PBDEs versus NBFR in wastewater treatment plants: occurrence and partitioning in water and sludge

Joyce Cristale; Silvia Lacorte; Joyce Cristale; Silvia Lacorte

doi:10.3934/environsci.2015.3.533

AIMS Environmental Science

2015, Volume 2, Issue 3: 533-546. doi: 10.3934/environsci.2015.3.533

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Research article Special Issues

PBDEs versus NBFR in wastewater treatment plants: occurrence and partitioning in water and sludge

Joyce Cristale ,
Silvia Lacorte ^,

Department of Environmental Chemistry, IDAEA-CSIC, Jordi Girona 18-26, 08034 Barcelona, Catalonia, Spain

Received: 06 February 2015 Accepted: 08 June 2015 Published: 10 June 2015

This study evaluates the occurrence of flame retardants (FR) in five wastewater treatment plants (WWTPs) located close to Barcelona (NE Spain), an area with high urban and industrial pressures. Compounds studied include eight polybromodiphenyl ethers (PBDEs) and eight New Brominated Flame Retardants (NBFRs), for which little information regarding their presence, partitioning and fate within the WWTPs is available. In unfiltered influent samples, PBDEs were not detected and bis(2-ethyl-1-hexyl)tetrabromophthalate was the only NBFR detected, and all WWTPs were efficient in eliminating this compound as no residues were found in the effluents. However, primary sludge contained from 279 to 2299 ng/g dry weight of ΣFR and the concentration increased in secondary (biological) sludge. NBFRs accounted for the main FR detected in sludge, representing a 63-97% of the total load, and among PBDEs, BDE-209 was the most ubiquitous congener. Considering the amount of sludge generated in each WWTP, it was estimated that 0.34-17.2 kg of FR are released annually through the sludge, which can have negative environmental and health implications if sludge is used as biosolid in agriculture. Overall, this study provides a sampling design and analytical protocol to be used to determine the evolution of FR in WWTPs and compares the levels detected, considering that PBDEs are being phased out to be substituted by other compounds which also have high accumulative and recalcitrant properties.
- polybrominated diphenyl ethers,
- new brominated flame retardants,
- wastewater,
- sludge,
- WWTP
Citation: Joyce Cristale, Silvia Lacorte. PBDEs versus NBFR in wastewater treatment plants: occurrence and partitioning in water and sludge[J]. AIMS Environmental Science, 2015, 2(3): 533-546. doi: 10.3934/environsci.2015.3.533

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Abstract

This study evaluates the occurrence of flame retardants (FR) in five wastewater treatment plants (WWTPs) located close to Barcelona (NE Spain), an area with high urban and industrial pressures. Compounds studied include eight polybromodiphenyl ethers (PBDEs) and eight New Brominated Flame Retardants (NBFRs), for which little information regarding their presence, partitioning and fate within the WWTPs is available. In unfiltered influent samples, PBDEs were not detected and bis(2-ethyl-1-hexyl)tetrabromophthalate was the only NBFR detected, and all WWTPs were efficient in eliminating this compound as no residues were found in the effluents. However, primary sludge contained from 279 to 2299 ng/g dry weight of ΣFR and the concentration increased in secondary (biological) sludge. NBFRs accounted for the main FR detected in sludge, representing a 63-97% of the total load, and among PBDEs, BDE-209 was the most ubiquitous congener. Considering the amount of sludge generated in each WWTP, it was estimated that 0.34-17.2 kg of FR are released annually through the sludge, which can have negative environmental and health implications if sludge is used as biosolid in agriculture. Overall, this study provides a sampling design and analytical protocol to be used to determine the evolution of FR in WWTPs and compares the levels detected, considering that PBDEs are being phased out to be substituted by other compounds which also have high accumulative and recalcitrant properties.

References

[1]	Vigil KM (2003) Clean Water - An Introduction to Water Quality and Water Pollution Control. 2 Ed, Corvallis, US: Oregon State University Press.
[2]	Sánchez-Avila J, Bonet J, Velasco G, et al. (2009) Determination and occurrence of phthalates, alkylphenols, bisphenol A, PBDEs, PCBs and PAHs in an industrial sewage grid discharging to a Municipal Wastewater Treatment Plant. Sci Total Environ 407: 4157-4167. doi: 10.1016/j.scitotenv.2009.03.016
[3]	Andresen J, Bester K (2006) Elimination of organophosphate ester flame retardants and plasticizers in drinking water purification. Water Res 40: 621-629. doi: 10.1016/j.watres.2005.11.022
[4]	Barber LB, Keefe SH, Brown GK, et al. (2013) Persistence and potential effects of complex organic contaminant mixtures in wastewater-impacted streams. Environ Sci Technol 47: 2177-2188. doi: 10.1021/es303720g
[5]	Costa LG, Giordano G (2007) Developmental neurotoxicity of polybrominated diphenyl ether (PBDE) flame retardants. Neurotoxicology 28: 1047-1067. doi: 10.1016/j.neuro.2007.08.007
[6]	Vonderheide AP, Mueller KE, Meija J, et al. (2008) Polybrominated diphenyl ethers: Causes for concern and knowledge gaps regarding environmental distribution, fate and toxicity. Sci Total Environ 400: 425-436. doi: 10.1016/j.scitotenv.2008.05.003
[7]	Chen SJ, Feng AH, He MJ, et al. (2013) Current levels and composition profiles of PBDEs and alternative flame retardants in surface sediments from the Pearl River Delta, southern China: Comparison with historical data. Sci Total Environ 444: 205-211. doi: 10.1016/j.scitotenv.2012.11.104
[8]	Cristale J, García Vázquez A, Barata C, et al. (2013) Priority and emerging flame retardants in rivers: Occurrence in water and sediment, Daphnia magna toxicity and risk assessment. Environ Int 59: 232-243. doi: 10.1016/j.envint.2013.06.011
[9]	Anderson TD, MacRae JD (2006) Polybrominated diphenyl ethers in fish and wastewater samples from an area of the Penobscot River in Central Maine. Chemosphere 62: 1153-1160. doi: 10.1016/j.chemosphere.2005.06.034
[10]	Lavandier R, Quinete N, Hauser-Davis RA, et al. (2013) Polychlorinated biphenyls (PCBs) and Polybrominated Diphenyl ethers (PBDEs) in three fish species from an estuary in the southeastern coast of Brazil. Chemosphere 90: 2435-2443. doi: 10.1016/j.chemosphere.2012.11.001
[11]	Washington State University, Department of Ecology: Olympia, WA,. Washington State polybrominated diphenyl ether (PBDE) chemical action plan: Final plan. 2006. Available from: https://fortress.wa.gov/ecy/publications/summarypages/0507048.html
[12]	Alaee M, Arias P, Sjödin A, et al. (2003) An overview of commercially used brominated flame retardants, their applications, their use patterns in different countries/regions and possible modes of release. Environ Int 29: 683-689. doi: 10.1016/S0160-4120(03)00121-1
[13]	Cristale J, Lacorte S (2013) Development and validation of a multiresidue method for the analysis of polybrominated diphenyl ethers, new brominated and organophosphorus flame retardants in sediment, sludge and dust. J Chromatogr A 1305: 267-275. doi: 10.1016/j.chroma.2013.07.028
[14]	Jaffé R (1991) Fate of hydrophobic organic pollutants in the aquatic environment: A review. Environ Pollut 69: 237-257. doi: 10.1016/0269-7491(91)90147-O
[15]	Mackay D, Shiu WY, Ma KC, et al. (2006) Handbook of physical-chemical properties and environmental fate for organic chemicals. 3 ed. Vol. III. Boca Raton (USA): Taylor & Francis Group.
[16]	Tittlemier SA, Halldorson T, Stern GA, et al. (2002) Vapor pressures, aqueous solubilities, and Henry's law constants of some brominated flame retardants. Environ Toxicol Chem 21: 1804-1810. doi: 10.1002/etc.5620210907
[17]	Wang W, Delgado-Moreno L, Ye Q, et al. (2011) Improved measurements of partition coefficients for polybrominated diphenyl ethers. Environ Sci Technol 45: 1521-1527. doi: 10.1021/es103087a
[18]	Cristale J, Quintana J, Chaler R, et al. (2012) Gas chromatography/mass spectrometry comprehensive analysis of organophosphorus, brominated flame retardants, by-products and formulation intermediates in water. J Chromatogr A 1241: 1-12. doi: 10.1016/j.chroma.2012.04.013
[19]	Kim M, Guerra P, Alaee M, et al. (2014) Occurrence and fate of four novel brominated flame retardants in wastewater treatment plants. Environ Sci Pollut Res 21: 13394-13404. doi: 10.1007/s11356-014-3262-4
[20]	Xiang N, Chen L, Meng XZ, et al. (2014) Polybrominated diphenyl ethers (PBDEs) and dechlorane plus (DP) in a conventional wastewater treatment plant (WWTP) in Shanghai: Seasonal variations and potential sources. Sci Total Environ 487: 342-349. doi: 10.1016/j.scitotenv.2014.04.014
[21]	Deng D, Chen H, Tam NFY (2015) Temporal and spatial contamination of polybrominated diphenyl ethers (PBDEs) in wastewater treatment plants in Hong Kong. Sci Total Environ 502: 133-142. doi: 10.1016/j.scitotenv.2014.08.090
[22]	Kim M, Guerra P, Theocharides M, et al. (2013) Parameters affecting the occurrence and removal of polybrominated diphenyl ethers in twenty Canadian wastewater treatment plants. Water Res 47: 2213-2221. doi: 10.1016/j.watres.2013.01.031
[23]	Rocha-Gutierrez B, Lee WY (2013) Investigation of polybrominated diphenyl ethers in wastewater treatment plants along the U.S. and Mexico border: A trans-boundary study. Water Air Soil Pollut 224: 1398-1411.
[24]	De la Torre A, Alonso E, Concejero MA, et al. (2011) Sources and behaviour of polybrominated diphenyl ethers (PBDEs), polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in Spanish sewage sludge. Waste Manag 31: 1277-1284. doi: 10.1016/j.wasman.2011.01.021
[25]	Sánchez-Brunete C, Miguel E, Tadeo JL (2009) Analysis of polybrominated diphenyl ethers in sewage sludge by matrix solid-phase dispersion and isotope dilution GC-MS. J Sep Sci 32: 109-117. doi: 10.1002/jssc.200800479
[26]	Gevao B, Muzaini S, Helaleh M (2008) Occurrence and concentrations of polybrominated diphenyl ethers in sewage sludge from three wastewater treatment plants in Kuwait. Chemosphere 71: 242-247. doi: 10.1016/j.chemosphere.2007.09.043
[27]	Stiborova H, Vrkoslavova J, Lovecka P, et al. (2015) Aerobic biodegradation of selected polybrominated diphenyl ethers (PBDEs) in wastewater sewage sludge. Chemosphere 118: 315-321. doi: 10.1016/j.chemosphere.2014.09.048
[28]	Knoth W, Mann W, Meyer R, et al. (2007) Polybrominated diphenyl ether in sewage sludge in Germany. Chemosphere 67: 1831-1837. doi: 10.1016/j.chemosphere.2006.05.113
[29]	Cincinelli A, Martellini T, Misuri L, et al. (2012) PBDEs in Italian sewage sludge and environmental risk of using sewage sludge for land application. Environ Pollut 161: 229-234. doi: 10.1016/j.envpol.2011.11.001
[30]	Lee HJ, Kim CJ, Hong GH, et al. (2014) Congener-specific accumulation and environmental risk assessment of polybrominated diphenyl ethers in diverse Korean sewage sludge types. Environ Sci Pollut Res 21: 7480-7488. doi: 10.1007/s11356-014-2664-7
[31]	Venkatesan AK, Halden RU (2014) Brominated flame retardants in U.S. biosolids from the EPA national sewage sludge survey and chemical persistence in outdoor soil mesocosms. Water Res 55: 133-142.
[32]	Gaylor MO, Mears GL, Harvey E, et al. (2014) Polybrominated diphenyl ether accumulation in an agricultural soil ecosystem receiving wastewater sludge amendments. Environ Sci Technol 48: 7034-7043. doi: 10.1021/es5014032
[33]	Gorga M, Martínez E, Ginebreda A, et al. (2013) Determination of PBDEs, HBB, PBEB, DBDPE, HBCD, TBBPA and related compounds in sewage sludge from Catalonia (Spain). Sci Total Environ 444: 51-59. doi: 10.1016/j.scitotenv.2012.11.066
[34]	Davis EF, Klosterhaus SL, Stapleton HM (2012) Measurement of flame retardants and triclosan in municipal sewage sludge and biosolids. Environ Int 40: 1-7. doi: 10.1016/j.envint.2011.11.008
[35]	Zeng L, Yang R, Zhang Q, et al. (2014) Current Levels and Composition Profiles of Emerging Halogenated Flame Retardants and Dehalogenated Products in Sewage Sludge from Municipal Wastewater Treatment Plants in China. Environ Sci Technol 48:12586-12594. doi: 10.1021/es503510q
[36]	Gerecke AC, Giger W, Hartmann PC, et al. (2006) Anaerobic degradation of brominated flame retardants in sewage sludge. Chemosphere 64: 311-317. doi: 10.1016/j.chemosphere.2005.12.016
[37]	Shin M, Duncan B, Seto P, et al. (2010) Dynamics of selected pre-existing polybrominated diphenylethers (PBDEs) in municipal wastewater sludge under anaerobic conditions. Chemosphere 78: 1220-1224. doi: 10.1016/j.chemosphere.2009.12.057
[38]	Gómez-Canela C, Barth JAC, Lacorte S (2012) Occurrence and fate of perfluorinated compounds in sewage sludge from Spain and Germany. Environ Sci Pollut Res 19: 4109-4119. doi: 10.1007/s11356-012-1078-7

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