Technetium reduction and reoxidation behaviour in Dounreay soils.

作者: James D. C. Begg , Ian T. Burke , John M. Charnock , Katherine Morris

DOI: 10.1524/RACT.2008.1547

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摘要: Summary. Technetium is a radioactive contaminant found in groundwaters at sites where nuclear wastes have been processed or stored. The redox chemistry of technetium major control on its environmental mobility. Under oxic conditions, exists as the pertechnetate ion, Tc(VII)O4 − ,w hich poorly sorbed by minerals across wide range environmentally relevant pH values. reducing conditions converted to lower valency species, which Tc(IV) tends predominate. Typically, oxidation state readily precipitates insoluble hydrous oxides or, low concentrations, removed from solution association with mineral surfaces. Here, we present novel X-ray absorption spectroscopy (XAS) data examining Tc associations reduced Dounreay soils. In unamended microcosms and added co-contaminants ethylenediaminetetraacetic acid (EDTA) bicarbonate investigate their effect biogeochemistry, was exposure sediments solids Tc(IV)O2-like phases. Furthermore, long term stability remobilization solid phase associated soils, reoxidized reduced, Tc(IV)-labeled presence air nitrate. extent dependent oxidant used. After reoxidation for 60 d, 42 ± 6% initial soil bound resolubilized. 25 100 mmol L −1 nitrate an oxidant, negligible microcosm occurred. XAS analysis soils treated two oxidants showed that both systems, remaining TcO2like recalcitrance under reoxidizing has implications fate contaminated environments.

参考文章(22)
Derek R. Lovley, Elizabeth J. P. Phillips, Availability of Ferric Iron for Microbial Reduction in Bottom Sediments of the Freshwater Tidal Potomac River Applied and Environmental Microbiology. ,vol. 52, pp. 751- 757 ,(1986) , 10.1128/AEM.52.4.751-757.1986
Sarah E. Pepper, Debbie J. Bunker, Nicholas D. Bryan, Francis R. Livens, John M. Charnock, Richard A.D. Pattrick, David Collison, Treatment of radioactive wastes: an X-ray absorption spectroscopy study of the reaction of technetium with green rust. Journal of Colloid and Interface Science. ,vol. 268, pp. 408- 412 ,(2003) , 10.1016/J.JCIS.2003.08.024
Karrie A. Weber, Flynn W. Picardal, Eric E. Roden, Microbially catalyzed nitrate-dependent oxidation of biogenic solid-phase Fe(II) compounds. Environmental Science & Technology. ,vol. 35, pp. 1644- 1650 ,(2001) , 10.1021/ES0016598
John M. Zachara, Steve M. Heald, Byong-Hun Jeon, Ravi K. Kukkadapu, Chongxuan Liu, James P. McKinley, Alice C. Dohnalkova, Dean A. Moore, Reduction of pertechnetate (Tc(VII)) by aqueous Fe(II) and the nature of solid phase redox products Geochimica et Cosmochimica Acta. ,vol. 71, pp. 2137- 2157 ,(2007) , 10.1016/J.GCA.2006.10.025
R.E. Wildung, S.W. Li, C.J. Murray, K.M. Krupka, Y. Xie, N.J. Hess, E.E. Roden, Technetium reduction in sediments of a shallow aquifer exhibiting dissimilatory iron reduction potential FEMS Microbiology Ecology. ,vol. 49, pp. 151- 162 ,(2004) , 10.1016/J.FEMSEC.2003.08.016
Daqing Cui, Trygve E. Eriksen, Reduction of Pertechnetate in Solution by Heterogeneous Electron Transfer from Fe(II)-Containing Geological Material Environmental Science & Technology. ,vol. 30, pp. 2263- 2269 ,(1996) , 10.1021/ES950627V
Ian T Burke, Christopher Boothman, Jonathon R Lloyd, Robert JG Mortimer, Francis R Livens, Katherine Morris, None, Effects of Progressive Anoxia on the Solubility of Technetium in Sediments Environmental Science & Technology. ,vol. 39, pp. 4109- 4116 ,(2005) , 10.1021/ES048124P
E. A. BONDIETTI, C. W. FRANCIS, Geologic migration potentials of technetium-99 and neptunium-237. Science. ,vol. 203, pp. 1337- 1340 ,(1979) , 10.1126/SCIENCE.203.4387.1337
K Morris, FR Livens, JM Charnock, IT Burke, JM McBeth, JDC Begg, C Boothman, JR Lloyd, None, An X-ray absorption study of the fate of technetium in reduced and reoxidised sediments and mineral phases Applied Geochemistry. ,vol. 23, pp. 603- 617 ,(2008) , 10.1016/J.APGEOCHEM.2007.10.014
James D.C. Begg, Ian T. Burke, Katherine Morris, The behaviour of technetium during microbial reduction in amended soils from Dounreay, UK. Science of The Total Environment. ,vol. 373, pp. 297- 304 ,(2007) , 10.1016/J.SCITOTENV.2006.10.034