Marine Pollution Bulletin 97 (2015) 512–517
Contents lists available at ScienceDirect
Marine Pollution Bulletin journal homepage: www.elsevier.com/locate/marpolbul
Baseline
New non-PBDE brominated flame retardants in sediment and plant samples from Jiaozhou Bay wetland Ling Wang a,⇑, Quansheng Zhao a, Yanyan Zhao a, Minggang Zheng b, Yinghua Lou a, Baijuan Yang b a b
Chemical and Environmental Engineering, Qingdao University, Qingdao 266071, China Research Center for Marine Ecology, The First Institute of Oceanography, State Oceanic Administration of China, Qingdao 266061, China
a r t i c l e
i n f o
Article history: Received 16 December 2014 Revised 23 April 2015 Accepted 12 May 2015 Available online 16 May 2015 Keywords: Non-polybrominated diphenyl ethers Brominated flame retardants Jiaozhou Bay wetland Sediment
a b s t r a c t Seven non-polybrominated diphenyl ethers (non-PBDE) (TBB, TBX, PBT, PBEB, HBB, DBHCTD and BB153) were analyzed in sediment and plant samples which were collected from Xiaojianxi landfill to Dagu river estuary in Jiaozhou Bay wetland. The species of non-PBDE were different in sediment and plant samples with the concentration of 0.41–9.66 ng g 1 and 0.15–1.2 ng g 1, respectively. DBHCTD was the main non-PBDE compared with other target compounds and its concentration was 1.21–9.66 ng g 1 dw. Generally, the concentration of non-PBDE in sediment showed a decreasing tendency while discrete decline in plant has been revealed. Furthermore, DBHCTD, HBB, as well as other BFRs, might have a common BFRs degradation or similar accumulation potential in sediment, as their Pearson relationship p < 0.05. Generally, the content of non-PBDE in Jiaozhou Bay wetland was higher than other published research. Therefore, more attention should be paid to non-PBDE on account of their persisting impact on human health and environment. Ó 2015 Elsevier Ltd. All rights reserved.
Brominated flame retardants (BFRs) are chemicals including aliphatics, cycloaliphatic, aromatic and aromatic–aliphatic bromine-containing compounds that are added to polymeric materials and other materials to prevent fires (Luo et al., 2010). In the past ten years, persistent organic pollutants (POPs) are becoming the forefront and hotspot in the field of environmental science. Recently, polybrominated diphenyl ethers (PBDEs) and the novel non-polybrominated diphenyl ethers (non-PBDE) BFRs have received much attention. On account of their ubiquitous presence in the environment, they maybe have adverse effects on human and wildlife (Hites, 2004; Covaci et al., 2011). With BFRs of PBDEs were restrictive usage by the Stockholm Convention, some non-PBDE BFRs are added as additives into a variety of commercial products, such as carpets, electronic cables, polyurethane foams, television sets, and computers (Marvin et al., 2011). Moreover, a number of studies have demonstrated that some BFRs known as 1,3,5-tribromobenzene (TBB), pentabromotoluene (PBT), penta-bromoethylbenzene (PBEB) and hexa-bromobenzene (HBB) probably are very stable in different environment matrics (Qiu et al., 2007), and some of them have accumulated in exposed biota (Wu et al., 2010).
⇑ Corresponding author. E-mail address: [email protected] (L. Wang). http://dx.doi.org/10.1016/j.marpolbul.2015.05.026 0025-326X/Ó 2015 Elsevier Ltd. All rights reserved.
Due to phase-outs of PBDEs in some industrial countries, some other non-PBDE BFRs, such as PBT, hexachlorocyclopentadienyl-di bromocyclooctane (DBHCTD), TBB have a broad development space. Meanwhile, some historically used BFRs are being reintroduced to the market, such as HBB and PBEB (Salamova and Hites, 2011). With wide usage of BFRs, they could be released into the environment through production process, and waste disposal stages. At present, they have been found in fishes, sediment of rivers and lakes, air and soil, and even human milk (Covaci et al., 2011; Moller et al., 2011; Davis et al., 2012; Zhu et al., 2009). In order to meet the rigorous fire regulations, these non-PBDE BFRs have been used as alternatives for the discontinued PBDEs in some applications (Betts, 2008). Consequentially, consumption and production of these non-PBDE BFRs will keep rising, and they will become a tough problem in the near future. Some targeted non-PBDEs in Jiaozhou Bay wetland are briefly introduced below. HBB is an organobromine flame retardant and it is often used in plastics, textiles, woods (Mattson et al., 1975), paper, electrical and manufactured products (Chemicals in the Environment, FY2001, 2003). Some studies reported HBB was degraded to debrominated products, which is mainly derived to penta-, tetra- and tri(Yukihiko et al., 1988). In Great Lakes, Velsicol Chemical Corporation (formerly Michigan Chemical Corporation), located in St. Louis, Michigan, was the major HBB manufacturer in history, while halted production in the 1980s (U.S. EPA, 2008). In Asia,
L. Wang et al. / Marine Pollution Bulletin 97 (2015) 512–517
Nippoh Chemical (Chiba, Japan) and Dayang Chemicals (Hangzhou City, China) have been producing HBB in recent years (Gauthier et al., 2007), and the production volume was 1000–5000 t per year. In Japan, the production of HBB was 270 tons in 1983 (Hirama, 1984), and 350 tons in 2001 (Gauthier et al., 2007), however, the production figures of HBB were not available in recent years. DBHCTD was identified as a flame retardant in 1975 (Riddell et al., 2008), and there is no report on its manufacturer, production and usage. It is a commercial BFRs and usually used in the polystyrene resin. DBHCTD’s molecule includes bromine and chlorine atoms, and exists as a pair of enantiomers. It may be the reason that the compound has not been detected in the environment for a long period. At present, the information about DBHCTD’s production and application is scarce. In 2008, DBHCTD was first detected in the environment by Zhu et al. (2008) in residential indoor air and dust of Canadian homes. The concentration of DBHCTD is a geometric mean of 2.70 ng g 1 and a median of 2.00 ng g 1. In 2012, Yang et al. (2012) detected DBHCTD in sediments in the Great Lakes, and the concentration was in the range of 0.21– 2.30 ng g 1 dw. Among them, TBB, PBT are also manufactured in China (Chen et al., 2013). However, the annual production is not available. As far as PBEB is concerned, there is no information about manufacture in China. In 2009, Lam et al. (2009) detected TBB in marine mammals in Hong Kong, and this is the first report of the presence of TBB in the environment. In 2012, Yang et al. (2012) detected TBB in sediment of Great Lakes, and the concentration is range of
Contents lists available at ScienceDirect
Marine Pollution Bulletin journal homepage: www.elsevier.com/locate/marpolbul
Baseline
New non-PBDE brominated flame retardants in sediment and plant samples from Jiaozhou Bay wetland Ling Wang a,⇑, Quansheng Zhao a, Yanyan Zhao a, Minggang Zheng b, Yinghua Lou a, Baijuan Yang b a b
Chemical and Environmental Engineering, Qingdao University, Qingdao 266071, China Research Center for Marine Ecology, The First Institute of Oceanography, State Oceanic Administration of China, Qingdao 266061, China
a r t i c l e
i n f o
Article history: Received 16 December 2014 Revised 23 April 2015 Accepted 12 May 2015 Available online 16 May 2015 Keywords: Non-polybrominated diphenyl ethers Brominated flame retardants Jiaozhou Bay wetland Sediment
a b s t r a c t Seven non-polybrominated diphenyl ethers (non-PBDE) (TBB, TBX, PBT, PBEB, HBB, DBHCTD and BB153) were analyzed in sediment and plant samples which were collected from Xiaojianxi landfill to Dagu river estuary in Jiaozhou Bay wetland. The species of non-PBDE were different in sediment and plant samples with the concentration of 0.41–9.66 ng g 1 and 0.15–1.2 ng g 1, respectively. DBHCTD was the main non-PBDE compared with other target compounds and its concentration was 1.21–9.66 ng g 1 dw. Generally, the concentration of non-PBDE in sediment showed a decreasing tendency while discrete decline in plant has been revealed. Furthermore, DBHCTD, HBB, as well as other BFRs, might have a common BFRs degradation or similar accumulation potential in sediment, as their Pearson relationship p < 0.05. Generally, the content of non-PBDE in Jiaozhou Bay wetland was higher than other published research. Therefore, more attention should be paid to non-PBDE on account of their persisting impact on human health and environment. Ó 2015 Elsevier Ltd. All rights reserved.
Brominated flame retardants (BFRs) are chemicals including aliphatics, cycloaliphatic, aromatic and aromatic–aliphatic bromine-containing compounds that are added to polymeric materials and other materials to prevent fires (Luo et al., 2010). In the past ten years, persistent organic pollutants (POPs) are becoming the forefront and hotspot in the field of environmental science. Recently, polybrominated diphenyl ethers (PBDEs) and the novel non-polybrominated diphenyl ethers (non-PBDE) BFRs have received much attention. On account of their ubiquitous presence in the environment, they maybe have adverse effects on human and wildlife (Hites, 2004; Covaci et al., 2011). With BFRs of PBDEs were restrictive usage by the Stockholm Convention, some non-PBDE BFRs are added as additives into a variety of commercial products, such as carpets, electronic cables, polyurethane foams, television sets, and computers (Marvin et al., 2011). Moreover, a number of studies have demonstrated that some BFRs known as 1,3,5-tribromobenzene (TBB), pentabromotoluene (PBT), penta-bromoethylbenzene (PBEB) and hexa-bromobenzene (HBB) probably are very stable in different environment matrics (Qiu et al., 2007), and some of them have accumulated in exposed biota (Wu et al., 2010).
⇑ Corresponding author. E-mail address: [email protected] (L. Wang). http://dx.doi.org/10.1016/j.marpolbul.2015.05.026 0025-326X/Ó 2015 Elsevier Ltd. All rights reserved.
Due to phase-outs of PBDEs in some industrial countries, some other non-PBDE BFRs, such as PBT, hexachlorocyclopentadienyl-di bromocyclooctane (DBHCTD), TBB have a broad development space. Meanwhile, some historically used BFRs are being reintroduced to the market, such as HBB and PBEB (Salamova and Hites, 2011). With wide usage of BFRs, they could be released into the environment through production process, and waste disposal stages. At present, they have been found in fishes, sediment of rivers and lakes, air and soil, and even human milk (Covaci et al., 2011; Moller et al., 2011; Davis et al., 2012; Zhu et al., 2009). In order to meet the rigorous fire regulations, these non-PBDE BFRs have been used as alternatives for the discontinued PBDEs in some applications (Betts, 2008). Consequentially, consumption and production of these non-PBDE BFRs will keep rising, and they will become a tough problem in the near future. Some targeted non-PBDEs in Jiaozhou Bay wetland are briefly introduced below. HBB is an organobromine flame retardant and it is often used in plastics, textiles, woods (Mattson et al., 1975), paper, electrical and manufactured products (Chemicals in the Environment, FY2001, 2003). Some studies reported HBB was degraded to debrominated products, which is mainly derived to penta-, tetra- and tri(Yukihiko et al., 1988). In Great Lakes, Velsicol Chemical Corporation (formerly Michigan Chemical Corporation), located in St. Louis, Michigan, was the major HBB manufacturer in history, while halted production in the 1980s (U.S. EPA, 2008). In Asia,
L. Wang et al. / Marine Pollution Bulletin 97 (2015) 512–517
Nippoh Chemical (Chiba, Japan) and Dayang Chemicals (Hangzhou City, China) have been producing HBB in recent years (Gauthier et al., 2007), and the production volume was 1000–5000 t per year. In Japan, the production of HBB was 270 tons in 1983 (Hirama, 1984), and 350 tons in 2001 (Gauthier et al., 2007), however, the production figures of HBB were not available in recent years. DBHCTD was identified as a flame retardant in 1975 (Riddell et al., 2008), and there is no report on its manufacturer, production and usage. It is a commercial BFRs and usually used in the polystyrene resin. DBHCTD’s molecule includes bromine and chlorine atoms, and exists as a pair of enantiomers. It may be the reason that the compound has not been detected in the environment for a long period. At present, the information about DBHCTD’s production and application is scarce. In 2008, DBHCTD was first detected in the environment by Zhu et al. (2008) in residential indoor air and dust of Canadian homes. The concentration of DBHCTD is a geometric mean of 2.70 ng g 1 and a median of 2.00 ng g 1. In 2012, Yang et al. (2012) detected DBHCTD in sediments in the Great Lakes, and the concentration was in the range of 0.21– 2.30 ng g 1 dw. Among them, TBB, PBT are also manufactured in China (Chen et al., 2013). However, the annual production is not available. As far as PBEB is concerned, there is no information about manufacture in China. In 2009, Lam et al. (2009) detected TBB in marine mammals in Hong Kong, and this is the first report of the presence of TBB in the environment. In 2012, Yang et al. (2012) detected TBB in sediment of Great Lakes, and the concentration is range of
