Elsevier

Chemosphere

Volume 67, Issue 9, April 2007, Pages 1831-1837
Chemosphere

Polybrominated diphenyl ether in sewage sludge in Germany

https://doi.org/10.1016/j.chemosphere.2006.05.113Get rights and content

Abstract

Sewage sludge samples from 11 municipal waste water treatment plants in Germany were collected from March 2002 to June 2003. Total Tri- to HpBDE concentrations (sum of significant congeners BDE 28, 47, 99, 153, 154 and 183) ranged from 12.5 to 288 (median 108) and DeBDE (BDE 209) concentrations from 97.1 to 2217 (median 256) ng/g d.m. BDE 209 dominated the congener profile. A significant change of the Tri- to HpBDE congener profile (% of total BDE 28, 47, 99, 153, 154, 183 without 209) in sludge from different stages of the waste water treatment process (primary sludge, secondary excess sludge and (dewatered) digested sludge), indicating a degradation of DeBDE to these congeners, was not observed.

Introduction

With the rapidly growing use of combustible polymer material, e.g. for IT/TV casings, mattresses, upholstered furniture, the use of flame retardants like polybrominated diphenyl ethers (PBDE) has also increased strongly.

PBDE are available as three commercial mixtures of BDE congeners named after their principal component: PeBDE (European and North American usage in 2001 150 and 7.100 t/a), OcBDE (610 and 1.500 t/a) and DeBDE (7.600 and 24.500 t/a). North America accounts for approximatively 95% of the global demand for PeBDE based on this data (BSEF, 2005). PBDEs can release into the environment during their production, use or after disposal and have become ubiquitous. Because of exponentially increasing levels of the dominating congeners of technical Pe- and OcBDE in human blood and milk, the use and sale of preparations and articles containing these two flame retardants in concentrations >0.1% by mass are prohibited from August 15, 2004 in the European Union (EU, 2003). PBDE are subject to regulation and legislation in many countries (BSEF, 2005, NCEL, 2005). The main North American manufacturer of PeBDE flame retardant has voluntarily ceased production by the end of 2004 (Tullo, 2003). DeBDE EU risk assessment was closed on May 26, 2004. It will be reviewed, if after voluntary emission reduction new data from a monitoring programme lasting for 6 years with a possible extension to 10 years, are available (EU, 2004). It was concluded that there is a need for further information on the possible degradation of DeBDE to more toxic and bioaccumulative compounds. In a paper recently presented on BFR 2004, the anaerobic degradation of DeBDE to No- and OcBDE in incubation experiments with sewage sludge over a period of 114 days was studied (Gerecke et al., 2004, Gerecke et al., 2005).

The objective of this study is to get more information about the actual levels and time trend of PBDE in sewage sludge in Germany to ascertain whether there is degradation of DeBDE to lower brominated congeners during waste water treatment process.

Section snippets

Sampling

Thirty-nine sewage sludge samples from different stages of the waste water treatment process (primary sludge, secondary excess sludge and (dewatered) digested sludge) (Fig. 1) were collected from 11 municipal waste water treatment plants (WWTP) of the Rhine-Main area in Germany from March 2002 to June 2003. The capacity of the WWTP investigated ranged from 45 000 to 1 820 000 population equivalents (Table 1).

Analysis

The complete sewage sludge sample was sterilized in an autoclave for 20 min at 121 °C, an

Results and discussion

The total concentration of BDE 28, 47, 99, 100, 153 and 154 the dominating congeners of technical PeBDE and BDE 183, the dominating congener of technical OcBDE, ranges from 12.5 to 288 (median 108) ng/g d.m. (Table 2). With the increasing use of flame retardant polymer material the median level has risen 13 fold since the report from Germany in 1992 (total Tri- to HpBDE 0.5 to 17.7 (median 8.4, n = 13), not designated which congeners) (Hagenmaier et al., 1992). An increasing time trend was also

Acknowledgement

We appreciate the good collaboration with the operators of the WWTP.

References (33)

  • EU, 2004. Update of the risk assessment of bis(pentabromophenyl)ether (decabromodiphenyl ether). Final environmental...
  • B. Fabrellas et al.

    Presence of polybrominated diphenyl ethers in Spanish sewage sludges: important contribution of Deca-BDE

    Organohalogen Compounds

    (2004)
  • Gerecke, A.C., Schmid, P., Heeb, N.V., Zennegg, M., Hartmann, P.C., Kohler, H.-P., Kohler, M., 2004. Formation of lower...
  • A.C. Gerecke et al.

    Anaerobic degradation of decabromodiphenyl ether

    Environmental Science and Technology

    (2005)
  • R.C. Hale et al.

    Flame retardants – persistent pollutants in land-applied sludges

    Nature

    (2001)
  • S. Hamm et al.

    Polybrominated diphenyl ethers in sewage sludge and effluents of sewage plants from a central region of Germany

    Organohalogen Compounds

    (2004)
  • Cited by (103)

    View all citing articles on Scopus
    View full text