Hostname: page-component-cd9895bd7-hc48f Total loading time: 0 Render date: 2024-12-27T10:38:34.442Z Has data issue: false hasContentIssue false
  • English
  • Français

Alteration of Kaolinite to Cancrinite and Sodalite by Simulated Hanford Tank Waste and its Impact on Cesium Retention

Published online by Cambridge University Press:  01 January 2024

Hongting Zhao ,
Youjun Deng ,
James B. Harsh ,
Markus Flury  and
Jeffrey S. Boyle
Hongting Zhao
Affiliation:
Department of Crop and Soil Sciences, Center for Multiphase Environmental Research, Washington State University, Pullman, WA 99164 USA
Youjun Deng
Affiliation:
Department of Crop and Soil Sciences, Center for Multiphase Environmental Research, Washington State University, Pullman, WA 99164 USA
James B. Harsh
Affiliation:
Department of Crop and Soil Sciences, Center for Multiphase Environmental Research, Washington State University, Pullman, WA 99164 USA
Markus Flury*
Affiliation:
Department of Crop and Soil Sciences, Center for Multiphase Environmental Research, Washington State University, Pullman, WA 99164 USA
Jeffrey S. Boyle
Affiliation:
Department of Crop and Soil Sciences, Center for Multiphase Environmental Research, Washington State University, Pullman, WA 99164 USA
*
*E-mail address of corresponding author: flury@mail.wsu.edu
Rights & Permissions [Opens in a new window]

Abstract

Core share and HTML view are not available for this content. However, as you have access to this content, a full PDF is available via the ‘Save PDF’ action button.

Caustic nuclear wastes have leaked from tanks at the US Department of Energy’s Hanford site in Washington State (USA) causing hundreds of thousands of gallons of waste fluids to migrate into the underlying sediments. In this study, four simulant tank waste (STW) solutions, which are high in NaOH (1.4 and 2.8 mol/kg), NaNO3 (3.7 mol/kg) and NaAlO2 (0.125 and 0.25 mol/kg), were prepared and reacted with reference kaolinite KGa-1 and KGa-2 at 50 and 80°C for up to 2 months. The structure and morphology of the resulting products were characterized using X-ray diffraction, scanning electron microscopy, and Fourier transform infrared spectroscopy. The products were also examined for cation exchange and Cs+ sorption as a function of ionic strength and types of cations in the background solutions. Cancrinite and sodalite were the only new minerals observed in all of the conditions tested in this experiment. Two major chemical processes were involved in the reactions: dissolution of kaolinite and precipitation of cancrinite and sodalite. Increasing NaOH concentration and temperature, and decreasing NaAlO2 concentration increased the transformation rate. Both cancrinite and sodalite appeared stable thermodynamically under the experimental conditions. The newly formed feldspathoids were vulnerable to acid attack and pronounced dissolution occurred at pH below 5.5. Cancrinite and sodalite can incorporate NaNO3 ion pairs in their cages or channels. Sodium in cancrinite and sodalite was readily exchangeable by K+, but less easily by Cs+ or Ca2+. The feldspathoid products sorb nearly an order of magnitude more Cs+ than the unaltered kaolinite. The Cs adsorption is reduced by competing cations in the background solutions. At low ionic strength (0.01 M NaNO3 or 0.005 M Ca(NO3)2), Ca2+ was more competitive than Na+. When the concentration of the background solution was increased 10 times, Na+ was more competitive than Ca2+.

Keywords

CancriniteCation ExchangeCesium SorptionFeldspathoidHanford Waste TanksKaoliniteMineral StabilityMineral TransformationSodalite
Type
Research Article
Information
Clays and Clay Minerals , Volume 52 , Issue 1 , February 2004 , pp. 1 - 13
Copyright
Copyright © 2004, The Clay Minerals Society

References

Alberti, A. Colella, C. Oggiano, G. Pansini, M. and Vezzalini, G., (1994) Zeolite production from waste kaolin-containing materials Materials Engineering (Modena, Italy) 5 145–158.Google Scholar
Barnes, M.C. Addai-Mensah, J. and Gerson, A.R., (1999) The mechanism of the sodalite-to-cancrinite phase transformation in synthetic spent Bayer liquor Microporous Mesoporous Materials 31 287–302 10.1016/S1387-1811(99)00079-7.CrossRefGoogle Scholar
Barnes, M.C. Addai-Mensah, J. and Gerson, A.R., (1999) A methodology for quantifying sodalite and cancrinite phase mixtures and the kinetics of the sodalite to cancrinite phase transformation Microporous Mesoporous Materials 31 303–319 10.1016/S1387-1811(99)00080-3.CrossRefGoogle Scholar
Barnes, M.C. Addai-Mensah, J. and Gerson, A.R., (1999) The solubility of sodalite and cancrinite in synthetic spent Bayer liquor Colloids and Surfaces A, Physicochemical and Engineering Aspects 157 106–116 10.1016/S0927-7757(99)00058-8.CrossRefGoogle Scholar
Barrer, R.M., (1978) Zeolites and Clay Minerals as Sorbents and Molecular Sieves London Academic Press 496 pp.Google Scholar
Bauer, A. Velde, B. and Berger, G., (1998) Kaolinite transformation in high molar KOH solutions Applied Geochemistry 13 619–629 10.1016/S0883-2927(97)00094-2.CrossRefGoogle Scholar
Bickmore, B.R. Nagy, K.L. Young, J.S. and Drexler, J.W., (2001) Nitrate-cancrinite precipitation on quartz sand in simulated Hanford tank solutions Environmental Science and Technology 35 4481–4486 10.1021/es0108234.CrossRefGoogle ScholarPubMed
Breck, D.W., (1974) Zeolite Molecular Sieves: Structure, Chemistry, and Use New York John Wiley 752 pp.Google Scholar
Buhl, J.-c., (1991) Synthesis and characterization of the basic and non-basic members of the cancrinite-natrodavyne family Thermochimica Acta 178 19–31 10.1016/0040-6031(91)80294-S.CrossRefGoogle Scholar
Buhl, J.-c. and Loens, J., (1996) Synthesis and crystal structure of nitrate enclathrated sodalite Na8[AlSiO4]6(NO3)2 Journal of Alloys and Compounds 235 41–47 10.1016/0925-8388(95)02148-5.CrossRefGoogle Scholar
Buhl, J.-c. Stief, F. Fechtelkord, M. Gesing, T.M. Taphorn, U. and Taake, C., (2000) Synthesis, X-ray diffraction and MAS NMR characteris tics of nitrate cancrinite Na7.6[AlSiO4]6(NO3)1.6(H2O)2 Journal of Alloys and Compounds 305 93–102 10.1016/S0925-8388(00)00724-6.CrossRefGoogle Scholar
Coombs, D.S. Alberti, A. Armbruster, T. Artioli, G. Colella, C. and Galli, E. (1997) et al. , Recommended nomenclature for zeolite minerals: report of the subcommittee on zeolites for the Internaltional Mineralogical Association, Commission on New Minerals and Mineral Names The Canadian Mineralogist 35 1571–1606.Google Scholar
Dudzik, Z. and Kowalak, S., (1974) Preparation of zeolites of faujasite type from kaolinite Przemyśl Chemiczny 53 616–618.Google Scholar
Fechtelkord, M. Posnatzki, B. and Buhl, J.-c., (2001) Synthesis of basic cancrinite in a butanediol-water system Chemistry of Materials 13 1967–1975 10.1021/cm001136z.CrossRefGoogle Scholar
Gephart, R.E. and Lundgren, R.E., (1998) Hanford Tank Cleanup: A Guide to Understanding the Technical Issues 4th Columbus, Ohio Battelle Press.Google Scholar
Gerson, A.R. and Zheng, K., (1997) Bayer process plant scale: transformation of sodalite to cancrinite Journal of Crystal Growth 171 209–218 10.1016/S0022-0248(96)00482-4.CrossRefGoogle Scholar
Gualtieri, A. Norby, P. Artioli, G. and Hanson, J., (1997) Kinetic study of hydroxysodalite formation from natural kaolinites by time-resolved synchrotron powder diffraction Microporous Materials 9 189–201 10.1016/S0927-6513(96)00111-3.CrossRefGoogle Scholar
Hackbarth, K. Gesing, T.M. Fechtelkord, M. Stief, F. and Buhl, J.-c., (1999) Synthesis and crystal structure of carbonate cancrinite Na8[AlSiO4]6CO3(H2O)3.4, grown under low-temperature hydrothermal conditions Microporous Mesoporous Materials 30 347–358 10.1016/S1387-1811(99)00046-3.CrossRefGoogle Scholar
Hanlon, B.M., (1996) Waste tank summary report for month ending January 31, 1996 WHC-EP-0182-94 Richland, WA Westinghouse Hanford Company.Google Scholar
Hund, F., (1984) Nitrate-, thiosulfate-, sulfate- and sulfide cancrinite Zeitschrift für Anorganische und Allgemeine Chemie 509 153–160 10.1002/zaac.19845090216.CrossRefGoogle Scholar
McBride, M., (1994) Environmental Chemistry of Soils New York Oxford University Press 406 pp.Google Scholar
Nyman, M. Krumhansl, J.L. Zhang, P. Anderson, H. and Nenoff, T.M., (2000) Chemical evolution of leaked high-level liquid wastes in Hanford soils Materials Research Society Symposium Proceedings 608 225–230 10.1557/PROC-608-225.CrossRefGoogle Scholar
Pruess, K. Yabusaki, S. Steefel, C. and Lichtner, P., (2002) Fluid flow, heat transfer, and solute transport at nuclear waste storage tanks in the Hanford vadose zone Vadose Zone Journal 1 68–88 10.2136/vzj2002.6800.CrossRefGoogle Scholar
Rabo, J.A. and Rabo, J.A., (1976) Salt occlusion in zeolite crystals Zeolite Chemistry and Catalysis Washington, D.C. American Chemical Society 332–349.Google Scholar
Schulthess, C.P. and Dey, D.K., (1996) Estimation of Langmuir constants using linear and nonlinear least squares regression analyses Soil Science Society of America Journal 60 433–442 10.2136/sssaj1996.03615995006000020014x.CrossRefGoogle Scholar
Serne, R.J. Zachara, J.M. and Burke, D.S., (1998) Chemical information on tank supernatants, Cs adsorption from tank liquids onto Hanford sediments, and field observations of Cs migration from past tank leaks Richland, Washington Pacific Northwest National Laboratory 10.2172/576087 PNNL-11498/UC-510.CrossRefGoogle Scholar
Sieger, P. Wiebcke, M. Felsche, J. and Buhl, J.-c., (1991) Orientational disorder of the nitrite anion in the sodalite sodium aluminum silicate nitrite (Na8[AlSiO4]6(NO2)2) Acta Crystallographica, Section C: Crystal Structure Communications C47 498–501.Google Scholar
Zheng, K. Gerson, A.R. Addai-Mensah, J. and Smart, R.S.C., (1997) The influence of sodium carbonate on sodium aluminosilicate crystallization and solubility in sodium aluminate solutions Journal of Crystal Growth 171 197–208 10.1016/S0022-0248(96)00480-0.CrossRefGoogle Scholar
Zheng, K. Smart, R.S.C. Addai-Mensah, J. and Gerson, A., (1998) Solubility of sodium aluminosilicates in synthetic Bayer liquor Journal of Chemical and Engineering Data 43 312–317 10.1021/je970187i.CrossRefGoogle Scholar