Abstract
The removal of 2,4-dinitrotoluene (2,4-DNT) by simultaneous UV-photo(cata)lysis and biodegradation was explored using intimately coupled photolysis/photocatalysis and biodegradation (ICPB) with two novel porous carriers. First, a porous ceramic carrier was used to attach the photocatalyst (TiO2) on its exterior and accumulate biomass in its interior. UV irradiation alone decomposed 71% of the 2,4-DNT in 60 h, and TiO2 catalyst improved the photolysis to 77%. Second, a macroporous sponge carrier was used to strongly adsorb 2,4-DNT and protect microorganisms from 2,4-DNT inhibition and UV irradiation. The main photolytic reactions were reduction of the nitryl to amino and hydrolysis of the amino to release NH +4 . The main biodegradation reactions were oxidative release of NO −3 and accelerated reductive release of NH +4 . ICPB more thoroughly released inorganic N, with nearly equal amounts being oxidized to nitrate and reduced to ammonium. The genera Burkholderia and Bacillus were found inside the sponge carriers, and they are associated with biodegradation of DNT and its photolysis intermediates. Therefore, using an adsorbent and macroporous biofilm carrier enabled the effective removal of 2,4-DNT by ICPB.
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References
Agency for Toxic Substances and Disease Registry (ATSDR) (1989) Toxicological profile for 2,4-dinitrotoluene and 2,6-dinitrotoluene. US Public Health Service, US Department of Health and Human Services
Berchtold SR, Vanderloop SL, Suidan MT, Maloney SW (1995) Treatment of 2,4-dinitrotoluene using a 2-stage system: fluidized-bed anaerobic granular activated carbon reactors and aerobic activated-sludge reactors. Water Environ Res 67:1081–1091
Bin AK, Machniewski P, Sakowicz R, Ostrowska J, Zielinski Z (2001) Degradation of nitroaromatics (MNT, DNT AND TNT) by AOPs. Ozone Sci Eng 23:343–349
Celin SM, Pandit M, Kapoor JC, Sharma RK (2003) Studies on photo-degradation of 2,4-dinitro toluene in aqueous phase. Chemosphere 53:63–69
Chen WS, Lin SZ (2009) Destruction of nitrotoluenes in wastewater by electro-Fenton oxidation. J Hazard Mater 168:1562–1568
Christopher HJ, Boardman GD, Freedman DL (2000) Aerobic biological treatment of 2,4-dinitrotoluene in munitions plant wastewater. Water Res 34:1595–1603
Diehl CA, Jafvert CT, Marley KA, Larson RA (2002) Surfactant-assisted UV-photolysis of nitroarenes. Chemosphere 46:553–560
Dodard SG, Renoux AY, Hawari J, Ampleman G, Thiboutot S, Sunahara GI (1999) Ecotoxicity characterization of dinitrotoluenes and some of their reduced metabolites. Chemosphere 38:2071–2079
Dontsova KM, Pennington JC, Hayes C, Simunek J, Williford CW (2009) Dissolution and transport of 2,4-DNT and 2,6-DNT from M1 propellant in soil. Chemosphere 77:597–603
Doppalapudi RB, Sorial GA, Maloney SW (2003) Electrochemical reduction of 2,4-dinitrotoluene in a continuous flow laboratory scale reactor. J Environ Eng-Asce 129:192–201
Gorontzy T, Drzyzga O, Kahl MW, Brunsnagel D, Breitung J, Vonloew E, Blotevogel KH (1994) Microbial-degradation of explosives and related-compounds. Crit Rev Microbiol 20:265–284
Heinze L, Brosius M, Wiesmann U (1995) Biological degradation of 2,4-dinitrotoluene in a continuous bioreactor and kinetic-studies. Acta Hydroch Hydrob 23:254–263
Hudcova T, Halecky M, Kozliak E, Stiborova M, Paca J (2011) Aerobic degradation of 2,4-dinitrotoluene by individual bacterial strains and defined mixed population in submerged cultures. J Hazard Mater 192:605–613
Hughes JB, Wang CY, Zhang CL (1999) Anaerobic biotransformation of 2,4-dinitrotoluene and 2,6-dinitrotoluene by Clostridium acetobutylicum: a pathway through dihydroxylamino intermediates. Environ Sci Technol 33:1065–1070
Kalafut T, Wales ME, Rastogi VK, Naumova RP, Zaripova SK, Wild JR (1998) Biotransformation patterns of 2,4,6-trinitrotoluene by aerobic bacteria. Curr Microbiol 36:45–54
Kilbane JJ (2005) Metabolic engineering to develop a pathway for the selective cleavage of carbon–nitrogen bonds. Annual technical report. Gas Technology Institute, Des Plaines, pp 13–14
Kumar S, Davis AP (1997) Heterogeneous photocatalytic oxidation of nitrotoluenes. Water Environ Res 69:1238–1245
Kuscu OS, Sponza DT (2011) Application of Box–Wilson experimental design method for 2,4-dinitrotoluene treatment in a sequential anaerobic migrating blanket reactor (AMBR)/aerobic completely stirred tank reactor (CSTR) system. J Hazard Mater 187:222–234
Lee HS, Parameswaran P, Kato-Marcus A, Torres CI, Rittmann BE (2008) Evaluation of energy-conversion efficiencies in microbial fuel cells (MFCs) utilizing fermentable and non-fermentable substrates. Water Res 42:1501–1510
Lendenmann U, Spain JC, Smets BF (1998) Simultaneous biodegradation of 2,4-dinitrotoluene and 2,6-dinitrotoluene in an aerobic fluidized-bed biofilm reactor. Environ Sci Technol 32:82–87
Li LS, Zhang PY, Zhu WP, Han WY, Zhang ZL (2005) Comparison of O-3-BAC, UV/O-3-BAC and TiO2/UV/O-3-BAC processes for removing organic pollutants in secondary effluents. J Photoch Photobio A 171:145–151
Marsolek MD, Torres CI, Hausner M, Rittmann BE (2008) Intimate coupling of photocatalysis and biodegradation in a photocatalytic circulating-bed biofilm reactor. Biotechnol Bioeng 101:83–92
Mccormick NG, Cornell JH, Kaplan AM (1978) Identification of biotransformation products from 2,4-dinitrotoluene. Appl Environ Microb 35:945–948
Nasr MA, Hwang KW, Akbas M, Webster DA, Stark BC (2001) Effects of culture conditions on enhancement of 2,4-dinitrotoluene degradation by Burkholderia engineered with the Vitreoscilla hemoglobin gene. Biotechnol Progr 17:359–361
Nishino SF, Spain JC, Lenke H, Knackmuss HJ (1999) Mineralization of 2,4- and 2,6-dinitrotoluene in soil slurries. Environ Sci Technol 33:1060–1064
Noguera DR, Freedman DL (1996) Reduction and acetylation of 2,4-dinitrotoluene by a Pseudomonas aeruginosa strain. Appl Environ Microb 62:2257–2263
Paca J, Halecky M, Barta J, Bajpai R (2009) Aerobic biodegradation of 2,4-DNT and 2,6-DNT: performance characteristics and biofilm composition changes in continuous packed-bed bioreactors. J Hazard Mater 163:848–854
Rajagopal C, Kapoor JC (2001) Development of adsorptive removal process for treatment of explosives contaminated wastewater using activated carbon. J Hazard Mater 87:73–98
Sambrook J, Russell D (2001) Molecular cloning: a laboratory manual, 3rd edn. Cold Spring Harbor Laboratory, New York
Spanggord RJ, Spain JC, Nishino SF, Mortelmans KE (1991) Biodegradation of 2,4-dinitrotoluene by a Pseudomonas sp. Appl Environ Microb 57:3200–3205
Spiegel K, Headley JV, Peru KM, Haidar N, Gurprasard NP (2005) Residues of explosives in groundwater leached from soils at a military site in Eastern Germany. Commun Soil Sci Plan 36:133–153
Suen WC, Spain JC (1993) Cloning and characterization of Pseudomonas sp strain Dnt genes for 2,4-dinitrotoluene degradation. J Bacteriol 175:1831–1837
Suen WC, Haigler BE, Spain JC (1996) Dinitrotoluene dioxygenase from Burkholderia sp strain DNT: similarity to naphthalene dioxygenase. J Bacteriol 178:4926–4934
Tamura K, Dudley J, Nei M, Kumar S (2007) MEGA4: molecular evolutionary genetics analysis (MEGA) software version 4.0. Mol Biol Evol 24:1596–1599
Thiruvenkatachari R, Vigneswaran S, Moon IS (2008) A review on UV/TiO2 photocatalytic oxidation process. Korean J Chem Eng 25:64–72
US Department of Health and Human Services (USDHHS) (1993) Registry of toxic effects of chemical substances (RTECS, online database). National Toxicology Information Program, National Library of Medicine, Bethesda
US Environmental Protection Agency (USEPA) (1988) Health effects assessment for 2,4- and 2,6-dinitrotoluene. EPA/600/8-88/032. Environmental Criteria and Assessment Office, Office of Health and Environmental Assessment, Office of Research and Development, Cincinnati
Vanderloop SL, Suidan MT, Moteleb MA, Maloney SW (1999) Biotransformation of 2,4-dinitrotoluene under different electron acceptor conditions. Water Res 33:1287–1295
Zhang YM, Liu H, Shi W, Pu XJ, Zhang HS, Rittmann BE (2010) Photobiodegradation of phenol with ultraviolet irradiation of new ceramic biofilm carriers. Biodegradation 21:881–887
Acknowledgements
This study was supported by the US National Science Foundation (Grant No. 0651794) and China Scholarship Council. We sincerely thank Prof. Yongming Zhang at Shanghai Normal University, China, for kindly providing the ceramic carriers and Samsung Engineering Co. Ltd, Korea, for kindly providing the sponge carriers. We also thank Bradley Lusk, who helped in DNA sequencing analysis, and Dr. Rosa Krajmalnik-Brown, who provided guidance and facilities for phylogenetic analysis.
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Wen, D., Li, G., Xing, R. et al. 2,4-DNT removal in intimately coupled photobiocatalysis: the roles of adsorption, photolysis, photocatalysis, and biotransformation. Appl Microbiol Biotechnol 95, 263–272 (2012). https://doi.org/10.1007/s00253-011-3692-6
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DOI: https://doi.org/10.1007/s00253-011-3692-6