Skip to main content
SpringerLink
Log in

Emulsion-enhanced recovery and biodegradation of decabrominated diphenyl ether in river sediments

  • Sediments, Sec 5 • Sediment Management • Research Article
  • Published:
Journal of Soils and Sediments Aims and scope Submit manuscript

Abstract

Purpose

Polybrominated diphenyl ethers (PBDEs) are flame retardants and regarded as emerging contaminants and persistent organic pollutants (POPs). Due to high lipophilicity and low biodegradability, they tend to accumulate in sediments. Decabrominated diphenyl ether (BDE-209) is the most predominant congener among 209 PBDE congeners in river sediments, accounting for more than 90 % of total PBDEs in most samples. This study is to explore the feasibility of an integrated remedial approach, direct removal by emulsion recovery and subsequent biological reductive debromination.

Materials and methods

A double emulsion (water in oil in water) was formulated and used in direct recovery of BDE-209 in sediment samples. After this recovery operation, the residual oil left in sediments was used as an electron donor for anaerobic microbial reductive debromination. In order to improve the robustness of this direct recovery method, a variety of operational parameters and environmental variables were tested, such as mixing speed, mixing time, initial concentrations of BDE-209, salinity contents of sediment, and fractions of humic acids. A biodegradation experiment with different humic acid contents and with or without residual emulsion was conducted to compare the biodegradation rates under different conditions. All samples were extracted by using accelerated solvent extraction and detected by a gas chromatography with an electron capture detector.

Results and discussion

In this study, we used an emulsion to recover BDE-209 in simulated sediment samples with different salinity and humic acid contents. BDE-209 was recovered as much as 96.10 % in a single recovery operation under a condition similar to the real situation of Er-Ren River in Taiwan. The biodegradation of unrecovered BDE-209 was assessed under anaerobic conditions with residual emulsion as an electron donor. The average half-life is 11.7 ± 1.9 days with residual emulsion, which is about 40 % shorter than that of those without emulsion and much shorter than those reported in literature. Real sediment samples were also tested and the result indicated that this method is highly feasible.

Conclusions

Emulsion-enhanced recovery and biodegradation could be a highly feasible way to remove BDE-209 in river sediments. This method is not sensitive to the initial concentration of BDE-209 but sensitive to the salinity and humic acid concentration in sediments.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6

Similar content being viewed by others

References

  • Adriaens P, Li MY, Michalak AM (2006) Scaling methods of sediment bioremediation processes and applications. Eng Life Sci 6:217–227. doi:10.1002/elsc.200520127

    Article  CAS  Google Scholar 

  • Allchin CR, Law RJ, Morris S (1999) Polybrominated diphenylethers in sediments and biota downstream of potential sources in the UK. Environ Pollut 105:197–207

    Article  CAS  Google Scholar 

  • An T, Chen J, Li G, Ding X, Sheng G, Fu J, Mai B, O'Shea KE (2008) Characterization and the photocatalytic activity of TiO2 immobilized hydrophobic montmorillonite photocatalysts: degradation of decabromodiphenyl ether (BDE 209). Catal Today 139:69–76

    Article  CAS  Google Scholar 

  • Aschebrook-Kilfoy B, DellaValle CT, Purdue M, Kim C, Zhang Y, Sjodin A, Ward MH (2015) Polybrominated diphenyl ethers and thyroid cancer risk in the prostate, colorectal, lung, and ovarian cancer screening trial cohort. Ame J Epidemiol 181:883–888

    Article  Google Scholar 

  • Beckingham B, Ghosh U (2011) Field-scale reduction of PCB bioavailability with activated carbon amendment to river sediments. Environ Sci Technol 45:10567–10574

    Article  CAS  Google Scholar 

  • Besis A, Samara C (2012) Polybrominated diphenyl ethers (PBDEs) in the indoor and outdoor environments—a review on occurrence and human exposure. Environ Pollut 169:217–229

    Article  CAS  Google Scholar 

  • Bilati U, Allémann E, Doelker E (2003) Sonication parameters for the preparation of biodegradable nanocapsules of controlled size by the double emulsion method. Pharm Dev Technol 8:1–9

    Article  CAS  Google Scholar 

  • BSEF (2009) An introduction to brominated flame retardants. Bromine Science and Environmental Forum. http://www.BSEF.com. Accessed 6 Nov 2015

  • Chang S-C, Chiang P-Y, Yu Y-H, Chen T-W, Luo Y-S, Tsai L-C, Yu K-C (2014) Soybean oil nanoemulsion and magnetite nanoparticle as remediation enhancers for river sediment: from lab to field. J Soil Groundwater Remediat 1:141–164

    Google Scholar 

  • Chao H-R, Wang S-L, Lee W-J, Wang Y-F, Päpke O (2007) Levels of polybrominated diphenyl ethers (PBDEs) in breast milk from central Taiwan and their relation to infant birth outcome and maternal menstruation effects. Environ Int 33:239–245

    Article  CAS  Google Scholar 

  • Chowdhury AK, Stolzenburg TR, Stanforth RR, Warner MA, Larowe ME (1996) Underwater treatment of lead-contaminated sediment. Remediat J 6:15–21

    Article  Google Scholar 

  • Dishaw LV, Macaulay L, Roberts SC, Stapleton HM (2014) Exposures, mechanisms, and impacts of endocrine-active flame retardants. Curr Opin Pharmacol 19:125–133

    Article  Google Scholar 

  • DOE (1994) Handbook of methods for the analysis of the various parameters of the carbon dioxide system in sea water, version 2. In: Dickson AG, Goyet C (eds) ORNL/CDIAC-74

  • Eriksson P, Viberg H, Jakobsson E, Örn U, Fredriksson A (2002) A brominated flame retardant, 2,2′,4,4′,5-pentabromodiphenyl ether: uptake, retention, and induction of neurobehavioral alterations in mice during a critical phase of neonatal brain development. Toxicol Sci 67:98–103

    Article  CAS  Google Scholar 

  • Eskenazi B, Chevrier J, Rauch SA, Kogut K, Harley KG, Johnson C, Trujillo C, Sjödin A, Bradman A (2013) In utero and childhood polybrominated diphenyl ether (PBDE) exposures and neurodevelopment in the CHAMACOS study. Environ Health Perspect 121:257–262

    Article  Google Scholar 

  • Förstner U, Apitz S (2007) Sediment remediation: U.S. focus on capping and monitored natural recovery. J Soils Sediments 7:351–358

    Article  Google Scholar 

  • Gerecke AC, Hartmann PC, Heeb NV, Kohler H-PE, Giger W, Schmid P, Zennegg M, Kohler M (2005) Anaerobic degradation of decabromodiphenyl ether. Environ Sci Technol 39:1078–1083

    Article  CAS  Google Scholar 

  • Hassanin A, Breivik K, Meijer SN, Steinnes E, Thomas GO, Jones KC (2004) PBDEs in European background soils: levels and factors controlling their distribution. Environ Sci Technol 38:738–745

    Article  CAS  Google Scholar 

  • He J-z, Robrock KR, Alvarez-Cohen L (2006) Microbial reductive debromination of polybrominated diphenyl ethers (PBDEs). Environ Sci Technol 40:4429–4434

    Article  CAS  Google Scholar 

  • Huang H-W, Chang B-V, Lee C-C (2014) Reductive debromination of decabromodiphenyl ether by anaerobic microbes from river sediment. Int Biodeterior Biodegradation 87:60–65

    Article  CAS  Google Scholar 

  • Jiang J-J, Lee C-L, Fang M-D, Ko F-C, Baker JE (2011) Polybrominated diphenyl ethers and polychlorinated biphenyls in sediments of southwest Taiwan: regional characteristics and potential sources. Mar Pollut Bull 62:815–823

    Article  CAS  Google Scholar 

  • Keum Y-S, Li QX (2005) Reductive debromination of polybrominated diphenyl ethers by zerovalent iron. Environ Sci Technol 39:2280–2286

    Article  CAS  Google Scholar 

  • Li A, Tai C, Zhao Z, Wang Y, Zhang Q, Jiang G, Hu J (2007) Debromination of decabrominated diphenyl ether by resin-bound iron nanoparticles. Environ Sci Technol 41:6841–6846

    Article  CAS  Google Scholar 

  • McDonald TA (2002) A perspective on the potential health risks of PBDEs. Chemosphere 46:745–755

    Article  CAS  Google Scholar 

  • Moon H-B, Kannan K, Lee S-J, Choi M (2007) Polybrominated diphenyl ethers (PBDEs) in sediment and bivalves from Korean coastal waters. Chemosphere 66:243–251

    Article  CAS  Google Scholar 

  • Moon H-B, Choi M, Yu J, Jung R-H, Choi H-G (2012) Contamination and potential sources of polybrominated diphenyl ethers (PBDEs) in water and sediment from the artificial Lake Shihwa, Korea. Chemosphere 88:837–843

    Article  CAS  Google Scholar 

  • Mulligan CN, Fukue M, Sato Y (2010) Sediment contamination and sustainable remediation. Taylor & Francis Group LLC, London

    Google Scholar 

  • Nyholm JR, Lundberg C, Andersson PL (2010) Biodegradation kinetics of selected brominated flame retardants in aerobic and anaerobic soil. Environ Pollut 158:2235–2240

    Article  CAS  Google Scholar 

  • Peng J-H, Huang C-W, Weng Y-M, Yak H-K (2007) Determination of polybrominated diphenyl ethers (PBDEs) in fish samples from rivers and estuaries in Taiwan. Chemosphere 66:1990–1997

    Article  CAS  Google Scholar 

  • POP Review Committee (2014) Report of the Persistent Organic Pollutants Review Committee on the work of its tenth meeting—decabromodiphenyl ether (commercial mixture, c-decaBDE) risk profile UNEP/UN, Rome

  • Rahman F, Langford KH, Scrimshaw MD, Lester JN (2001) Polybrominated diphenyl ether (PBDE) flame retardants. Sci Total Environ 275:1–17

    Article  CAS  Google Scholar 

  • Robrock KR, Korytár P, Alvarez-Cohen L (2008) Pathways for the anaerobic microbial debromination of polybrominated diphenyl ethers. Environ Sci Technol 42:2845–2852

    Article  CAS  Google Scholar 

  • Roze E, Meijer L, Bakker A, Van Braeckel KNJA, Sauer PJJ, Bos AF (2009) Prenatal exposure to organohalogens, including brominated flame retardants, influences motor, cognitive, and behavioral performance at school age. Environ Health Perspect 117:1953–1958

    Article  CAS  Google Scholar 

  • Shih YH, Tai YT (2010) Reaction of decabrominated diphenyl ether by zerovalent iron nanoparticles. Chemosphere 78:1200–1206

    Article  CAS  Google Scholar 

  • Shih YH, Wang C-K (2009) Photolytic degradation of polybromodiphenyl ethers under UV-lamp and solar irradiations. J Hazard Mater 165:34–38

    Article  CAS  Google Scholar 

  • Smith KEC, Thullner M, Wick LY, Harms H (2009) Sorption to humic acids enhances polycyclic aromatic hydrocarbon biodegradation. Environ Sci Technol 43:7205–7211

    Article  CAS  Google Scholar 

  • Söderström G, Sellström U, de Wit CA, Tysklind M (2004) Photolytic debromination of decabromodiphenyl ether (BDE 209). Environ Sci Technol 38:127–132

    Article  Google Scholar 

  • Taiwan Environmental Protection Administration (2009) The outcome report on the fate and transport of toxic substances in Taiwan. Taiwan Environmental Protection Administration, Taipei

    Google Scholar 

  • Tokarz JA, Ahn M-Y, Leng J, Filley TR, Nies L (2008) Reductive debromination of polybrominated diphenyl ethers in anaerobic sediment and a biomimetic system. Environ Sci Technol 42:1157–1164

    Article  CAS  Google Scholar 

  • Tu L-K, Wu Y-L, Wang L-C, Chang-Chien G-P (2012) Monitoring and dispersion modeling of polybrominated diphenyl ethers (PBDEs) in the ambient air of two municipal solid waste incinerators and a coal-fired power plant. Aerosol Air Qual Res 12:113–122

    CAS  Google Scholar 

  • United States Environmental Protection Agency (2013) Contaminants of emerging concern (CECs) in fish: polybrominated diphenyl ethers (PBDEs). Office of Water, Environmental Protection Agency, Washington DC EPA-820-F-13-003

    Google Scholar 

  • Unknown (2015) Taiwan bans PBDEs used as flame retardants in electronics goods. SGS Taiwan Limited. http://www.sgs.com.tw/en/Local/Taiwan/News-and-Press-Releases/2014/09/N_20140910_2.aspx. Accessed 6 Nov 2015

  • Verslycke TA, Vethaak AD, Arijs K, Janssen CR (2005) Flame retardants, surfactants and organotins in sediment and mysid shrimp of the Scheldt estuary (The Netherlands). Environ Pollut 136:19–31

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This study was funded by a research project supported by the Taiwan Environmental Protection Administration (Taiwan EPA). The views or opinions expressed in this article are those of the writers and should not be construed as opinions of the Taiwan EPA. Mention of trade names, vendor names, or commercial products does not constitute endorsement or recommendation by the Taiwan EPA.

Author information

Authors and Affiliations

  1. Department of Environmental Engineering, National Chung Hsing University, No. 250, Kuo-Kuang Road, Taichung, 40227, Taiwan

    Shu-Chi Chang, Wei-Ting Wang, Yi-Ju Chen, Tzu-Wen Chen, Peng-Yu Chiang & Yun-Sung Lo

Authors
  1. Shu-Chi Chang
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Wei-Ting Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Yi-Ju Chen
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Tzu-Wen Chen
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Peng-Yu Chiang
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Yun-Sung Lo
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Shu-Chi Chang.

Additional information

Responsible editor: Karl J. Rockne

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Chang, SC., Wang, WT., Chen, YJ. et al. Emulsion-enhanced recovery and biodegradation of decabrominated diphenyl ether in river sediments. J Soils Sediments 17, 1197–1207 (2017). https://doi.org/10.1007/s11368-016-1590-3

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11368-016-1590-3

Keywords

Search

Navigation