Skip to main content
Log in

Enhanced anaerobic biodegradation of BTEX-ethanol mixtures in aquifer columns amended with sulfate, chelated ferric iron or nitrate

  • Published:
Biodegradation Aims and scope Submit manuscript

Abstract

Flow-through aquifer columns were used to investigate the feasibility of adding sulfate, EDTA–Fe(III) or nitrate to enhance the biodegradation of BTEX and ethanol mixtures. The rapid biodegradation of ethanol near the inlet depleted the influent dissolved oxygen (8 mg l-1), stimulated methanogenesis, and decreased BTEX biodegradation efficiencies from >99% in the absence of ethanol to an average of 32% for benzene, 49% for toluene, 77% for ethylbenzene, and about 30% for xylenes. The addition of sulfate, EDTA–Fe(III) or nitrate suppressed methanogenesis and significantly increased BTEX biodegradation efficiencies. Nevertheless, occasional clogging was experienced by the column augmented with EDTA–Fe(III) due to iron precipitation. Enhanced benzene biodegradation (>70% in all biostimulated columns) is noteworthy because benzene is often recalcitrant under anaerobic conditions. Influent dissolved oxygen apparently played a critical role because no significant benzene biotransformation was observed after oxygen was purged out of the influent media. The addition of anaerobic electron acceptors could enhance BTEX biodegradation not only by facilitating their anaerobic biodegradation but also by accelerating the mineralization of ethanol or other substrates that are labile under anaerobic conditions. This would alleviate the biochemical oxygen demand (BOD) and increase the likelihood that entraining oxygen would be used for the biotransformation of residual BTEX.

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

Access this article

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

Instant access to the full article PDF.

Similar content being viewed by others

References

  • U Altenschmidt G Fuchs (1991) ArticleTitleAnaerobic degradation of toluene in denitrifying Pseudomonas sp–indication for toluene methylhydroxylation and benzoyl-Coa as central aromatic intermediate Arch. Microbiol. 156 152–158 Occurrence Handle1:CAS:528:DyaK3MXlsFCktb8%3D

    CAS  Google Scholar 

  • PJJ Alvarez LA Cronkhite CS Hunt (1998) ArticleTitleUse of benzoate to establish reactive buffer zones for enhanced attenuation of BTX migration: Aquifer column experiments Environ. Sci. Technol. 32 509–515 Occurrence Handle1:CAS:528:DyaK1cXjsVGgsg%3D%3D

    CAS  Google Scholar 

  • PJJ Alvarez TM Vogel (1995) ArticleTitleDegradation of BTEX and their aerobic metabolites by indigenous microorganisms under nitrate-reducing conditions Water Sci. Technol. 31 15–28 Occurrence Handle1:CAS:528:DyaK2MXns1Cmsbc%3D

    CAS  Google Scholar 

  • RT Anderson DR Lovley (1997) ArticleTitleEcology and biogeochemistry of in situ groundwater bioremediation Adv. Microb. Ecol. 15 289–350 Occurrence Handle1:CAS:528:DyaK1cXktFGm

    CAS  Google Scholar 

  • RT Anderson DR Lovley (2000) ArticleTitleAnaerobic bioremediation of benzene under sulfate-reducing conditions in a petroleum-contaminated aquifer Environ. Sci. Technol. 34 2261–2266 Occurrence Handle1:CAS:528:DC%2BD3cXitlyqt7Y%3D

    CAS  Google Scholar 

  • PJ Anid PJJ Alvarez TM Vogel (1993) ArticleTitleBiodegradation of monoaromatic hydrocarbons in aquifer columns amended with hydrogen-peroxide and nitrate Water Res. 27 685–691 Occurrence Handle1:CAS:528:DyaK3sXisVShurk%3D

    CAS  Google Scholar 

  • RM Atlas R Bartha (1998) Microbial Ecology: Fundamentals and Applications EditionNumber4 Benjamin Cummings Menlo Park, California 694

    Google Scholar 

  • HA Ball M Reinhard (1996) ArticleTitleMonoaromatic hydrocarbon transformation under anaerobic conditions at Seal Beach, California: Laboratory studies Environ. Toxicol. Chem. 15 114–122 Occurrence Handle1:CAS:528:DyaK28XpsFyntA%3D%3D

    CAS  Google Scholar 

  • G Bratbak (1985) ArticleTitleBacterial biovolume and biomass estimations Appl. Environ. Microbiol. 49 1488–1493

    Google Scholar 

  • G Bratbak I Dundas (1984) ArticleTitleBacterial dry-matter content and biomass estimations Appl. Environ. Microbiol. 48 755–757 Occurrence Handle1:STN:280:DyaL2M%2FntFWjsw%3D%3D

    CAS  Google Scholar 

  • SM Burland EA Edwards (1999) ArticleTitleAnaerobic benzene biodegradation linked to nitrate reduction Appl. Environ. Microbiol. 65 529–533 Occurrence Handle1:CAS:528:DyaK1MXpvFClug%3D%3D

    CAS  Google Scholar 

  • TP Clement BS Hooker RS Skeen (1996) ArticleTitleMacroscopic models for predicting changes in saturated porous media properties caused by microbial growth Ground Water 34 934–942 Occurrence Handle1:CAS:528:DyaK28XlsVahsb0%3D

    CAS  Google Scholar 

  • JD Coates RT Anderson DR Lovley (1996) ArticleTitleOxidation of polycyclic aromatic hydrocarbons under sulfate-reducing conditions Appl. Environ. Microbiol. 62 1099–1101 Occurrence Handle1:CAS:528:DyaK28XhsVWqt7o%3D

    CAS  Google Scholar 

  • JD Coates R Chakraborty JG Lack SM O’Connor KA Cole KS Bender LA Achenbach (2001) ArticleTitleAnaerobic benzene oxidation coupled to nitrate reduction in pure culture by two strains of Dechloromonas Nature 411 1039–1043 Occurrence Handle1:CAS:528:DC%2BD3MXltVCku7o%3D

    CAS  Google Scholar 

  • AB Cunningham WG Characklis F Abedeen D Crawford (1991) ArticleTitleInfluence of biofilm accumulation on porous-media hydrodynamics Environ. Sci. Technol. 25 1305–1311 Occurrence Handle1:CAS:528:DyaK3MXkt1OltLg%3D

    CAS  Google Scholar 

  • JA Cunningham H Rahme GD Hopkins C Lebron M Reinhard (2001) ArticleTitleEnhanced in situ bioremediation of BTEX contaminated groundwater by combined injection of nitrate and sulfate Environ. Sci. Technol. 35 1663–1670 Occurrence Handle1:CAS:528:DC%2BD3MXhvVKisbY%3D

    CAS  Google Scholar 

  • JA Cunningham M Reinhard (2002) ArticleTitleInjection-extraction treatment well pairs: an alternative to permeable reactive barriers Ground Water 40 599–607 Occurrence Handle1:CAS:528:DC%2BD38XosF2mtbs%3D

    CAS  Google Scholar 

  • MLB Silva ParticleDa PJJ Alvarez (2002) ArticleTitleEffects of ethanol versus MTBE on benzene, toluene, ethylbenzene, and xylene natural attenuation in aquifer columns J. Environ. Eng.-ASCE 128 862–867

    Google Scholar 

  • PA Domenico FW Schwartz (1998) Physical and Chemical Hydrogeology Wiley New York, NY

    Google Scholar 

  • LPW Durant PC D’Adamo EJ Bouwer (1999) ArticleTitleAromatic hydrocarbon biodegradation with mixtures of O2 and NO -3 as electron acceptors Environ. Eng. Sci. 16 487–500 Occurrence Handle10.1089/ees.1999.16.487 Occurrence Handle1:CAS:528:DyaK1MXnslKqsbY%3D

    Article  CAS  Google Scholar 

  • EA Edwards D Grbić-Galić (1992) ArticleTitleComplete mineralization of benzene by aquifer microorganisms under strictly anaerobic conditions Appl. Environ. Microbiol. 58 2663–2666 Occurrence Handle1:CAS:528:DyaK38XlsVKqsLY%3D

    CAS  Google Scholar 

  • M Ficker K Krastel S Orlicky E Edwards (1999) ArticleTitleMolecular characterization of a toluene-degrading methanogenic consortium Appl. Environ. Microbiol. 65 5576–5585 Occurrence Handle1:CAS:528:DyaK1MXnvVGju78%3D

    CAS  Google Scholar 

  • KT Finneran DR Lovley (2001) ArticleTitleAnaerobic degradation of methyl tert-butyl ether (MTBE) and tert-butyl alcohol (TBA) Environ. Sci. Technol. 35 1785–1790 Occurrence Handle1:CAS:528:DC%2BD3MXit1Cks70%3D

    CAS  Google Scholar 

  • D Freedman R Pisani R Purves (1998) Tests of significance Statistics WW Norton & Co. Inc. New York

    Google Scholar 

  • JR Haas TJ Dichristina (2002) ArticleTitleEffects of Fe(III) chemical speciation on dissimilatory Fe(III) reduction by Shewanella putrefaciens Environ. Sci. Technol. 36 IssueID3 373–380 Occurrence Handle1:CAS:528:DC%2BD38XhsVWhsA%3D%3D

    CAS  Google Scholar 

  • J Heider AM Spormann HR Beller F Widdel (1998) ArticleTitleAnaerobic bacterial metabolism of hydrocarbons FEMS Microbiol. Rev. 22 459–473 Occurrence Handle1:CAS:528:DyaK1MXksFCquw%3D%3D

    CAS  Google Scholar 

  • SR Hutchins (1991) ArticleTitleBiodegradation of monoaromatic hydrocarbons by aquifer microorganisms using oxygen, nitrate, or nitrous-oxide as the terminal electron-acceptor Appl. Environ. Microbiol. 57 2403–2407 Occurrence Handle1:CAS:528:DyaK38XitlWms74%3D

    CAS  Google Scholar 

  • SR Hutchins DE Miller A Thomas (1998) ArticleTitleCombined laboratory/field study on the use of nitrate for in situ bioremediation of a fuel-contaminated aquifer Environ. Sci. Technol. 32 1832–1840 Occurrence Handle1:CAS:528:DyaK1cXivVaqsr0%3D

    CAS  Google Scholar 

  • SR Hutchins GW Sewell DA Kovacs GA Smith (1991) ArticleTitleBiodegradation of aromatic-hydrocarbons by aquifer microorganisms under denitrifying conditions Environ. Sci. Technol. 25 68–76 Occurrence Handle1:CAS:528:DyaK3MXivFOltw%3D%3D

    CAS  Google Scholar 

  • D Johnson T Mizoguchi (1978) ArticleTitleSelecting the kth element in x + y and x1 + x2 +···+ xm SIAM J. Comput. 7 147–153

    Google Scholar 

  • J Kazumi ME Caldwell JM Suflita DR Lovley LY Young (1997) ArticleTitleAnaerobic degradation of benzene in diverse anoxic environments Environ. Sci. Technol. 31 813–818 Occurrence Handle1:CAS:528:DyaK2sXotVWluw%3D%3D

    CAS  Google Scholar 

  • Lehmann E (1975) Nonparametrics. Statistical Methods Based on Ranks. Holden-Day.

  • DR Lovley JC Woodward FH Chapelle (1994) ArticleTitleStimulated anoxic biodegradation of aromatic-hydrocarbons using Fe(III) ligands Nature 370 128–131 Occurrence Handle1:CAS:528:DyaK2cXkvFWis7w%3D

    CAS  Google Scholar 

  • DR Lovley JC Woodward FH Chapelle (1996) ArticleTitleRapid anaerobic benzene oxidation with a variety of chelated Fe(III) forms Appl. Environ. Microbiol. 62 288–291 Occurrence Handle1:CAS:528:DyaK28XitFeksQ%3D%3D

    CAS  Google Scholar 

  • DW Major CI Mayfield JF Baker (1991) ArticleTitleBiotransformation of benzene by denitrification in aquifer sand Groundwater 26 8–14

    Google Scholar 

  • P Morgan ST Lewis RJ Watkinson (1993) ArticleTitleBiodegradation of benzene, toluene, ethylbenzene and xylenes in gas-condensate-contaminated groundwater Environ. Pollut. 82 181–190 Occurrence Handle1:CAS:528:DyaK3sXmtFSjsr0%3D

    CAS  Google Scholar 

  • National Research Council (2000) Natural Attenuation for Groundwater Remediation. National Academy of Sciences Washington, DC

  • SE Powers CS Hunt SE Heermann HX Corseuil D Rice PJJ Alvarez (2001a) ArticleTitleThe transport and fate of ethanol and BTEX in groundwater contaminated by gasohol Crit. Rev. Environ. Sci. Technol. 31 79–123 Occurrence Handle1:CAS:528:DC%2BD3MXhtlygu7s%3D

    CAS  Google Scholar 

  • SE Powers D Rice B Dooher PJJ Alvarez (2001b) ArticleTitleWill ethanol-blended gasoline affect groundwater quality? Using ethanol instead of MTBE as a gasoline oxygenate could be less harmful to the environment Environ. Sci. Technol. 35 24A–30A Occurrence Handle1:CAS:528:DC%2BD3MXhsVGjsQ%3D%3D Occurrence Handle10.1021/es012247h

    Article  CAS  Google Scholar 

  • PSC Rao LS Lee R Pinal (1990) ArticleTitleCosolvency & sorption of hydrophobic organic-chemicals Environ. Sci. Technol. 24 647–654 Occurrence Handle1:CAS:528:DyaK3cXhslOnu7g%3D

    CAS  Google Scholar 

  • M Reinhard S Shang PK Kitanidis E Orwin GD Hopkins CA Lebron (1997) ArticleTitleIn situ BTEX biotransformation under enhanced nitrate- and sulfate-reducing conditions Environ. Sci. Technol. 31 28–36 Occurrence Handle1:CAS:528:DyaK28XntVOqu74%3D

    CAS  Google Scholar 

  • BE Rittmann PL McCarty (2001) Environmental Biotechnology: Principles and Applications McGraw-Hill Inc. New York, NY

    Google Scholar 

  • GML Ruiz-Aguilar JM Fernandez-Sanchez SR Kane D Kim PJJ Alvarez (2002a) ArticleTitleEffect of ethanol and methyl-tert-butyl ether on monoaromatic hydrocarbon biodegradation: response variability for different aquifer materials under various electron-accepting conditions Environ. Toxicol. Chem. 21 2631–2639 Occurrence Handle1:CAS:528:DC%2BD38XovFOgsrk%3D

    CAS  Google Scholar 

  • GML Ruiz-Aguilar K O’Reilly PJJ Alvarez (2002b) ArticleTitleA comparison of benzene and toluene plume lengths for sites contaminated with regular vs ethanol-amended gasoline Ground Water Monit. R. 23 48–53 Occurrence Handle1:CAS:528:DC%2BD3sXitVWrsLk%3D

    CAS  Google Scholar 

  • RP Schwarzenbach OM Gschwend DM Imboden (1993) Environmental Organic Chemistry John Wiley & Sons New York, NY

    Google Scholar 

  • United States Environmental protection (2004) Washington, DC 20460 Mail Code 5401G.

  • U Gunten ParticleVon J Zobrist (1993) ArticleTitleBiogeochemical changes in groundwater-infiltration systems - column studies Geochim. Cosmochim. Acta 57 3895–3906

    Google Scholar 

  • JM Weiner DR Lovley (1998) ArticleTitleAnaerobic benzene degradation in petroleum-contaminated aquifer sediments after inoculation with a benzene-oxidizing enrichment Appl. Environ. Microb. 64 775–778 Occurrence Handle1:CAS:528:DyaK1cXpsVWhsg%3D%3D

    CAS  Google Scholar 

  • L Yerushalmi MF Manuel SR Guiot (1999) ArticleTitleBiodegradation of gasoline and BTEX in a microaerophilic biobarrier Biodegradation 10 341–352 Occurrence Handle1:CAS:528:DC%2BD3cXksFSltb4%3D

    CAS  Google Scholar 

Download references

Author information

Authors and Affiliations

Authors

Rights and permissions

Reprints and permissions

About this article

Cite this article

Da Silva, M.L.B., Ruiz-Aguilar, G.M.L. & Alvarez, P.J.J. Enhanced anaerobic biodegradation of BTEX-ethanol mixtures in aquifer columns amended with sulfate, chelated ferric iron or nitrate. Biodegradation 16, 105–114 (2005). https://doi.org/10.1007/s10532-004-4897-5

Download citation

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10532-004-4897-5

Keywords

Navigation