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Cesium and strontium incorporation into zeolite-type phases during homogeneous nucleation from caustic solutions

Nelson Rivera, Sunkyung Choi, Caleb Strepka, Karl Mueller, Nicolas Perdrial, Jon Chorover and Peggy A. O'Day
Cesium and strontium incorporation into zeolite-type phases during homogeneous nucleation from caustic solutions
American Mineralogist (December 2011) 96 (11-12): 1809-1820

Abstract

Formation of faujasite- and sodalite/cancrinite-type phases associated with caustic waste reactions in the environment may structurally incorporate contaminant species such as radioactive Sr (super 2+) and Cs (super +) and thus provide a mechanism of attenuation. To investigate mineral evolution and structural incorporation of cations in simplified experiments, aluminosilicate solids were precipitated homogeneously at room temperature from batch solutions containing a 1:1 molal ratio of Si to Al and 10 (super -3) molal Sr and/or Cs and aged for 30 or 548 days. Syntheses were done with solutions in equilibrium with atmospheric CO (sub 2) and with gas-purged solutions. Experimental products were characterized by bulk chemical analyses, chemical extractions, XRD, SEM/TEM, TGA, solid-state (super 27) Al NMR, and Sr EXAFS. Chemical analysis showed that solids had a 1:1 Al:Si molar ratio and that Sr was sequestered at higher amounts than Cs. After 30 days of aging in purged solutions, XRD showed that zeolite X (faujasite-type) was the only crystalline product. After aging 30 and 548 days in solutions equilibrated with atmospheric CO (sub 2) , a mixture of sodalite, cancrinite, and minor zeolite X was produced. Surface areas of solids at 30 days were much lower than published values for zeolite phases synthesized at high temperature, although particle aging produced more crystalline and less aggregated phases with higher bulk surface areas. Characterization of products by (super 27) Al NMR indicated only tetrahedrally coordinated Al. Measured isotropic shifts of primary resonances did not change substantially with precipitate aging, although the primary mineral phase changed from zeolite X to sodalite/cancrinite, indicating local ordering of Al-Si tetrahedra. Analysis of reaction products by Sr EXAFS suggested Sr bonding in hexagonal prisms and six-membered rings of the supercages of zeolite X that may be more site specific than those of monovalent cations. For samples aged for 548 days, interatomic distances from Sr-EXAFS are consistent with partial Sr dehydration and bonding to framework oxygen atoms in sodalite cages or in large channels in cancrinite. Incorporation of Sr into both faujasite and sodalite/cancrinite phases is favored over Cs during room-temperature synthesis, possibly because of increased cation site competition between Cs (super +) and Na (super +) . Results of this study help constrain cation incorporation into sodalite/cancrinite mineral assemblages that form at caustic waste-impacted field sites and may aid in the predictive modeling of contaminant release.


ISSN: 0003-004X
EISSN: 1945-3027
Coden: AMMIAY
Serial Title: American Mineralogist
Serial Volume: 96
Serial Issue: 11-12
Title: Cesium and strontium incorporation into zeolite-type phases during homogeneous nucleation from caustic solutions
Affiliation: University of California, Merced, School of Natural Sciences, Merced, CA, United States
Pages: 1809-1820
Published: 201112
Text Language: English
Publisher: Mineralogical Society of America, Washington, DC, United States
References: 82
Accession Number: 2012-009950
Categories: Mineralogy of silicates
Document Type: Serial
Bibliographic Level: Analytic
Illustration Description: illus. incl. 6 tables
Secondary Affiliation: U. S. Environmental Protection Agency, USA, United StatesPennsylvania State University, USA, United StatesUniversity of Arizona, USA, United States
Country of Publication: United States
Secondary Affiliation: GeoRef, Copyright 2017, American Geosciences Institute. Abstract, copyright, Mineralogical Society of America. Reference includes data from GeoScienceWorld, Alexandria, VA, United States
Update Code: 201205
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