Union, the Russian Federation, South Korea, Japan, Thailand, and other plastics get transferred in the marine environment; (2) Quantitative
countries and regions. Therefore, distribution of microplastic contami tracing analysis of microplastics to assess the range of microplastic types
nants in seafood from Zhejiang may impact global trading partners. and accumulation in marine ecosystems.
In 2020, 1.72 M t of fish, 0.50 M t of shrimp, 0.18 M t of crabs, 20.50 High microplastic contamination was found in the tidal flats and
k t of shellfish and 0.13 M t of cephalopods were caught in the waters off organisms in Hangzhou Bay (average abundance of sediments: 16.85
Zhejiang province [62]. Among the representative marine economic ± 1.92 items/kg; average abundance of organisms: 0.70 ± 0.24 items/g,
species selected in this study, Boleophthalmus pectinirostris, Harpadon 0.92 ± 0.12 items/individual), and several microplastic characteristics
nehereus, Pampus argenteus, and Larimichthys polyactis are fish, in sediments and organisms were correlated in the same environment
9
X. Cai et al. Journal of Hazardous Materials 457 (2023) 131838
(type, size, and polymer type), confirming the link between microplastic Appendix A. Supporting information
contamination in organisms and the environment. Furthermore, we
found (1) spatial autocorrelation in the distribution of microplastic Supplementary data associated with this article can be found in the
abundances in marine and tidal flat sediments in Hangzhou Bay, but no online version at doi:10.1016/j.jhazmat.2023.131838.
spatial autocorrelation in the offshore tidal flat environment as a whole.
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