Elsevier

Environment International

Volumes 92–93, July–August 2016, Pages 507-514
Environment International

Time trends of polybrominated diphenyl ethers in East China Seas: Response to the booming of PBDE pollution industry in China

https://doi.org/10.1016/j.envint.2016.04.033Get rights and content

Highlights

  • There was a sharp increase of PBDEs from 1990s in China.

  • There were different time trends of PBDEs between developed countries and China.

  • Increasing PBDE level was accompanied by the booming of manufacturing industry.

  • PBDE emissions from recycling centers of e-wastes were important source.

  • Better management of these PBDE-containing products is urgently needed in China.

Abstract

The East China Seas (ECSs) are the receptors of the land-based persistent organic pollutants (POPs), such as polybrominated diphenyl ethers (PBDEs) mainly from China through atmospheric deposition driven by the East Asian winter monsoon and fluvial discharge (e.g., Yangtze River and Yellow River), making the offshore sediments to be a good proxy to reconstruct history of those pollutants in China. In this work, four well-placed sediment cores were extracted from the mud areas in the ECSs, and the 210Pb-dated cores were analyzed to yield historical concentration profiles of PBDEs in the area. The results showed that there was a persistent increase from 1970s and almost no clear sign in the decline of PBDEs until recently in China. More importantly, there was a faster increase of PBDEs from 1990s in China; while this period was just shown as gradually leveling off or even declining trends in developed countries. The persistently increasing trend of PBDEs in China since 1990s could be largely due to the booming of the manufacturing industry and unexpectedly transfer of PBDE pollution from developed countries to China. Besides, the relative high concentrations and fluxes of PBDEs in the core from coastal ECS located near a well-known electrical/electronic waste (e-waste) recycling area suggests an important contribution of PBDE emissions from recycling centers of e-waste in China. Although efforts in environmental monitoring of PBDE contamination have been substantially increased over the last decade, China is still lagging behind in terms of nationwide regulation of PBDE usage and treatment of disposal PBDE-containing products.

Introduction

Polybrominated diphenyl ethers (PBDEs) are used as additives in many electrical and electronic products, textiles, plastics, building materials and furnishings to reduce flammability. PBDEs dissolve in the polymers and can therefore easily escape from these products during their production, usage and disposal (de Wit, 2002, Rahman et al., 2001). Generally, PBDEs are commercially available in three technical mixtures as penta-, octa- and deca-BDE mixtures (Siddiqi et al., 2003). The industrialized countries started to use PBDEs and the usage increased from the early 1970s. In 1992, the global production of PBDEs was ~ 40,000 t, but in 1999 this increased to close 70,000 t (Renner, 2000). High levels of PBDEs in the environment (including water, soil, atmosphere and various organism bodies) have been documented in the USA and Western European countries (Minh et al., 2007, Song et al., 2004, Song et al., 2005a, Song et al., 2005b, Zegers et al., 2003). The penta- and octa-BDE mixtures were banned in Europe and United States in 2004 largely due to environmental and public health concerns. In May 2009, two kinds of PBDEs were listed on the Stockholm Convention. Shortly afterwards, restrictions have been imposed on the production and use of deca-BDE in Europe and United States. As PBDEs were banned in those developed nations, lots of manufacturing capacities were moved to the less developed nations such as China, India, Indonesia, Malaysia, the Philippines, Thailand and Vietnam (Hale et al., 2003, Kwan et al., 2014). Especially in China and India, as the manufacturing industry has been increasing considerably, there has been a heavy demand for PBDEs in recent decades (Chen et al., 2007). The production of deca-BDE technical mixture, the predominant commercial PBDE product, increased from 10,000 t to about 30,000 t from 2000 to 2005 in China (Chen et al., 2007). More importantly, as Asian countries, China, India and Pakistan have long been suspected of receiving and disposing the bulk of the world's obsolete electronic goods so-called “e-waste” (Martin et al., 2004). Because no definite regulations have been imposed on PBDE production and usage, it could be expected that the environmental levels of PBDEs will continue to increase in some Asian countries.

PBDEs have been found in various environmental media and gradually become a critical problem in China in recent decades (Kang et al., 2011, Li et al., 2012, Mai et al., 2005, Wang et al., 2011, Wang et al., 2012). However, continuous data about the pollution status of these pollutants was extremely scarce in China. In most cases, the market demand of these PBDE compounds is not fully known and there is an absence of production and usage data, thus making it difficult to track the time trend and evaluate the recent pollution situation of these chemicals. PBDEs preserved in undisturbed and well-dated sediment cores could be an effective means to reconstruct the historical record of these chemicals.

The East China Marginal Seas (including Bohai Sea (BS), Yellow Sea (YS) and East China Sea (ECS)) (Fig. 1) adjoin the famous industrial districts in China. Adjacent four provinces (including Shandong, Hebei, Jiangsu and Zhejiang) and three municipalities under the direct jurisdiction of the Central Government (including Beijing, Tianjin and Shanghai) supported almost 40% of the national GDP in the past twenty years (http://www.stats.gov.cn). These developed areas could be considered to account large demand and emission of PBDEs in China. The continental shelves of the East China Marginal Seas are in the pathway of Asian continental outflow to the northwest Pacific Ocean driven by the East Asian monsoon (Lang et al., 2008, Lin et al., 2011, Primbs et al., 2007, Zhang et al., 1992). Besides, the East China Marginal Seas receive discharge from two dominate rivers (Yellow River and Yangtze River) in China. They are thus the receptors of the land-based POPs through atmospheric deposition and fluvial discharge (Lin et al., 2011, Lin et al., 2013). The coastal ECS is a major sink of the Yangtze River-derived sediments and associated pollutants into the sea (Li et al., 2012, Liu et al., 2006). The mud deposits from the central BS, YS and distal ECS contain airborne contaminants transported from the upwind region, Mainland China, therefore, they can memory the PBDE pollution in North and East China (Guo et al., 2006, Guo et al., 2007). In the previous studies, the historical records of polycyclic aromatic hydrocarbons (PAHs) and organochlorine pesticides (OCPs) in these areas were well documented to coincide with the emission or usage of these pollutants in China (Guo et al., 2006, Lin et al., 2016). In this study, four well-placed 210Pb dated sediment cores collected from the different mud areas in the central BS, central YS, coastal ECS and central ECS were analyzed in order to identify their possible sources and provide a better understanding of the long-term trends of PBDE pollution in China.

Section snippets

Sample collection

Core M7 (39°32′N, 120°27′E) was collected from the central BS in 2013 using a box corer with the water depth of 29 m and the core length of 53 cm. Core F0306 (34°59′N, 122°30′E) was collected from the central mud in the south YS in 2007 using a box corer with the water depth of 65 m and the core length of 37 cm. Core C0803 (27°38′N, 121°39′E) was collected from the inner shelf mud in ECS in 2009 using a gravity corer with the water depth of 50 m and the core length of 189 cm, and core FFJ103

Concentrations and deposition fluxes of PBDEs

The four cores (M7, F0306, FFJ103 and C0803) were measured for the following 9 PBDE congeners: BDE-28, -47, -99, -100, -138, -153, -154, -183 and -209, and their concentrations are shown in Tables S1–S4. These congeners have also been reported in abundance and high detection frequencies in the coastal air, soils, sediments and water in China (Han et al., 2009, Li et al., 2012, Qiu et al., 2010, Wang et al., 2011). BDE-209 in the environment has been reported to originate only from deca-BDE

Implication for the transfer of PBDE pollution from developed countries to China

In U.S.A., it was reported that the ∑12PBDEs and BDE-209 concentrations increased exponentially from the 1960s to 1980s, and after which they leveled off in the sediment core collected from the Lake Michigan (Zhu and Hites, 2005). Historical trends of PBDEs were investigated in three countries of Western Europe, and found that the penta-BDE-derived congeners and BDE-209 were almost detected leveling off and decrease in the early or late 1990s (Zegers et al., 2003). Besides, PBDE concentrations

Conclusions

This work examined the time trend of PBDEs in China based on the dated sediment cores collected from East China Seas. The concentrations of PBDEs sharply increased in 1990s and almost no sign of declining trend; while a gradually leveling off or even declining trends appeared in the some major developed countries during the same period. This could provide a significant evidence for the booming of the manufacturing activities in China and further indicates an inevitable transfer of PBDE

Acknowledgements

This work was supported by the Natural Science Foundation of China (NSFC) (Nos. 41376051, 41506124, 41103046 and 41176085), National Basic Research Program of China (No. 2014CB953701), and the National Programme on Global Change and Air-Sea Interaction (GASI-GEOGE-03). We are most grateful to Prof. Ming Fang for his invaluable advices and comments. The anonymous reviewers should be sincerely appreciated for their constructive comments that greatly improved this work.

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