South-central Arkansas (AR) is home to major manufacturing facilities for brominated flame retardant chemicals (BFRs) in the U.S. Unintended release during production may have caused accumulation of the BFRs in the local environment. In this work, sediment cores were collected from six water bodies in AR, including three located close to the BFR manufacturing facilities in El Dorado and Magnolia, to investigate past and recent deposition histories. A total of 49 polybromodiphenyl ethers (PBDEs) and decabromodiphenyl ethane (DBDPE) were detected, with concentrations as high as 57 000 and 2400 ng/g dry weight for decabromodiphenyl ether (BDE209) and DBDPE, respectively. Log−log regression of BDE209 and DBDPE surface concentrations versus distance to known BFR manufacturing facilities fit the Gaussian Plume Dispersion model, and showed that, if the distance is shortened by half, concentrations of BDE209 and DBDPE would increase by 5-fold. The spatial distribution and temporal trend of the contamination indicate that the manufacturing of PBDEs and DBDPE is the primary source for these compounds in the environment of southern Arkansas. Interestingly, the occurrence of debromination of PBDEs in the sediments of a previously used wastewater sludge retention pond in Magnolia is indicated by the presence of congeners that had not been detected in any commercial PBDE mixtures and by increased fractions of lower brominated congeners relative to higher brominated congeners. Two unknown brominated compounds were detected in the sediments, and identified as nonabromodiphenyl ethanes. ■ INTRODUCTION Decabromodiphenyl ether (BDE209) is the main component of the commercial polybrominated diphenyl ether (PBDE) product nicknamed “deca”, which has been marketed since the late 1970s. In the U.S., deca has been marketed under the trade names Saytex102E of Albemarle Corp. and DE-83R of Chemtura Corp. The aggregated U.S. national production volume of deca was in the range of 10−50 million pounds in 1986 and 1990, and 50−100 million pounds in 1994, 1998, 2002, and 2006, according to the U.S. EPA Inventory Update Reporting (IUR) data. Following the cessation of penta and octa production, Albemarle and Chemtura, as well as the largest U.S. importer, ICL Industrial Products, Inc., announced their commitments to phase out deca in the U.S. by December 31, 2012, and to end all its uses by the end of 2013. Decabromodiphenyl ethane (DBDPE) was introduced in the mid-1980s as a replacement for deca. It is marketed in the U.S. under the trade names Saytex8010 by Albemarle and Firemaster 2100 by Chemtura. Information on global consumption of DBDPE is not available. The U.S. EPA IUR record of DBDPE production volume is in the range of 10−50 million pounds for 2006. DBDPE has been detected in the air, tree bark, herring gulls eggs and sediments in the environment of North America. South-central Arkansas, with the largest natural bromine reserves in the country and the largest bromine production in the world, is home to major manufacturing facilities for BFRs in the U.S. Despite the strict measures in controlling and preventing discharges during the manufacturing process and voluntary actions to reduce emissions, unintended release of the products to the environment may not be avoidable. PBDEs Received: March 29, 2012 Revised: July 11, 2012 Accepted: July 13, 2012 Published: July 13, 2012 Article
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