Accepted Manuscript

Assessment of microplastics derived from mariculture in Xiangshan Bay, China

Minglong Chen, Meng Jin, Peiran Tao, Zheng Wang, Weiping Xie, Xubiao Yu, Kan
Wang

PII: S0269-7491(18)32247-4
DOI: 10.1016/j.envpol.2018.07.133
Reference: ENPO 11437

To appear in: Environmental Pollution

Received Date: 19 May 2018

Revised Date: 13 July 2018
Accepted Date: 31 July 2018

Please cite this article as: Chen, M., Jin, M., Tao, P., Wang, Z., Xie, W., Yu, X., Wang, K., Assessment
of microplastics derived from mariculture in Xiangshan Bay, China, Environmental Pollution (2018), doi:
10.1016/j.envpol.2018.07.133.

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1 Assessment of microplastics derived from mariculture in Xiangshan Bay,

2 China

3 Minglong Chen1, Meng Jin1, Peiran Tao1, Zheng Wang1, Weiping Xie2, Xubiao Yu1*, Kan Wang1

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Faculty of Architectural, Civil Engineering and Environment, Ningbo University, Ningbo, Zhejiang,

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7 315211, PR China
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Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo,

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10 Zhejiang, 315211, PR China
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14 *: Corresponding Author

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16 Email: yuxubiao@nbu.edu.cn (X. Yu)

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17 Mailing Address: 818 Fenghua Rd., Jiangbei District, Ningbo 315211, China
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27 Assessment of microplastics derived from mariculture in Xiangshan Bay, China

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28 Abstract

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Mariculture activities including enclosure, raft and cage cultures employ a variety of plastic gear

30 such as fishing nets, buoyant material and net cages. The plastic gear poses a potential source of

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31 microplastics to the coastal environment, but relevant data on the impacts of mariculture are still

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32 limited. To this end, a semi-enclosed narrow bay (i.e., Xiangshan Bay, China) with a long-term
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33 mariculture history was investigated to assess how mariculture activities affect microplastics in

34 seawater and sediment. The results indicated that mariculture-derived microplastics accounted for
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35 approximately 55.7% and 36.8% of the microplastics in seawater and sediment, respectively. The
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36 average microplastic abundances of seawater and sediment were 8.9±4.7 (mean±SD, n=18)
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37 items/m3 seawater and 1739±2153 (n=18) items/kg sediment, respectively. The types of

38 mariculture-derived microplastics included polyethylene (PE) foam, PE nets, PE film,

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39 polypropylene (PP) rope, polystyrene (PS) foam and rubber. PE foam had the highest proportion
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40 (38.6%) in the seawater samples. High usage rates and the porous structure of PE foam led to the
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41 high abundance. The average microplastic sizes of seawater and sediment are 1.54±1.53 mm and

42 1.33±1.69 mm, respectively. The spatial variations in the abundance and size of microplastics

43 implied that the mariculture-derived microplastics in Xiangshan Bay were transported along the

44 Bay to the open sea. The results of this study indicate that mariculture activity can be a significant

45 source of microplastics. Further research is required to investigate how the high microplastic

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46 abundance in mariculture zone affects marine organisms, especially cultured seafood.

47 Keywords: marine debris, nearshore, coastal water, sediment, pollution

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49 Capsule:

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Results of this work imply that the long-term intensive mariculture activities have caused a

51 significant microplastic issue for Xiangshan Bay, China.

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67 1 Introduction

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The environmental issue of marine microplastics has attracted great concern due to extensive

69 distribution (Cole et al. 2011) and potential risks for marine organisms (Wright et al. 2013). The

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70 ingestion and bioaccumulation of microplastics by wild (Li et al. 2016) (Li et al. 2018) and

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71 laboratorial (Cole et al. 2013) marine organisms has been observed, and the toxicological effects of
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72 microplastics have been reported (Jin et al. 2018, Lei et al. 2018). As marine organisms serve as

73 important protein and nutrition sources for humans, social concerns have been increasingly raised
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74 on the potential health risks of microplastics for seafood consumers (Carbery et al. 2018, Rist et al.
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75 2018). Mariculture has become an important and resource-efficient way to provide seafood globally
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76 (Bouwman et al. 2013). Of the total global seafood produced in 2014, approximately one quarter

77 was provided by mariculture (FAO, 2016). In mariculture production, plastic gear such as fishing
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78 nets, buoyant material and net cages are necessary materials. Under long-term sunlight
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79 decomposition and wind/wave friction (Song et al. 2017), these materials could be a considerable
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80 source of microplastics being released into local seawater. Thus, cultured seafood might be more

81 vulnerable to microplastics than wild-caught seafood. However, current assessment data on the

82 contribution of microplastics to mariculture are still limited.

83 China represents over 60 percent of the world’s aquaculture production (FAO, 2016), and its

84 mariculture industry has experienced rapid growth due to a substantial domestic demand (Feng et al.
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85 2004). Since the mid-1990s, mariculture production in China has undergone a rapid expansion to

86 exceed the production of wild capture fisheries (Liu and Su 2017). In 2013, the ratio between

87 mariculture production and wild capture reached 140%, which is much higher than that of Europe

88 (18%) and other continents (<15%) (Liu and Su 2017). With rapid mariculture expansion, a series

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89 of environmental issues have been frequently reported, such as: harmful algal blooms (HABs) (Li et

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al. 2017a, Liu and Su 2017), organic contaminants (Cheng et al. 2018, Wang et al. 2014, Zong et al.

91 2014), heavy metals (Liang et al. 2016, Liang et al. 2011), antibiotic resistance genes (Gao et al.

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92 2018, Zhao et al. 2017) and changing bacterial communities (Li et al. 2013) in the mariculture

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93 zones in China. As emerging marine pollutants, microplastics have been detected in the nearshore
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94 and offshore environments along China’s coastline (Qiu et al. 2015, Tang et al. 2018, Tsang et al.

95 2017b, Zhao et al. 2014b) in the past three years. However, no studies have yet assessed
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96 mariculture-derived microplastic pollution in China.

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97 To assess the impacts of mariculture activities on the abundance and distribution of microplastics in
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98 a coastal environment, Xiangshan Bay, a southeastern Chinese bay in Zhejiang Province, was
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99 investigated. Due to long-term intensive mariculture production, Xiangshan Bay has been reported

100 to have many pollution issues (Jiang et al. 2013, Li et al. 2012, Wang et al. 2015, Yang et al. 2011,
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101 Zhou et al. 2014). It is a semi-enclosed narrow bay, and the wind and waves in the bay are weak (Li
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102 et al. 2017b). Regarding the aspect of microplastic transport, the weak wind and wave action might

103 lead to a high accumulation of microplastics in the bay (Iwasaki et al. 2017, Kukulka et al. 2012).

104 Thus, Xiangshan Bay is an ideal mariculture zone for studying microplastic pollution. The

105 abundance and composition of microplastics in the seawater and sediment samples of Xiangshan

106 Bay were analyzed. Samples of the main mariculture gear used in Xiangshan Bay were also
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107 collected and characterized to clarify the contribution of microplastics to mariculture activities.

108 2 Materials and methods

109 2.1 Fundamentals of Xiangshan Bay and mariculture

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110 Xiangshan Bay is located on the coast of Zhejiang Province in southeastern China (Fig. 1). The Bay

111 has a length of approximately 70 km (from the mouth to the upper head), but the average width is

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112 only approximately 10 km (Li et al. 2017b). The total area and average depth of Xiangshan Bay are

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113 approximately 560 km2 and 10 m, respectively (Xu et al. 2016). The bay has three branches as

114 shown in Fig. 1, i.e., Tie Bay (Branch 1), Huangdun Bay (Branch 2) and Xihu Bay (Branch 3).

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Xiangshan Bay has very weak waves all year round, and the annual-averaged wave height is only

116 0.4 m in the outer bay (Li et al. 2017b). These geographical and hydrological characteristics make
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117 Xiangshan Bay a favorable area for mariculture activities, which have experienced rapid growth
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118 during the past two decades. The total mariculture area reached ~100 km2 in 2013, accounting for
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119 approximately one sixth of the total area of Xiangshan Bay. The predominant mariculture types in

120 Xiangshan Bay include enclosure cultures for crab farming, raft cultures for oyster and seaweed
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121 farming, cage cultures for fish farming and tidal flat cultures for clam farming. The total production
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122 of farmed seafood in Xiangshan Bay was approximately 1.03×105 t/y in 2013 (Ningbo Government,
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123 2014). The distribution map of mariculture activities is shown in Fig. 1.

124 2.2 Sample collection

125 The sampling events in Xiangshan Bay were conducted in October 2017. The locations of sampled

126 sites are shown in Fig. 1. Surface seawater and sediment samples from Xiangshan Bay were

127 collected. In addition, the plastic samples from mariculture gear such as fishing nets, plastic foam
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128 and plastic film were collected from corresponding farms for identifying the sources of the

129 field-detected microplastics.

130 2.2.1 Surface seawater sampling

131 All surface seawater samples were collected with plankton net tows. Surface seawater samples were

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132 collected from nine sites, as shown in Fig. 1. These sites were distributed from the inner (i.e.,

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133 Branch 1) to the outer areas of the Bay (i.e., Xiangshan Bay Bridge). Two ring trawl nets (330 µm

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134 mesh and a diameter of 20 cm) were towed at a speed of two knots for 15 min. A flowmeter

135 （Hydro-Bios, Germany）was mounted across the trawl mouth during all deployments to measure

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the volume filtered. After each tow, the nets were rinsed with Milli-Q water (Millipore, France)
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137 from the exterior with a sprayer, and debris in the nets was transferred to a 1 L glass bottle. The nets
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138 were turned over and rinsed again with Milli-Q water before the next sampling. The initial

139 flowmeter reading (V1) and the final reading (V2) values were recorded to calculate the volume
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140 filtered (V = (V2 - V1) × 0.8 m3) by the nets according to the manual for the flowmeter. The
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141 calculated volume was used to calculate the microplastic abundance, i.e., items/m3.
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142 2.2.2 Sediment sampling

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143 Five sites, as shown in Fig. 1, were selected for sediment sampling. One sample (S1) was collected
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144 from the intertidal zone, and four samples (S2-S5) were collected from the benthic sediments. The

145 sediment layers in the middle and outer regions of the Bay are very thin; thus, not enough quantities

146 of sediment were obtained. The sampling method for S1 was similar to previous beach studies (Yu

147 et al. 2016). Briefly, the top layer (depth ~5 cm) of sediment from the intertidal zone was collected

148 with a metal shovel and subsequently transferred into an aluminum foil bag. The sample size was

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149 approximately 2 kilograms. For the benthic sediments, the top layer of sediment was grabbed with

150 an Ekman sampler (Ejer, China). Approximately 2 kilograms of sediment were grabbed and stored

151 in a series of premade aluminum foil bags. A total of 3 sediment samples were collected from each

152 site. The samples were transferred to the laboratory at Ningbo University within 24 h.

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153 2.2.3 Collection of mariculture gear samples

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154 Samples of the primary plastic gear employed by the mariculture farms in Xiangshan Bay were also

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155 collected. Based on our field observations, raft cultures, enclosure cultures and cage cultures were

156 the three major mariculture productions that employed large amounts of plastic gear. A total of six

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mariculture gear types, including PE foam, PE nets, PE film, PP rope, PS foam and rubber tires,
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158 were collected. Detailed information for these mariculture gear types are listed in Table 1, and
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159 photographs are shown in the first row of Fig. 2(a). For cage cultures, we did not obtain sufficient

160 samples of the plastic cages because they were placed underwater at a depth of approximately 1.5
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161 m.
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162 Table 1
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163 2.3 Microplastic isolation and quantification

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164 The microplastics in the seawater and sediments were isolated and quantified in the laboratory at
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165 Ningbo University according to the literature methods. The 1-L seawater sample was first passed

166 through a stainless-steel sieve (with a mesh size of 2 mm). Materials retained on the sieve were

167 examined and sorted by the naked eye, and suspected microplastics were transferred to a petri dish

168 for further examination. Water passed through the sieve was collected in a beaker, and then it was

169 filtrated with GF/B (1.0 µm pore size) filters (Whatman, UK). The beaker was rinsed multiple times
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170 with Milli-Q water to ensure no significant losses through container adhesion. Finally, the filters

171 were air dried and transferred to covered glass dishes.

172 All sediment samples were dried at 50 °C for at least 48 h. A density separation method, as

173 described in Hidalgo-Ruz et al. (2012) and Yu et al. (2016), was employed for isolating

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174 microplastics from the sediment samples. In a shallow aluminum plate (35 cm diameter), 100 g of

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175 dried sediment was mixed with 250 mL of saturated salt solution (ZnCl2 with ρ= 1.75 g/mL) by

176 manually stirring with a glass rod for 2 min. After 2 h of settlement, the water solution above the

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177 sediment layer was carefully transferred to a 500 mL beaker for another hour of settlement. All the

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178 containers (i.e., plates and beakers) were covered by aluminum foil during settlement to reduce the
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179 possibility of airborne contamination. The solution was then filtered through the same glass filter

180 mentioned above. The 500 mL beaker and all the transfer apparatuses were washed with deionized
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181 water multiple times, and all washing solutions were filtered through the same filter to minimize
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182 any sample loss due to adhesion of microplastics on the wall of the filter apparatuses. Filters were
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183 air dried for 24 h and then individually sealed in glass petri dishes for further quantitative and
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184 qualitative analyses. This isolation process was repeated three times for each sample in order to

185 increase recovery. With each set of samples per day, blank controls were run using the above
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186 procedure with only saline solution. No airborne contamination was observed during the test.
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187 The separated particles on the filters were examined using an AM3011 digital microscope

188 (Dino-Lite Digital Microscope, USA) at 20-70x magnification. The entire filters were thoroughly

189 scanned, and a detection range of 0.01-10.0 mm was achieved. Large pieces of vegetable debris

190 such as seaweed and dry leaves were visually sorted out with tweezers.

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191 2.4 Verification and characterization of microplastics

192 The samples of mariculture gear and suspected microplastics were characterized with an FTIR

193 microscope. The FTIR spectra were measured using an Agilent Cary 620 FTIR microscope (Agilent Inc.,

194 USA). An MCT-A detector was used for measurements of the ATR technique with a multicoated,

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195 conical-shaped germanium tip crystal (350 µm spherical finish, single reflection, throughput 450% and

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196 27° average angle). Each spectrum was recorded in the range of 4000-400 cm-1 at a spectral resolution of

197 4 cm-1 and with an average of 64 scans, using KnowItAll software (Bio-Rad Inc., USA). The obtained

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198 spectra were compared with the multiple libraries provided by the Sadtler and Knowitall FTIR library

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199 (Bio-Rad Inc, USA). The scanning electron microscopy (SEM) photographs were captured with a
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200 S-4800 Field Emission Scanning Electron Microscope (Hitachi, Japan).
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201 2.5 Identification of microplastics derived from mariculture activity

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202 To identify the microplastics derived from mariculture activity, the field-collected microplastics were
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203 compared with the six types of mariculture gear (Table 1) by two steps: morphology and chemical

204 comparisons. Morphological comparison was the first step which compared microplastics and
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205 mariculture gear by the characteristics such as color, transparency, shape, size and surface microstructure.
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206 Then, the suspected mariculture-derived microplastics were compared with the corresponding
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207 mariculture gear by FTIR spectrum. The microplastics passed these two steps were identified as

208 mariculture-derived microplastics.2.6 Statistical analysis

209 The microplastic abundance and length data were tested for normality using the Shapiro-Wilk

210 goodness-of-fit test (p > 0.05). Differences in abundance and length among the sites were determined

211 using one-way ANOVA with a Tukey post-hoc test. The difference of length between two samples (e.g.,

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212 the seawater vs sediment samples and PE foam vs other microplastics) was tested by Student's t-Test.

213 The Mann-Whitney U test was used as the nonparametric alternative to the independent-samples t-Test

214 when the assumptions of the independent-samples T-test fail. Statistical analyses were performed by

215 SPSS 19.0 software (IBM Co. Ltd, USA).

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216 3 Results and discussion

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217 3.1 Identification and characterization of microplastics in Xiangshan Bay

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218 Xiangshan Bay has sustained long-term and intensive mariculture production, in which large

219 amounts of plastic gear have been employed. We suspected that these plastic materials could be a

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major source of microplastics in seawater. To verify this theory, the field-collected microplastics

221 were compared with the six types of mariculture gear shown in Table 1 for both morphology and
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222 chemical composition. A visual appearance check is often the first step for identifying microplastics
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223 from non-plastic particles (Hidalgo-Ruz et al. 2012). Fig. 2(a) shows photographs of the detected
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224 microplastics (second and third rows) and their possible sources of origin (first row). Except for the

225 rubber particles, microplastic samples sharing similar morphological characteristics with the
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226 corresponding mariculture gear were all detected in the surface seawater samples. Due to their
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227 relatively high density, the rubber particles were only detected in the sediment samples. PE foams
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228 and PE nets are the two dominant mariculture gear components used in Xiangshan Bay. The

229 microplastics derived from these components can be easily identified by their unique color, texture

230 and size. For example, the diameter of the green PE fibers from fishing nets has an average value of

231 2.2 mm, which is significantly larger than the other fibrous microplastics (less than 0.07 mm). The

232 width of fibrous microplastics reported previously are typically less than 10 µm, such as

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233 microplastics from washing effluent (Frias et al. 2010, Napper and Thompson 2016). For the

234 microplastics from PE film and PP rope, transparency and shape indicate their close ties with the

235 corresponding plastic gear. SEM images further show the surface characteristics of the

236 microplastics. A rough and cracked texture is typical of the morphology of marine microplastics,

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237 reflecting the weathering effects of natural factors.

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238 Fig. 2

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239 To further verify the source of microplastics, the samples were examined by FTIR, and the spectra

240 are shown in Fig. 3(a). The FTIR results indicate high similarities of chemical composition between

241
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the microplastics and the corresponding source plastics. The main polymer absorption band showed
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242 little change, but some surface functional groups showed clear changes. For example, a clear
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243 change was the strengthening of the C-O stretching vibration band, which appeared at the

244 wavenumbers between 1010-1050 cm-1 (Zenkiewicz et al. 2003). This absorption band is closely
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245 related to the surface oxidation extent. Except for the rubber particles, all microplastics in Fig. 3(a)
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246 showed increases of the C-O band, indicating weathering effects. The rubber samples were only
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247 found in sediments, and no significant change of the C-O band was attributed to low sunlight

248 exposure. Combining the morphology and chemical comparisons, clear evidence was found that the
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field-detected microplastics were derived from the mariculture gear.

250 Fig. 3

251 Some microplastics that have no clear relation to the selected mariculture gear were also detected,

252 as shown in Figure 2b. The majority of these microplastics are fibrous, including PP, PET and

253 cellulose. The average diameter of PP fibers is 0.07 mm, while the diameters of PET fibers and

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254 cellulose are even smaller at 0.02 mm. In addition, the SEM image of cellulose fibers shows clear

255 characteristics belonging to viscose fiber, which is a synthetic fabric and is commonly used in

256 dresses, linings, shirts, coats, jackets, and other outerwear (Yu et al. 2016).

257 3.2 Microplastics in seawater

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258 3.2.1 Abundance

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259 The microplastic abundances in surface seawater are shown in Fig. 4(a). The sampled sites have

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260 microplastic abundances that ranged from 4.6±0.5 to 20.1±0.2 (mean±SD, n=2) items/m3 seawater.

261 The total average abundance of the nine sites in Xiangshan bay is 8.9±4.7 (n=18) items/m3 seawater.

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Table 2 compares the abundances of this study with previous international studies. The sampling

263 method employed in this study is comparable to the previous studies. Clearly, the microplastic
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264 abundance in Xiangshan Bay is at a high level. The high microplastic abundance of Xiangshan Bay
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265 could be related to two aspects. First, Xiangshan Bay is characterized by minimal runoff, calm
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266 winds and weak waves throughout the whole year (Li et al. 2017b). Studies have revealed that

267 surface currents and wind waves are the major driving forces in the transport of marine
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268 microplastics (Iwasaki et al. 2017, Kukulka et al. 2012). Thus, the lack of driving forces could lead
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269 to a high accumulation of microplastics in the Bay. Second, the long-term and intensive mariculture
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270 activities could lead to the high abundance of microplastics. The plastic gear on/under the seawater

271 surface could be a continuously releasing source of microplastics.

272 Fig. 4

273 Table 2

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274 Fig. 4(a) also indicates that microplastic abundance has clear variation within the bay. Generally,

275 microplastics exhibit a relatively low abundance in the middle region of the bay (i.e., W3-W6),

276 while the abundances are high at the inner (W1 and W2) and outer (W7, W8 and W9) regions of the

277 bay. ANOVA results indicate that W2 has larger abundance than any other sites (P< 0.005). W1 and

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278 W2 are located in Branch 1, where the most intensive enclosure cultures and raft cultures are

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distributed. In particular, W2 is in the central region of a large oyster culture farm. The high

280 microplastic abundances in W1 and W2 could result from the intensive usage of fishing nets and

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281 buoyant plastics. Compared with W1 and W2, the sites from W3 to W6 are far from the mariculture

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282 farms in Branches 1 and 2. Distance from pollution sources, such as river input (Cai et al. 2018, Yu
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283 et al. 2018) and other point sources (Xiong et al. 2018), is the key factor affecting the distribution of

284 marine microplastics. Surprisingly, the sites in the outermost region, i.e., W7, W8 and W9, show an
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285 increase in microplastic abundance. A possible reason is the fact that Branch 3 has the largest area
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286 of cage cultures (Fig. 1). The plastic debris from the fish cages could contribute a large portion of
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287 microplastics. The distribution pattern of microplastic abundance initially shows the influences of

288 mariculture in the Bay. To further analyze the impacts of mariculture, the compositions of
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289 microplastics from each site are shown in Figure 5.

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290 3.2.2 Composition

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291 The nine sampled sites exhibited significant variation in microplastic composition. A composition

292 map of these sites is provided in Fig. S1. As shown in Fig. 5(a), PE foam-derived microplastic

293 occupies the largest proportion at 38.6%. For the sites from W1 to W5, there is a high proportion of

294 PE foam ranging from 26.3% (W1) to 62.5% (W2). The sites from W6 to W9, however, show

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295 dramatic decreases in the proportion of PE foam, from only 4.7% to 12.5%. This result might imply

296 the spreading action of PE foams from the raft culture area in Branch 1 to outside of the Bay. In

297 addition, W3 shows a higher PE foam abundance than W1. Comparing the distances to the raft

298 cultures, W1 is closer than W3. The higher abundance in W3 might further suggest that transport

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299 towards the outer area of the Bay could be the main direction of PE foam movement. In contrast,

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other types of microplastics account for much smaller proportions than PE foam. The total

301 proportion of PE nets, PE film, PP rope, PS foam, PP nets, nylon and PET is only 28.9%. PE nets

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302 are also widely used in the enclosure cultures of Xiangshan Bay, particularly in Branch 1, but their

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303 proportion is only between 2.7% to 9.3% among all the sites. A major reason for the high
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304 percentage of PE foam could be its structural characteristics. PE foam has more porous structures

305 than other plastics do. As such, PE foam might be more easily broken down into microscopic debris
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306 by sunlight, wind and current erosion. Song et al. compared fragmentation by mechanical abrasion
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307 for three plastic types, i.e., PE, PP and expanded polystyrene (EPS, a foamed polystyrene) (Song et
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308 al. 2017). Their results showed that EPS was more susceptible to frictional forces than PE and PP

309 and can be readily torn apart by friction. Our field data concur with the laboratory data of Song et
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310 al.
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311 Fig. 5
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312 Despite their relatively low abundance, PE net-derived microplastics exhibit a similar spreading

313 pattern to PE foam. Fig. 6 shows a strong linear relationship (R2=0.84, p<0.001) between the

314 abundance of PE foam and PE nets. Branch 1 has the largest enclosure and raft culture areas of

315 Xiangshan Bay, corresponding to the major sources of PE nets and PE foams, respectively. This

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316 result suggest that Branch 1 plays an important role in the contribution of PE foam- and PE

317 net-derived microplastics to the Bay. Moreover, PS foam also exhibited strong linear relationship

318 (see Fig. S2) with PE foam (R2=0.68, p=0.042) and PE nets (R2=0.84, p=0.009), further indicating

319 that mariculture-derived microplastics have similar transfer path within the bay.

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320 Fig. 6

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321 For W7, W8 and W9, a significant increase in the PP net-derived microplastic was observed. The

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322 large area of cage cultures, which employs plastic cages to farm fishes in Branch 3, might be an

323 important source. Surprisingly, in the inner part of the Bay (sites W1 to W6), few PP net-derived

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microplastics were detected. This phenomenon can be attributed to the lower distribution of cage
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325 cultures in the inner bay. When comparing the average abundances, PP nets in the outer sites (W7 to
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326 W9, 45.7±8.3, n=6) have a higher value than the PE nets in the inner sites (W1 to W5, 42.4±28.0,

327 n=10). The higher abundance of PP net-derived microplastic could also be related to material
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328 characteristics. The laboratory data of Song et al. (2017) showed that PP material produced a
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329 number of fragments over 2 orders of magnitude higher than PE material under UV exposure and
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330 mechanical abrasion. The field data from Xiangshan Bay are in accordance with the laboratory data

331 of Song et al.

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332 Synthetic cellulose (Remy et al. 2015) and PET (Browne et al. 2011) fibers are common

333 microplastics from terrestrial sources such as sewage effluent. The average abundance and

334 proportion of synthetic cellulose at the nine sites are 126.9±51.2 (n=18) items/m3 seawater and

335 41.5%±17.3% (n=18), respectively. There is a generally increasing trend of the synthetic cellulose

336 proportion from the inner sites to the outer sites. This could due to the increasing freshwater input

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337 along the bay from west to east. Generally, microplastics derived from mariculture account for

338 ~55.7% of the total sampled sites. For the sites closer to a mariculture farm, the proportion is much

339 higher, e.g., W2 has a proportion of 78.1%. The above data demonstrate that mariculture production

340 was a significant source of microplastics for the seawater in Xiangshan Bay.

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341 3.2.3 Size

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342 The sizes of detected microplastics were measured, and Fig. S3(a) shows the size distribution. The

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343 majority of the microplastics range from 0.25 to 2 mm, and the average length is 1.54±1.53 mm.

344 The inset of Fig. S3(a) shows the size data for each sampling site. The average size of microplastics

345
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exhibits a decreasing trend from W1 to W9. For example, W1-W3 have statistical larger sizes than
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346 the sites of S6, S7 and S9 (ANOVA, p< 0.005). As discussed in 3.2.2, microplastics including PE
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347 foams and PE nets undergo a spreading process from the inner to the outer areas of the Bay. During

348 this movement, the size of microplastic could be reduced due to wind/wave friction. Since PE foam
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349 essentially has a single source (i.e., Branch 1), the sizes of microplastics from W1 to W9 were
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350 analyzed separately to observe the trend. Fig. S3(b) shows a clearly decreasing trend of PE foam
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351 from the inner to the outer regions of the Bay. The average sizes from W2 and W3 are 1.68±1.54

352 and 1.77±1.64 mm, respectively. Statistical test indicates that W2 has significantly larger size than
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353
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W6-W9 (ANOVA, p< 0.05). However, the average sizes of PE foams in W8 and W9 decreased to

354 0.72±0.35 and 0.80±0.76 mm, respectively. The decrease in microplastic size further supports the

355 evidence that microplastics in Xiangshan Bay exhibit movements toward the open sea.

356 3.3 Microplastics in sediments

357 3.3.1 Abundance

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358 In addition to being transported to the open sea, microplastics can enter and accumulate in the

359 sediment of a bay. Previous studies have suggested that marine sediment is a major sink for marine

360 microplastics (Van Cauwenberghe et al. 2013, Woodall et al. 2014). Fig. 4(b) shows the

361 microplastic abundance in five sampled sites. S1 exhibits microplastic abundance at approximately

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362 an order of magnitude higher (i.e., 5570±296 items/kg sediment, ANOVA, p< 0.005) than the other

363

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sites. The large difference between S1 and other sites could be attributed to location. As a

364 beach-like sample, S1 has periodic contact and exchange with the surface seawater; thus,

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365 microplastics in the surface seawater can be retained in the sediments. For sites S2 to S5, the

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366 microplastic abundances ranged from 416.8±70.9 to 985.2±120.2 items/kg sediment. The sediment
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367 microplastic abundances in this study are also compared with other reports, as shown in Table 3.

368 The comparison suggests that the total average abundance of Xiangshan Bay is at a high level. If
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369 site S1 is excluded, the average abundance (781.3±258.3) would be lower but still at a median level
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370 among literature data.

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371 Table 3
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372 Generally, microplastic abundances in sediments show a decreasing trend from the inside to outside

373 of the Bay, which is similar to the trend observed in the surface seawater samples. This trend is
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374
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reasonable because most of the microplastics in sediment likely come from the physical and

375 biological transportation of microplastics in seawater. The results of this study suggest that

376 long-term mariculture development has caused the accumulation of a large amount of microplastics

377 in the sediment of Xiangshan Bay.

378 3.3.2 Composition and size

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379 As shown in Fig 5(b), PE foams and synthetic cellulose fibers are still the predominant

380 microplastics. Compared with water samples, the average proportion of PE foams decreased to

381 20.7±13.6%, whereas synthetic cellulose’s average proportion increased to 56.3±14.5% in the five

382 sites. A high abundance of PE foam still occurred in the sites close to the raft culture area, i.e., S2

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383 (32.7%) and S3 (38.0%), which is in accordance with the results of water samples. Thus, raft

384

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cultures impacted not only seawater but also bottom sediments. Biofouling (Kooi et al. 2017) and

385 ingestion-egestion (Cozar et al. 2014) could be the major factors leading to the sink of low-density

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386 microplastics in sediments. Notably, even though S4 was closer to a raft culture area than S5, S5

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387 shows a higher abundance of PE foam. This result further indicates that PE foam has a movement
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388 direction away from Branch 1. Both the results from seawater and sediment samples demonstrate

389 that the microplastics produced in the inner part of the Bay are transferred to the open sea. The size
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390 distribution of the microplastics detected in the sediment samples is shown in Fig. S4. Compared
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391 with seawater samples (1.53±1.54), microplastics in sediment showed a slightly smaller average
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392 size of 1.33±1.69 mm but there is no statistical difference (p= 0.597, two side t-Test). This kind of

393 decrease could result from the friction during the transportation process.
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394 Conclusion
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395
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The above results imply that the long-term intensive mariculture activities have caused a significant

396 microplastic issue for Xiangshan Bay. Through the comparison of morphology, color and FTIR

397 spectra, the ties between field-detected microplastics and mariculture gear were clarified.

398 Approximately 55.7% and 36.8% of the microplastics in surface seawater and sediment were

399 released from various plastic gear, respectively. Among the microplastics, PE foam exhibited a

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400 significantly higher abundance than the other microplastics. This finding is a strong validation of

401 the previous laboratory result that the porous structure makes PE foam more prone to fragmentation

402 than other plastic types. The microplastic abundances in the Xiangshan Bay environment are at a

403 high level compared to the literature data. The long-term intensive mariculture development and the

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404 weak current in Xiangshan Bay are likely the main reasons. The spatial variations in abundance and

405

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size also indicate that mariculture-derived microplastics undergo a transport process toward the

406 open sea. The high level of microplastics in mariculture farms not only are a considerable

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407 contamination source for the marine environment but also pose a potential risk to cultured seafood

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408 and consumer health. Further studies are required to evaluate the safety of cultured seafood, and
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409 control measures should be taken during mariculture production.

410 Acknowledgement
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411 We thank the editor and the anonymous reviewers for their helpful review comments. This study
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412 was supported by the National Natural Science Foundation of China (No. 41676104), Key Program
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413 of Ningbo Science and Technology Bureau (No. 2015C110001), and the K.C. Wong Magna Fund in
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414 Ningbo University.

415
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416
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Appendix: Supplementary data

417 Supplementary data (Fig. S1-S4) related to this manuscript can be found in the supporting information.

418 Further information regarding microplastic composition map, relationship between PS foam and PE

419 foam and PE nets and the size distribution of the microplastics.

420

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609 Table captions:

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Table 1 The specifics of the mariculture gear collected from farms in Xiangshan Bay
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611 Table 2 Comparison of microplastic abundances in surface seawater between Xiangshan Bay and
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612 the literature data

613 Table 3 Comparison of microplastic abundances in sediments between Xiangshan Bay and the
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614 literature
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633 Table 1 The specifics of the mariculture gear collected from farms in Xiangshan Bay
No. Material Shape Color Deployments
1 PE foam white/black/blue/pink raft cultures
2 PE nets green enclosure cultures
3 PE film semi-transparent multiple deployments
4 PP rope semi-transparent multiple deployments
5 PS foam white raft cultures

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6 Rubber tire black raft cultures
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650 Table 2 Comparison of microplastic abundances in surface seawater between Xiangshan Bay and
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651 the literature data

Trawling parameters
Net mesh Abundance
Location Speed Time References
(µm) (items/m3 water)
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(knots) (minutes)
Black Sea 200 ~2 5 1100±900 (Aytan et al. 2016)
Mediterranean Sea 500 ~2 20 0.15 (de Lucia et al. 2014)
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Hong Kong coast 333 ~2 20 3.973±1.177 (Cheung et al. 2018)

Northeast Pacific 505 1.5-2.0 10 0.004-0.19 (Doyle et al. 2011)
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Seto Inland Sea 335 2–3 10–15 0.39 (Isobe et al. 2014)
East Asian Sea 335 2–3 20 3.7±10.4 (Isobe et al. 2015)
California offshore 333 2-4.5 10 3.92 (Lattin et al. 2004)
Arctic polar 333 1.2 20 0.34±0.31 (Lusher et al. 2015)
Bohai Sea, China 333 1.5-2.0 15 0.167±0.138 (Zhang et al. 2017)
East China Sea 333 1.75-2.45 25-30 0.33±0.36 (Zhao et al. 2014a)
Xiangshan Bay 333 ~2 15 8.91±4.70 Present study
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654
655 Table 3 Comparison of microplastic abundances in sediments between Xiangshan Bay and the
656 literature
Isolation parameters Abundance
Location 3
References
Solution Density（g/cm ） (items/kg)
Baltic bottom ZnCl2 1.6 34±10 (Zobkov and Esiukova 2017)
Yangtze River Estuary, China NaCl 1.2 121±9 (Peng et al. 2017)
Deep Bay, Hong Kong NaCl saturated 49-279 (Tsang et al. 2017a)

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South Tuscany, Italy NaCl 1.2 42-1069 (Cannas et al. 2017)
Hong Kong ZnCl2 1.6-1.7 0.58-2216 (Lo et al. 2018)
Rudong Offshore, China NaCl saturated 2580±1140 (Wang et al. 2018)

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West of Svalbard, Norway ZnCl2 1.7-1.8 4356±675 (Bergmann et al. 2017)
Xiangshan Bay, China ZnCl2 1.75 1739±2153 Present study

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657

658 Figure captions:

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Fig. 1 Distribution map of mariculture types and sampling locations of microplastics in Xiangshan
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660 Bay, China.
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661 Fig. 2 Photographs and SEM images of the collected mariculture gear and the field-detected

662 microplastics from Xiangshan Bay. (a) Comparisons between microplastic samples and their
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possible sources of origin: the first row shows types of mariculture gear, and the second and third

664 rows show detected microplastics. (b) The representative detected microplastics that have no clear
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665 relation to the mariculture gear in Xiangshan Bay.

666 Fig. 3 The FTIR spectra of the collected mariculture gear and the field-detected microplastics from
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667 Xiangshan Bay. (a) Comparisons between the microplastic samples and their possible sources of

668 origin. (b) Spectra of the microplastics with no clear sources in Xiangshan Bay.

669 Fig. 4 The abundances of microplastics in the surface seawater (a) and sediment (b) samples in

670 Xiangshan Bay. Error bars indicate standard deviations.

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672 Fig. 5 Chemical compositions of microplastics in the surface seawater (a) and sediment (b) samples

673 from Xiangshan Bay.

674 Fig. 6 Relationship between the microplastic abundance of PE foam and PE nets in the surface

675 seawater samples from Xiangshan Bay.

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715 (a)
716 Rubber tire
PE foam PE net PE film PP rope PS foam
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747 Figure 2 Photographs and SEM images of the collected mariculture gear and the field-detected
748 microplastics from Xiangshan Bay. (a) Comparisons between microplastic samples and their
749 possible sources of origin: the first row shows types of mariculture gear, and the second and third
750 rows show detected microplastics. (b) The representative detected microplastics that have no clear
751 relation to the mariculture gear in Xiangshan Bay.
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758 Mariculture gear Microplastics detected
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799 Figure 3 The FTIR spectra of the collected mariculture gear and the field-detected microplastics
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800 from Xiangshan Bay. (a) Comparisons between the microplastic samples and their possible sources
801 of origin. (b) Spectra of the microplastics with no clear sources in Xiangshan Bay.
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918
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920 Appendix: Supporting Information
921 Assessment of microplastics derived from mariculture in Xiangshan Bay,

922 China

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923 Minglong Chen1, Meng Jin1, Peiran Tao1, Zheng Wang1, Weiping Xie2, Xubiao Yu1*, Kan Wang1

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926 1
Faculty of Architectural, Civil Engineering and Environment, Ningbo University, Ningbo, Zhejiang,

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927 315211, PR China
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Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo,

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933 *: Corresponding Author

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935 Email: yuxubiao@nbu.edu.cn (X. Yu)

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936 Mailing Address: 818 Fenghua Rd., Jiangbei District, Ningbo 315211, China

937 Files in this SI

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938 Fig. S1-S4

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940 Figure captions:

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Figure S1 The composition map of microplastics in the surface seawater of Xiangshan Bay.

942 Figure S2 Relationships between the microplastic abundance of PS foam and PE foam and PE nets

943 in the surface seawater samples from Xiangshan Bay.

944

945 Figure S3 The size distribution of microplastics from the nine sampled sites in Xiangshan Bay: (a)

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946 data for all types of microplastics and (b) data for PE foams. Description of box plots: top and

947 bottom of box = 75th and 25th percentiles, respectively; top and bottom whisker end = 90th and

948 10th percentiles, respectively; top and bottom outlier = maximum and minimum values,

949 respectively; solid line in box = median value; scqure in box = mean value.

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Figure S4 The size distribution of microplastics from the sediments in Xiangshan Bay. Description

952 of box plots: top and bottom of box = 75th and 25th percentiles, respectively; top and bottom

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995 Figure S3 The size distribution of microplastics from the nine sampled sites in Xiangshan Bay: (a)
996 data for all types of microplastics and (b) data for PE foams. Description of box plots: top and

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997 bottom of box = 75th and 25th percentiles, respectively; top and bottom whisker end = 90th and
998 10th percentiles, respectively; top and bottom outlier = maximum and minimum values,
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1026 whisker end = 90th and 10th percentiles, respectively; top and bottom outlier = maximum and
1027 minimum values, respectively; solid line in box = median value; square in box = mean value.
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1 The surface seawater of Xiangshan Bay had 8.9±4.7 (n=18) microplastics per m3 seawater.

2 The sediments of Xiangshan Bay had 1739±2153 (n=18) microplastics per kg sediment.

3 Approximately 55.7% and 36.8% of the seawater and sediment microplastics were from mariculture,

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respectively.

4 The porous structure of PE foam led to high fragmentation.

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5 Mariculture-derived microplastics in Xiangshan Bay were transported to the open sea.

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