Perrhenate incorporation into binary mixed sodalites: The role of anion size and implications for technetium-99 sequestration

Dickson, Johnbull O.; Harsh, James B.; Lukens, Wayne W.; Pierce, Eric M.

doi:10.1016/j.chemgeo.2014.12.009

Perrhenate incorporation into binary mixed sodalites: The role of anion size and implications for technetium-99 sequestration

Journal Article · Sat Dec 20 00:00:00 EST 2014 · Chemical Geology

DOI:https://doi.org/10.1016/j.chemgeo.2014.12.009· OSTI ID:1327622

Dickson, Johnbull O. ^[1]; Harsh, James B. ^[1]; Lukens, Wayne W. ^[2]; Pierce, Eric M. ^[3]

Washington State Univ., Pullman, WA (United States). Department of Crop and Soil Sciences
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Environmental Sciences Division

Perrhenate (ReO₄^-), as a TcO₄^- analogue, was incorporated into mixed-anion sodalites from binary solutions containing ReO₄^- and a competing anion X^n- (Cl^-, CO₃^2-, SO₄^2-, MnO₄^-, or WO₄^2-). For this study, our objective was to determine the extent of solid solution formation and the dependence of competing ion selectivity on ion size. Using equivalent aqueous concentrations of the anions (ReO₄^-/X^n- molar ratio = 1:1), we synthesized mixed-anion sodalites from zeolite and NaOH at 90 °C for 96 h. The resulting solids were characterized by bulk chemical analysis, powder X-ray diffraction, scanning electron microscopy, and X-ray absorption near edge structure (XANES) spectroscopy to determine crystal structure, chemical composition, morphology, and rhenium (Re) oxidation state. Rhenium in the solid phase occurred predominately as Re(VII)O₄^- in the sodalites, which have a primitive cubic pattern in the space group P43n. The refined unit-cell parameters of the mixed sodalites ranged from 8.88 to 9.15 Å and showed a linear dependence on the size and mole fraction of the incorporated anion(s). The ReO₄^- selectivity, represented by its distribution coefficient (K_d), increased in the following order: Cl^- < NO₃^- < MnO₄^- and CO₃^2- < SO₄^2- < WO₄^2- for the monovalent and divalent anions, respectively. The relationship between the ReO₄^- distribution coefficient and competing anion size was nonlinear. When the difference in ionic radius (DIR) between ReO₄^- and X^{n -} (n = 1 or 2) was greater than ~ 12%, then ReO₄^- incorporation into sodalite was insignificant. The results imply that anion size is the major factor that determines sodalite anion compositions. Given the similarity in chemical behavior and anion size, ReO₄^- serves as a suitable analogue for TcO₄^- under oxidizing conditions where both elements are expected to remain as oxyanions in the + 7 oxidation state.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725

OSTI ID:: 1327622

Alternate ID(s):: OSTI ID: 1246658
OSTI ID: 1374723

Report Number(s):: LBNL--181861; KP1702030; ERKP796

Journal Information:: Chemical Geology, Journal Name: Chemical Geology Vol. 395; ISSN 0009-2541

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Synthesis and characterization of iodosodalite Chong, Saehwa; Peterson, Jacob; Nam, Junghune Journal of the American Ceramic Society, Vol. 100, Issue 5 https://doi.org/10.1111/jace.14772	journal	March 2017

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
54 ENVIRONMENTAL SCIENCES
Anion selectivity
Distribution coefficient
Mixed-anion sodalites
Nuclear waste
Perrhenate
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technetium-99

CSD 1791138: Experimental Crystal Structure Determination O., Dickson, Johnbull; B., Harsh, James; W., Lukens, Wayne https://doi.org/10.25505/fiz.icsd.cc1y3tnj The current record is supplemented by this dataset	dataset	January 2015
CSD 1791139: Experimental Crystal Structure Determination O., Dickson, Johnbull; B., Harsh, James; W., Lukens, Wayne https://doi.org/10.25505/fiz.icsd.cc1y3tpk The current record is supplemented by this dataset	dataset	January 2015
CSD 1791140: Experimental Crystal Structure Determination O., Dickson, Johnbull; B., Harsh, James; W., Lukens, Wayne https://doi.org/10.25505/fiz.icsd.cc1y3tql The current record is supplemented by this dataset	dataset	January 2015

Perrhenate incorporation into binary mixed sodalites: The role of anion size and implications for technetium-99 sequestration

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