Elsevier

Marine Pollution Bulletin

Volume 138, January 2019, Pages 333-340
Marine Pollution Bulletin

Improvements in polycyclic aromatic hydrocarbon contamination in the Japan Sea: An interannual survey from 2008 to 2014

https://doi.org/10.1016/j.marpolbul.2018.11.061Get rights and content

Highlights

  • PAHs in the surface waters of the Japan Sea have been decreasing from 2008 to 2014.

  • PAH composition has shifted from petrogenic to combustion based sources.

  • PAH concentration and composition between the Tsushima and Korean currents differed.

  • The Kuroshio current is likely not the source of PAH contamination in the Japan Sea.

Abstract

The concentrations and distributions of polycyclic aromatic hydrocarbons (PAHs) were examined from 2008 to 2014 in the surface waters of the Japan Sea region. PAH concentrations decreased in the Japan Sea and Tsushima Strait; consistent with improvements in atmospheric pollution from Japan. There were no changes in the Korean Strait, suggesting a continual influx of contamination separate from the Japan Sea. At all sites, PAHs in the dissolved phase were greater than in the particulate phase. A separate survey in 2011 studied whether contamination in the Kuroshio current accounted for the contamination in the Tsushima strait and Japan Sea. PAH concentrations increased as waters moved into the Tsushima strait and the Japan Sea, suggesting inputs were local and not from the Kuroshio current. This was however confounded by the greater influence of particulate phase PAHs, which are likely deposited by seasonal desert storms.

Introduction

The Japan Sea is a region of important economic and industrial activity, as well an important route for international oil shipments (Varlamov et al., 1999). It is a marginal sea where the major inputs are the southern Tsushima and Korean Straits, which are respectively sourced from an offshoot of the Kuroshio current and the East China Sea (Ichikawa and Beardsley, 2002; Ohshima, 1994; Senjyu et al., 2008). This latter source is a concern, as it is highly polluted by terrestrial sources such as the Yangtze (Changjiang) river (Lin et al., 2013), but from shipping oil discharge as well (Shi et al., 2008). Like the Soya and Tsugaru straits in the north, the Tsushima and Korean straits in the south are shallow and narrow, making the Japan Sea a relatively isolated water body where it is believed contaminants are liable to accumulate (Hayakawa et al., 2016). However, there is limited evidence for this and the extent of contamination in these waters remains poorly understood, especially in surface waters away from the coastlines.

These contaminants include the polycyclic aromatic hydrocarbons (PAHs), a group of compounds with fused aromatic rings and known mutagenic properties (Pashin and Bakhitova, 1979; Ren et al., 2010; Suzuki et al., 2017). In East-Asia, much research has been devoted to their atmospheric distributions and transboundary dispersal (Inomata et al., 2012; Iwasaka et al., 2009; Li et al., 2014; Sato et al., 2008). However, less is known about their distributions in Asian marine ecosystems, particularly in the Japan Sea, despite these environments being the terminal destinations for these compounds (Chizhova et al., 2013; Hayakawa et al., 2016). In their studies of the northern areas of the Japan Sea, Chizhova et al. (2013) found that PAHs were predominantly in the surface waters, especially in the particulate phase, suggesting that atmospheric deposition was a major contributor to marine water PAHs. Direct atmospheric inputs, via gas partitioning and particulate deposition, as well as surface runoff are major PAH sources in marine waters. However, PAHs also leach into the marine environment through anthropogenic oil spills and natural seep (Duran and Craveo-Laureau, 2016). Many studies of PAH concentrations examine sediment loadings, as PAHs are hydrophobic and rapidly sorb onto particulate matter, which subsequently becomes part of the marine sediment (Boitsov et al., 2013; Kafilzadeh, 2015; Wang et al., 2014a). However, there remains a dissolved phase in the surface layers that is available for biological interaction (Zhou et al., 1996). While PAHs are regarded as persistent compounds, in surface waters abiotic factors such as photolysis (Smith et al., 1978) and biotic factors such as microbial degradation (Duran and Craveo-Laureau, 2016) can degrade these compounds or transform them into more harmful congeners. However, trace levels of PAHs remain and can be a gauge of the extent of atmospheric deposition.

In this study, surveys were conducted to understand the concentrations, distributions and composition of PAHs in the surface marine waters of the Japan Sea between 2008 and 2014 in the Japan Sea, as well as in the Korean and Tsushima straits. Furthermore, a separate survey examined the PAH concentrations and composition for the Tsushima strait and the Kuroshio current to understand whether the PAH composition of these source waters reflect what is found in the Japan Sea.

Section snippets

Marine water surveys

Since there is significant seasonal variability in marine water PAH concentrations (Ya et al., 2017; Zhang et al., 2016), for the purposes of an interannual comparison sample collection was performed in the autumn, when samples could be consistently collected. Samples were acquired using a series of marine vessel surveys from 2008 to 2014 in the Japan Sea as well as in the Tsushima Strait and the Korean Strait. These two straits respectively represent the eastern and western channels from which

Interannual changes in PAH concentration and composition in the Japan Sea, Tsushima strait and Korean strait: 2008–2014

Preliminary analyses, using PCAs and calculations of PAH relative abundance, were based on separate DPAH and PPAH studies and it was found that the PAH composition between the two phases did not differ (data not shown). This was despite the disparity in kow values between 3 and 5 ring PAHs which can range between 4 and 7 (Hayakawa, 2018), though this may be due to particles smaller than the GFF pore size (0.5 μm) passing into the dissolved fraction during the filtering process. These smaller

Conclusion

In this study, PAH concentrations were examined in the surface waters of the Japan Sea for the period between 2008 and 2014 and can be related to decreases in emissions from the Japanese islands and possibly improvements in pollution levels from China. There were significant decreases in TPAH concentrations in the Japan Sea and similar changes were also seen in the Tsushima strait. The Korean strait however did not show a similar trend, suggesting either additional terrestrial inputs from Korea

Acknowledgements

The authors would like to thank the Ministry of Education, Culture, Sports, Science and Technology of Japan (Grants-in-aid for Scientific Research #21256001) and the Ministry of the Environment of Japan (Environmental Research and Technology Development Fund # B-0905) for their generous funding of this research. We would also like to thank the Steel Foundation for Environmental Protection Technology, Japan for their financial support. We would also like to acknowledge Dr. Takuya Kawanishi for

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