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Incorporation of Radioactive Contaminants into Pyroaurite-Like Phases by Electrochemical Synthesis

Published online by Cambridge University Press:  28 February 2024

Y. Roh ,
S. Y. Lee ,
M. P. Elless  and
J. E. Foss
Y. Roh*
Affiliation:
Department of Plant and Soil Sciences, The University of Tennessee, Knoxville, Tennessee 37996, USA
S. Y. Lee
Affiliation:
Environmental Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
M. P. Elless
Affiliation:
Edenspace System Corporation, Reston, Virginia 20191, USA
J. E. Foss
Affiliation:
Department of Plant and Soil Sciences, The University of Tennessee, Knoxville, Tennessee 37996, USA
*
†Present address: Environmental Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831-6038, USA.
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Abstract

During electrochemical remediation of radionuclide, 235U, 238U, and 99Tc-contaminated aqueous solutions, pyroaurite-like phases, ideally [M(II)M(III)(OH)16CO3·4H2O] where M = Fe, were synthesized following coprecipitation with iron from metal iron electrodes. The effect of radionuclides on the transformation of amorphous precipitates to crystalline pyroaurite-like phases was investigated using X-ray diffraction (XRD), scanning electron microscopy with energy dispersive X-ray analysis, Fourier-transform infrared (FTIR) spectroscopy, and fluorescence spectroscopy. The synthetic iron carbonate hydroxide phases showed primary XRD peaks at 0.7 and 0.35 nm and FTIR spectra that indicated the presence of a brucite-like sheet structure with carbonate anions occupying the interlayer. Divalent and trivalent iron, eroded from the electrode, occupies the octahedral sites of the brucite-like sheets. The carbonate anions in the interlayer balance the excess positive charge from isomorphous substitution of the Fe2+ or Fe3+ by reduced uranium (U4+) and technetium (Tc4+). Because of the lower solubility associated with crystalline phases than amorphous phases, incorporation of radioactive contaminants into pyroaurite-like phases by electrochemical syntheses represents a more effective approach for removing U and Tc from contaminated aqueous solutions than traditional technologies.

Keywords

CoprecipitationGroundwater RemediationPyroauriteTechnetiumUraniumZero-Valent Iron
Type
Research Article
Information
Clays and Clay Minerals , Volume 48 , Issue 2 , April 2000 , pp. 266 - 271
Copyright
Copyright © 2000, The Clay Minerals Society

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References

Bish, D.L., 1977 The occurrence and crystal chemistry of nickel in silicate and hydroxide minerals Pennsylvania The Pennsylvania State University, University Park.Google Scholar
Brewster, M.D. and Passmore, R.J., 1994 Use of electrochemical iron generation for removing heavy metals from contaminated groundwater Environmental Progress 13 143–148 10.1002/ep.670130221.CrossRefGoogle Scholar
Brown, G. and Brown, G.W., 1980 Associated minerals The X-ray Identification and Crystal Structures of Clay Minerals 2nd edition London Mineralogical Society 361–410.CrossRefGoogle Scholar
Cantrell, K.J. Kaplan, D.I. and Wietsma, T.W., 1995 Zerovalent liron for the in situ remediation of selected metals in groundwater Journal of Hazardous Materials 42 201–212 10.1016/0304-3894(95)00016-N.CrossRefGoogle Scholar
Cutshall, N.H. and Larsen, I.L., 1980 BGSUB and BGFIX: Fortran programs to correct Ge(Li) gamma-ray spectra for photopeaks from radionuclides in background Oak Ridge, Tennessee Oak Ridge National Laboratory 10.2172/5349290.CrossRefGoogle Scholar
Dai, S. Xu, W. Metcalf, D.H. and Toth, L.M., 1996 Energy transfer between UO2 2+ and Eu3+ in sol-gel glasses: A spectroscopic investigation Chemical Physics Letters 262 315–320 10.1016/0009-2614(96)01088-3.CrossRefGoogle Scholar
Erbs, M. Hansen, H.C.B. and Olsen, C.E., 1999 Reductive dechlorination of carbon tetrachloride using iron(II) and iron(III) hydroxide sulfate (green rust) Environmental Science and Technology 33 307–311 10.1021/es980221t.CrossRefGoogle Scholar
Farmer, V.C., 1974 The Infrared Spectra of Minerals London Mineralogical Society 10.1180/mono-4.CrossRefGoogle Scholar
Gu, B. Liang, L. Dickey, M.J. Yin, X. and Dai, S., 1998 Reductive precipitation of uranium(VI) by zero-valent iron Environmental Science and Technology 32 3366–3373 10.1021/es980010o.CrossRefGoogle Scholar
Hansen, H.C.B., 1989 Composition, stabilization, and light absorption of Fe(II)-Fe(III) hydroxy carbonate (green rust) Clay Minerals 24 663–669 10.1180/claymin.1989.024.4.08.CrossRefGoogle Scholar
Hansen, H.C.B. Borggaard, O.K. and Sorensen, J., 1994 Evaluation of the free energy of formation of Fe(II)-Fe(III) hydroxide-sulfate (green rust) and its reduction of nitrite Geochimica et Cosmochimica Acta 12 2599–2608 10.1016/0016-7037(94)90131-7.CrossRefGoogle Scholar
Hansen, H.C.B. Koch, C.B. Nancke-Krogh, H. Borggaard, O.K. and Sorensen, J., 1996 Abiotic nitrate reduction to ammonium: Key role of green rust Environmental Science and Technology 30 2053–2056 10.1021/es950844w.CrossRefGoogle Scholar
Huang, C.K. and Kerr, P.F., 1960 Infrared study of the carbonate minerals American Mineralogist 45 311–324.Google Scholar
Koch, C.B. Hansen, H.C.B. and Lee, S.Y., 1996 On the reaction of pyroaurite with glycerol Abstract, Annual Meeting of the Clay Minerals Society, June 15–20, Gatlinberg, Tennessee 96.Google Scholar
Langmuir, D., 1978 Uranium solution-mineral equilibria at low temperatures with applications to sedimentary ore deposits Geochimica et Cosmochimica Acta 42 547–569 10.1016/0016-7037(78)90001-7.CrossRefGoogle Scholar
Lee, S.Y. and Bondietti, E.A., 1983 Removing uranium from drinking water by metal hydroxide and anion exchange resin Journal of American Water Work Association 75 537–540.Google Scholar
Myneni, S.C.B. Tokunaga, T.K. and Brown, G.E., 1997 Abiotic selenium redox transformation in the presence of Fe(II,III) oxides Science 278 1106–1109 10.1126/science.278.5340.1106.CrossRefGoogle Scholar
Nakamoto, K., 1997 Theory and applications of inorganic chemistry. Part A Infrared and Raman Spectra of Inorganic and Coordination Compounds 5th edition New York John Wiley & Sons, Inc..Google Scholar
Roh, Y. Lee, S.Y. Elless, M.P. and Tedder, D.U., 1996 Electroremediation of uranium and technetium contaminated waters Extended Abstract, Annual Meeting of the Chemical Society, I&EC Division, Emerging Technologies in Hazardous Waste Management VIII, Sept., 9–12, 1996, Birmingham, Alabama 582–585.Google Scholar
Schwertmann, U. and Cornell, R.M., 1991 Iron Oxides in the Laboratory New York VCH Publishers, Inc..Google Scholar
Smith, E.H., 1996 Uptake of heavy metals in batch systems by a recycled iron-bearing material Water Research 30 2424–2434 10.1016/0043-1354(96)00105-4.CrossRefGoogle Scholar
Sorg, T.J., Cothern, C.R. and Revers, P.A., 1990 Removal of uranium from drinking water by conventional treatment methods Radon, Radium and Uranium in Drinking Water Michigan Lewis Publishers, Inc. Chelsea.Google Scholar
Taylor, R.M., 1980 Formation and properties of Fe(II)Fe(III) hydroxycarbonate and its possible significance in soil formation Clay Minerals 15 369–382 10.1180/claymin.1980.015.4.04.CrossRefGoogle Scholar
Young, R.S., 1961 Cobalt: Its Chemistry, Metallurgy, and Uses New York Reinhold Publication Corporation.Google Scholar