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. Author manuscript; available in PMC: 2022 Sep 1.
Published in final edited form as: Chemosphere. 2021 Apr 11;279:130551. doi: 10.1016/j.chemosphere.2021.130551

Quantitative analysis of polyethylene terephthalate and polycarbonate microplastics in freshwater and coastal sediment collected from South Korea, Japan and the USA

Junjie Zhang a,b, Lei Wang b, Kurunthachalam Kannan a,*
PMCID: PMC8205972  NIHMSID: NIHMS1694793  PMID: 33866094

Abstract

Microplastics (MPs) have emerged as contaminants of public health and environmental concern. Although studies have reported the occurrence of MPs in sediment, quantitative determination of polyethylene terephthalate (PET) and polycarbonate (PC) concentrations is limited. In this study, marine coastal and freshwater sediment collected from various locations in South Korea, Japan and the United States were analyzed for PET and PC MPs using a depolymerization method of sample preparation followed by high performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS) detection. PET MPs were found in surface sediments from South Korea (n=20), Japan (n=4) and the United States (n=43) at concentrations (dry weight) in the ranges of <MQL-13,000,000 ng/g (median: 6,600 ng/g), 3,600-5,400 ng/g (4,400 ng/g) and <MQL-10,000 ng/g (<MQL), respectively. Similarly, PC MPs were found in the concentration ranges of <MQL-140,000 ng/g (median: 290 ng/g, South Korea), 150-510 ng/g (100 ng/g, Japan) and <MQL-110,000 ng/g (160 ng/g, the United States). Spatial analysis of concentrations of PET and PC MPs in sediment from Lake Shihwa watershed in South Korea showed a decreasing trend with increasing distance from inland point source areas (Ansan industrial area). No distinct vertical profiles were recorded for PET or PC MPs in sediment cores collected from Tokyo Bay (Japan) or inland lakes in Michigan (the United States). The measured concentrations of MPs in sediment provide baseline data to evaluate future trends and for ecological risk assessment.

Keywords: Microplastics, Polyethylene terephthalate, Polycarbonate, Sediment

1. Introduction

It has been estimated that over 8300 million metric tons of plastics have been produced globally during 1950-2015 (Geyer et al., 2017). Plastics, manufactured from derivatives of petroleum hydrocarbons such as ethylene and propylene, are non-biodegradable and therefore accumulate in landfills or the natural environment (Zubris and Richards, 2005). Of the 6300 million metric tons of plastic waste generated over the past 7 decades, 79% of them were discarded in the open environment (Geyer et al., 2017). It has been projected that by 2050, 12500 million metric tons of plastics would be discarded in the environment (Geyer et al., 2017). Plastic debris occur in all oceans and an estimated 4-12 million metric tons of plastics have reached the marine environment in 2010 alone (Geyer et al., 2017). Approximately 10% of the plastic waste generated so far have entered into the marine environment (Li et al., 2018). Plastics can fragment into millimeter or micrometer size particles from weathering and abiotic transformation over time (Browne et al., 2007). Microplastics (MPs) are plastic particles of <5 mm in size, and have received considerable attention in recent years due to their ubiquitous occurrence in the environment (Sarker et al., 2020; Zhang et al., 2020b; Arthur, 2008). The sources of MPs were small plastics produced for use as ingredients in certain personal care products (primary sources) and those fragmented from large plastics (secondary sources) (Law and Thompson, 2014).

The environmental issue surrounding small plastic particles in oceans was first reported by Carpenter et al (1972). Thompson and coworkers were the first to coin the term "microplastics" (MPs) in 2004. Thus far, studies on MPs have predominantly focused on oceanic environment (Boucher, 2017). MPs have been detected in oceans from around the world (Peeken et al., 2018; Peng et al., 2019). MPs of density greater than seawater are likely to sink and deposit on sediments (Andrady, 2011). High-density MPs such as PET were reported to occur in marine sediments (Wang et al., 2019). Ships, fisheries and other maritime activities were reported to emit ~20% of all MPs in the oceans (Andrady, 2011). Furthermore, MPs discharged from the terrestrial environment account for 80% of the sources. Estuaries are important pathways of MPs to the marine environment (Lebreton et al., 2017).

Polyethylene terephthalate (PET) is the most commonly used polyester and its global production was 53.3 million tons in 2015 (ECI, 2016). The production of polycarbonate (PC) was relatively small (4.4 million tons in 2016), but it is widely used in consumer products (ECI, 2017). The densities of PET (1.37 g/cm3) and PC (1.20-1.22 g/cm3) are greater than that of river and seawater and therefore they are expected to sink in the aquatic ecosystems (Li et al., 2016), and accumulate in benthic environments (Zhang, 2017).

Although there have been several reports of occurrence of MPs in riverine and oceanic sediments, there is still a paucity of information on spatial distribution as well as quantitative analysis of these pollutants. Majority of the earlier studies on MPs in sediments reported numbers, sizes, shapes and types of MPs. In this study, we quantitatively determined the occurrence of PET and PC MPs in surface sediment and sediment cores collected from several locations, including Tokyo Bay (Japan), Ansan industrial complex and Lake Shihwa (South Korea), and inland lakes (Michigan, USA), rivers and coastal areas in the United States using a novel depolymerization method coupled with high performance liquid chromatography–tandem mass spectrometry (Wang et al., 2017) to assess spatial distribution and vertical profiles in sediments.

2. Materials and Methods

2.1. Sample collection

Surface sediments (0–4 cm) were collected, using a stainless-steel box core sampler (40 x 37 x 56 cm), from an artificial saltwater lake, Lake Shihwa, South Korea, in 2008 (n = 20) (Figure S1a). Two sediment cores were collected in April 2012 from Tokyo Bay, Japan (Figure S1b). Sediment cores were sliced at 1-cm increments at the top 4 cm and then at 1.5-cm increments for the remainder of the core. Surface sediment collected using stainless-steel Ponar grab sampler from the Detroit River, Michigan, in 1998 (n = 3) (Kannan et al., 2001), Chesapeake Bay, Virginia, in 2002 (n = 3), several rivers (the Niagara, Oswego, Ashtablua, and Buffalo Rivers) that flow into Lakes Erie and Ontario in 2009 (n = 8), Saginaw River watershed (the Saginaw River, Saginaw Bay, and Tittabawassee River), Michigan, in 2002 and 2004 (n = 10) (Kannan et al., 2008; Yun and Kannan, 2011), and the Hudson River (near Albany), New York, in 2012 (n = 3) were also analyzed. Sediment cores were collected from Gratiot (1999) and Whitmore Lakes (2001) in Michigan (Kannan et al., 2005). Both of these cores were sliced at 0.5-cm intervals at the top 5–8 cm and then at 1-cm intervals for the remainder of the core. The average dates of deposition were estimated using 210Pb and 137Cs profiles (Kannan et al., 2005; Ahrens et al., 2009). Most of the sampling sites were located adjacent to industrialized areas (Figure S1c). All samples were homogenized, freeze-dried, and stored in glass jars at −20° C prior to analysis. Sediment that came into contact with the walls of core samplers were removed prior to transfer into glass jars. Further details of the samples have been reported elsewhere (Kannan et al., 2001; Kannan et al., 2005; Kannan et al., 2008; Ahrens et al., 2009; Yun and Kannan, 2011; Moon et al., 2012b).

2.2. Chemicals and reagents

PET (3-5 mm) and PC (3 mm) particles were purchased from Goodfellow Cambridge Ltd (Huntingdon, England). 1-Pentanol was purchased from Fisher Scientific (Pittsburgh, PA, USA). Terephthalic acid (TPA; >99% purity) was purchased from Toronto Research Chemicals Inc (North York, ON, Canada). D4-TPA (99%) and BPA (>99%) were purchased from Sigma-Aldrich (St. Louis, MO, USA). 13C12-BPA (99%) was purchased from Cambridge Isotope Laboratories (Andover, MA, USA). High-performance liquid chromatography (HPLC) grade methanol and water were supplied by J.T. Baker (Phillipsburg, NJ, USA). Solid-phase extraction (SPE) cartridges (HLB, 200 mg/6 cc) were purchased from Waters (Milford, MA, USA).

2.3. Analysis

Freeze-dried sediment samples were ground and sieved through a 1-mm stainless steel sieve. PET and PC MPs were quantified following depolymerization into their corresponding monomers, TPA and BPA, respectively. Sediment samples were refluxed under alkaline condition for the depolymerization of MPs, as described earlier (Wang et al., 2017). Approximately 0.2 g of sediment (fortified with 500 ng D4-TPA and 200 ng 13C12-BPA) and 0.2 g KOH pellets were taken in a 100 mL round bottom flask that contained 20 mL of 1-pentanol. The mixture was refluxed at 135 °C in a stirring heating mantle (Azzota Scientific SHM-100, Claymont, DE, USA) for 30 min. The pentanol solution, after cooling down to room temperature, was transferred into a 50 mL polypropylene (PP) tube. The flask was rinsed twice with 10 mL of HPLC grade water each time. The water was transferred into the pentanol-containing PP tube. The depolymerized products of PET and PC were extracted from pentanol by shaking in an orbital shaker (Eberbach, Ann Arbor, MI, USA) at 180 strokes per minute for 5 min, which was then centrifuged at 3000 r/min for 5 min (Eppendorf Centrifuge 5804, Hamburg, Germany). The upper organic pentanol phase was transferred into another PP tube, and 20 mL of HPLC grade water was added to repeat the extraction. The aqueous extracts were combined and the volume was made up to 50 mL in HPLC grade water. Ten milliliters of the extracts were purified by SPE, as described earlier (Text S1) (Zhang et al., 2019c).

The quantitative analysis of free TPA and BPA, that may be present in sediment prior to depolymerization, is described in the supporting information (Text S1). The concentrations of free TPA and BPA found in sediments prior to depolymerization were subtracted from values measured post-depolymerization for the calculation of PET and PC MP concentrations.

2.4. Instrumental analysis

A Shimadzu Prominence LC-20 AD HPLC (Shimadzu, Kyoto, Japan) interfaced with an API 3200 electrospray triple quadrupole mass spectrometer (ESI-MS/MS; Sciex, Foster City, CA, USA) was used for the determination of concentrations of TPA and BPA. TPA and BPA were chromatographically separated by the analytical columns, Ultra Biphenyl USP L11 (100 × 2.1 mm, 3 μm; Restek Corporation, Bellefonte, PA, USA) and Betasil® C18 (100 × 2.1 mm, 3 μm; Thermo Electron Corporation, Waltham, MA, USA) connected to a Betasil® C18 Javelin guard column (20 × 2.1 mm), respectively (Table S1). The negative ion multiple reaction monitoring (MRM) mode was used in the identification of target chemicals. Further details of MS/MS parameters are listed in Table S2.

2.5. Quality assurance and quality control (QA/QC)

The depolymerization efficiency of alkaline pentanol was tested by fortifying 0.1 g of pure PET and PC particles in sediment; the recoveries of PET and PC fortified into sediment samples were >95-120%. Round-bottom flasks were muffled at 450 °C for 12 h and rinsed with acetone and methanol prior to use. All experiments were carried out in a fume hood. The recoveries of TPA and BPA in spiked sediment ranged from 92.6±9.2% to 116±2.6% (Table S3).

Procedural blanks were analyzed with every batch of 15 samples, by passing solvents and reagents through the entire analytical procedure including the alkaline depolymerization step. TPA was found in procedural blanks (following depolymermization step), at an average concentration of 850 ng/g (RSD: 11%). Procedural blanks also contained 13 ng/g (RSD: 3.8%) freely available TPA. These results indicated that chemicals and reagents used in the depolymerization step contained remarkable concentrations of TPA. The sources of TPA in procedural blanks were solvents such as 1-pentanol, KOH pellets, and HPLC grade water. Due to the widespread use of PET plastics in various laboratory products, the high background levels of its monomer, TPA, were expected. Therefore, we set our quantification limits above the background levels, to accurately determine the concentrations in samples (Armbruster and Pry, 2008). Background subtraction was performed for TPA in the quantification of concentrations in samples. BPA was not found in any procedural blanks at concentrations above the method quantification limits (MQL). The MQLs, which were calculated from the lowest acceptable calibration standard and a nominal sample weight of 0.2 g, are shown in Table S3. The MQLs of PET (1300 ng/g) and PC (13 ng/g) were calculated from the depolymerization methods of extraction. A midpoint calibration standard was injected after every 20 samples as a check for instrumental drift in sensitivity. A pure solvent was injected into HPLC-MS/MS as a check for carry-over of target chemicals between samples. Instrumental calibration was verified by the injection of standards at concentrations that ranged from 0.2 to 50 ng/mL for BPA and from 0.5 to 200 ng/mL for TPA, and the regression coefficient of the calibration curve (r) was >0.99. For those samples with concentrations above the calibration range, the extracts were diluted and reanalyzed.

2.6. Statistical analysis

The concentrations of PET and PC in sediment were calculated as the difference between depolymerized and free (Cdepolymerization-Cfree) TPA and BPA, divided by 0.90 and 0.86, respectively (Wang et al., 2017). Statistical analyses were performed with GraphPad Prism 8 (GraphPad Software; San Diego, CA, USA) and SPSS 16.0 (IBM; Armonk, NY, USA). Concentrations below the MQLs were substituted with a value equal to MQL divided by the square root of 2, for the calculation of mean. Prior to Pearson correlation analysis and one-way ANOVA, the data were ln-transformed to meet the normality assumptions. The probability value of p≤0.05 was set for statistical significance. All the concentrations are reported on a dry weight basis.

3. Results and Discussion

3.1. PET and PC MPs in surface sediments

Among 20 surface sediment (0-4 cm) samples collected from Lake Shihwa, South Korea, PET and PC MPs were found in 15 sediment samples at a concentration range of <MQL-13000000 ng/g (median: 6600 ng/g) and <MQL-140000 ng/g (290 ng/g), respectively (Table 1). The concentrations of MPs were 4-8 orders of magnitude higher than those of other micropollutants, like polychlorinated dibenzo-p-dioxins, dibenzofurans (0.1-1590 pg/g) (Moon et al., 2012a) and organophosphate flame retardants (2.99-3800 ng/g) (Lee et al., 2018). The concentrations of PET and PC MPs in four surface sediment (0-4 cm) samples from Tokyo Bay, Japan, were 3600-5400 ng/g (median: 4400 ng/g) and 160-510 ng/g (410 ng/g), respectively, which were lower than those found in Lake Shihwa. A study conducted in southern coast of Norway reported the occurrence of PET MPs in 10 surface sediment samples at a concentration range of 120-1365 ng/g, although PC MPs were not detected in those samples (Gomiero et al., 2019). The concentrations measured in Lake Shihwa and Tokyo Bay sediments were higher than those reported from Norway. Sediment collected in Ansan industrial zone in the Lake Shihwa watershed showed elevated concentrations of PET and PC MPs (Figure 1). Approximately 13,000 machinery, electronic/electrical, petrochemical, steel and textile industries are located in this industrial zone (Moon et al., 2012b). PET plastic is mainly used in the production of polyester textile fibers (ECI, 2016) whereas PC plastic is widely used in electronics/electrical applications (ECI, 2017). The proximity of industrial complex explains high concentrations of PET and PC MPs found in surface sediment from Lake Shihwa. A significant positive correlation was found between the concentrations of PET and PC MPs (r=0.993, p=0.000, Figure S2), which suggests the existence of common pollution sources for these two types of plastics. As the distance from the industrial area increased, the concentrations of PET and PC MPs in sediments decreased, and five sediment collected at the farthest distance from the industrial complex, nearby the open waters, did not contain quantifiable levels of MPs. A recent study showed that the number of MPs found in sediments collected near the Chinese coast was 0.20/g, and that number decreased to 0.05/g off the coast (Zhang et al., 2019a).

Table 1.

Concentrations of PET and PC microplastics in surface sediment collected from several locations in South Korea, Japan, and the USA

ng/g TPA PET BPA PC
South Korea n=20 max 1100 13000000 4300 140000
min <MQL <MQL <MQL <MQL
median <MQLs 6550 16 290
DR 45% 75% 80% 75%
Japan n=4 max 32 5400 40 510
min <MQL 3600 23 160
median 19 4400 27 100
DR 75% 100% 100% 100%
USA n=43 max 4600 100000 300 110000
min <MQL <MQL <MQL <MQL
median 16 <MQLs 8.3 160
DR 51 35 65 67
Total n=67 max 4600 13000000 4300 140000
min <MQL <MQL <MQL <MQL
median 16 2200 10 210
DR 51% 51% 72% 72%
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MQL = Method quantification limit; DR = Detection rate

Figure 1.

Figure 1.

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Distribution of PET and PC microplastics in surface sediment collected from Lake Shihwa watershed in South Korea (ng/g, different colors of the inner and outer circles represent different concentrations, gray circles represent non-detects).

Inland freshwater and coastal surface sediments collected from the United States contained PET and PC MPs at concentrations in the range of <MQL-100000 ng/g (median: <MQL) and <MQL-110000 ng/g (160 ng/g), respectively. The wide range of concentrations detected in sediment suggests deposition of MPs in sediments near point source areas (Figure S1c). High concentrations of PET and PC MPs (PET/PC: 63000/5500, 85000/110000, 100000/2500 ng/g) were detected in three Detroit River sediments. The Detroit River watershed encompasses industrial manufacturing sites, waste landfills, and urban runoff, which could explain the presence of elevated concentrations of MPs (Kannan et al., 2001).

3.2. MPs in sediment cores

Sediment cores collected from Tokyo Bay contained PET and PC MPs at concentration ranges of <MQL-8300 ng/g (median: 2700 ng/g) and <MQL-750 ng/g (290 ng/g), respectively. The concentrations of PET MPs in sediment were approximately an order of magnitude higher than those of PC MPs. The concentrations of PET and PC MPs measured in two sediment cores (A and B) were similar. In both cores, PET and PC MPs were not found at concentrations above the MQL in layers corresponding to the years prior to 1980 (Figure 2). Although PET and PC plastics have been produced since the 1940s and 1950s (McIntyre, 2004; Kyriacos, 2017), absence of MPs in deep sediment layers may be an artifact of high MQL (1300 ng/g for PET). Although it was speculated that the concentrations of PET and PC MPs increase with time, such a trend was not discernible in sediment cores. The highest concentration of PET MP (8300 ng/g) was found in 13-14.5 cm section that corresponded to the year 2001, whereas PC MP was found (750 ng/g) in 4-5.5 cm section (corresponded to 2009). A similar pattern was reported for sediment cores collected from the Northwest Pacific Ocean (Xue et al., 2020), in which the number of MPs at a depth of 20-30 cm (1918-1933) was 1200/kg, whereas that in 0-5 cm was (2017) 300/kg. Lack of temporal resolution in MPs distribution in sediment core may suggest bioturbation or other anthropogenic activities. Sandworms (Arenicola marina) have been reported to transport MPs from surface (0-2 cm) to deeper sediment layers (20 cm) (Gebhardt and Forster, 2018). Similar to that found for Tokyo Bay, no distinct pattern in vertical profiles of MP concentrations was found in sediment cores collected from inland lakes in Michigan (Figure S3). Sediment core collected from Gratiot Lake contained PET MPs as high as 42000 ng/g in the surface layer (0.5 cm, corresponded to 1999). PC MPs were also found at the highest concentration (6400 ng/g) in the surface layer (Figure S3). Sediment core collected from Whitmore Lake contained PET and PC MPs at concentrations as high as 17000 and 5000 ng/g, respectively (Figure S3).

Figure 2.

Figure 2.

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Vertical profiles and concentrations of PET and PC microplastics in sediment cores (A and B) collected from Tokyo Bay, Japan.

3.3. Free TPA and BPA in sediment

The concentrations of free TPA (prior to depolymerization) in Lake Shihwa sediment were in the range of <MQL-1100 ng/g (median: <MQL), which were several orders of magnitude lower than those of PET MPs. Free BPA was found at a concentration range of <MQL-4300 ng/g (median: 16 ng/g). The reported concentrations of BPA in sediment from coastal areas of northern China were in the range of <MQL-116 ng/g (Liao et al., 2019). The highest concentrations of TPA and PET MPs were found in the same sediment sample. Similarly, sediments with elevated PC MPs also contained high BPA concentrations. There was a significant positive correlation between the concentrations of TPA and PET MPs as well as between BPA and PC MPs (PET vs.TPA: r=0.963, p=0.000; PC vs. BPA: r=0.976, p=0.000, Figure 3). These results indicate that PET and PC MPs are the sources of TPA and BPA, respectively, in sediments. More than 93% of TPA is used in the production of PET plastic (Markit, 2017), and more than 70% of BPA is used in the production of PC plastic (Groshart et al., 2001). In three sediment samples from Lake Shihwa, the concentrations of TPA were lower than those of BPA (TPA/BPA: 1100/2800, 260/4300, 200/2600 ng/g), suggesting the existence of point sources of BPA in these sampling locations.

Figure 3.

Figure 3.

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Correlation between concentrations of PET and PC microplastics and free TPA and BPA in surface sediment collected from Lake Shihwa, South Korea.

The concentrations of free TPA in sediment core from Tokyo Bay were in the range of <MQL-32 ng/g. BPA was detected in all sediments from Tokyo Bay at a concentration range of 4.6-41 ng/g. The concentrations of free TPA were lower than those of BPA, a pattern similar to that found in surface sediments of Lake Shihwa (Figure S4). The occurrence of TPA and BPA in deep sediment layers suggests vertical migration of these compounds (Diaz-Cruz et al., 2003). In the two sediment core samples, no correlation was found between PET MPs and TPA (core A: r=0.299, p=0.401; core B: r=0.262, p=0.437), whereas a significant correlation was found between PC MPs and BPA (core A: r=0.706, p=0.023; core B: r=0.815, p=0.001). These results suggest the existence of other sources of TPA (besides PET) in Tokyo Bay. TPA is also used as a plasticizer in various products (Wang et al., 2017). The concentrations of BPA in surface sediment were higher than those in deep sediment (Figure S4). The production of BPA has increased annually since the 1950s (Groshart et al 2001). Japan is the top five BPA producers worldwide (Merchant Research & Consulting Ltd., 2013). The high concentration of BPA found in surface sediment from Tokyo Bay can be attributed to ongoing releases of this chemical into the environment.

TPA and BPA were found in freshwater sediments from Michigan, at a concentration in the range of <MQL-4600 ng/g and <MQL-300 ng/g, respectively. The concentrations of free TPA in sediment from Whitmore Lake (<MQL-150 ng/g, median: 33 ng/g) were higher than those in Tokyo Bay (core A: <MQL-30 ng/g, median: <MQL; core B: <MQL-32 ng/g, median: <MQL).

3.4. Comparison of MPs among sediment, indoor dust and sewage sludge

The reported concentrations of PET and PC MPs in sediment, indoor dust (Zhang et al., 2020a) and sewage sludge (Zhang et al., 2019b) from the United States were compared. The reported concentrations of PET MPs in indoor dust were significantly higher than those in sewage sludge (p<0.01, one-way ANOVA) and sediments (p<0.01, one-way ANOVA) (Figure 4a). The concentrations of PET MPs in sewage sludge were significantly higher than those in sediments (p<0.01, one-way ANOVA) (Figure 4a). The concentrations of PC MPs in indoor dust and sludge were similar (Figure 4b), but significantly higher than those in sediments (p<0.01, one-way ANOVA, Figure 4b). These results suggested that indoor environment is an important source of PET MPs. The concentration ratio of PC/PET was the highest in sediments (~10−1), followed by sludge (~10−2), and indoor dust (~10−3) (Figure 4c). An earlier study showed that the concentrations of PET MPs in indoor dust were significantly higher than those in outdoor dust, whereas the concentrations of PC MPs in indoor and outdoor dust were similar (Liu et al., 2019). These results suggest the differences in the applications of PET and PC plastics. PET plastic is mainly used in textile fibers (65%) and packaging (30%), which are widely used indoors. PC plastic is mainly used in construction materials (24.1%), electronic/electrical products (22.4%), automotive industry (16.5%), consumer appliances (11.4%), medical and packaging (9.1%) (Energy, 2019). Thus, the indoor environment is the main source for PET MPs, whereas PC MPs arise from multiple sources from both indoor and outdoor environments.

Figure 4.

Figure 4.

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Comparison of concentrations of PET (a) and PC (b) microplastics and the ratios of concentrations of PC and PET (c) in indoor dust, sewage sludge and sediments from the United States (the upper and lower black horizontal lines represent the 75th and 25th percentile values, and the pink horizontal line represents the median value).

4. Conclusions

This study provides a quantitative measure of PET and PC microplastic concentrations in freshwater and marine sediments collected from three global regions. This study establishes baseline data on the concentrations of MPs in sediments that can be used in future trend monitoring. It should be noted that sediments were sieved through a 1-mm sieve prior to extraction and therefore PET and PC MPs measured in sediments represent only a fraction of the total concentrations. Further studies are needed to quantitatively assess other types of MPs present in sediment (e.g., polystyrene, polyurethane, polypropylene) and their effects on benthic organisms.

Supplementary Material

1

HIGHLIGHTS.

  • Polyethylene terephthalate and polycarbonate microplastics were found in sediment at concentrations of up to 13000 and 140 μg/g, respectively.

  • PET and PC concentrations were correlated with those of terephthalate and BPA, respectively.

  • PET and PC concentrations decreased in sediment with increasing distance from the source.

  • No distinct vertical profile was recorded for PET or PC microplastics in sediment cores.

Acknowledgements

We thank Drs. Hyo-Bang Moon and Nobuyoshi Yamashita for providing sediment samples from Lake Shihwa and Tokyo Bay, respectively. This work was supported in part by the National Natural Science Foundation of China (41722304) and the 111 Program of the Ministry of Education, China (T2017002) and by Chinese Scholarship Council (CSC 201806200120). The study was funded, in part (method development), by the National Institute of Environmental Health Sciences of the National Institutes of Health under Award No. U2CES026542. The content is solely the responsibility of the authors and does not necessarily represent the official views of the National Institutes of Health. All the authors declare that they have no competing interests.

Footnotes

Declaration of interests

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

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Appendix A. Supplementary data

Supplementary data to this article can be found online at: https://doi.org/10.1016/j.chemosphere.2021.130551.

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