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Pressure-Induced Metathesis Reaction To Sequester Cs

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Department of Earth System Sciences, Yonsei University, Seoul 120-749, Korea
Division of Radwaste Disposal Research, Korea Atomic Energy Research Institute, Daejeon 305-353, Korea
§ NanoCenter & Department of Chemistry and Biochemistry, University of South Carolina, Columbia, South Carolina 29208, United States
Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025-7015, United States
*E-mail: [email protected]. Tel: +82-2-2123-5667.
Cite this: Environ. Sci. Technol. 2015, 49, 1, 513–519
Publication Date (Web):December 1, 2014
Copyright © 2014 American Chemical Society

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    Abstract Image

    We report here a pressure-driven metathesis reaction where Ag-exchanged natrolite (Ag16Al16Si24O80·16H2O, Ag-NAT) is pressurized in an aqueous CsI solution, resulting in the exchange of Ag+ by Cs+ in the natrolite framework forming Cs16Al16Si24O80·16H2O (Cs-NAT-I) and, above 0.5 GPa, its high-pressure polymorph (Cs-NAT-II). During the initial cation exchange, the precipitation of AgI occurs. Additional pressure and heat at 2 GPa and 160 °C transforms Cs-NAT-II to a pollucite-related, highly dense, and water-free triclinic phase with nominal composition CsAlSi2O6. At ambient temperature after pressure release, the Cs remains sequestered in a now monoclinic pollucite phase at close to 40 wt % and a favorably low Cs leaching rate under back-exchange conditions. This process thus efficiently combines the pressure-driven separation of Cs and I at ambient temperature with the subsequent sequestration of Cs under moderate pressures and temperatures in its preferred waste form suitable for long-term storage at ambient conditions. The zeolite pollucite CsAlSi2O6·H2O has been identified as a potential host material for nuclear waste remediation of anthropogenic 137Cs due to its chemical and thermal stability, low leaching rate, and the large amount of Cs it can contain. The new water-free pollucite phase we characterize during our process will not display radiolysis of water during longterm storage while maintaining the Cs content and low leaching rate.

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    Representative final Rietveld fits (Figure S1), changes of the unit cell parameters as a function of pressure and heat treatment (Table S1), refined atomic coordinates (Tables S2) and selected interatomic distances and angles (Table S3) for natrolite to pollucite as a function of pressure and heat treatment, refined atomic coordinates (Table S4) and selected interatomic distances and angles (Table S5) for the recovered monoclinic pollucite, and bond valence sum of the recovered monoclinic pollucite (Table S6). This material is available free of charge via the Internet at

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    Cited By

    This article is cited by 9 publications.

    1. Wooseung Choi, Jinhyuk Choi, Huijeong Hwang, Yongjae Lee. Transformation of natural pollucite into hexacelsian under high pressure and temperature. Physics and Chemistry of Minerals 2022, 49 (5)
    2. Donghoon Seoung, Hyeonsu Kim, Pyosang Kim, Yongmoon Lee. Pressure- and Temperature-Induced Insertion of N2, O2 and CH4 to Ag-Natrolite. Materials 2020, 13 (18) , 4096.
    3. Jingwei Li, Dong Xu, Wenlong Wang, Xujiang Wang, Yanpeng Mao, Chao Zhang, Wen Jiang, Changliang Wu. Review on Selection and Experiment Method of Commonly Studied Simulated Radionuclides in Researches of Nuclear Waste Solidification. Science and Technology of Nuclear Installations 2020, 2020 , 1-13.
    4. Sung-Min Kang, Muruganantham Rethinasabapathy, Seung Kuy Hwang, Go-Woon Lee, Sung-Chan Jang, Cheol Hwan Kwak, Sang-Rak Choe, Yun Suk Huh. Microfluidic generation of Prussian blue-laden magnetic micro-adsorbents for cesium removal. Chemical Engineering Journal 2018, 341 , 218-226.
    5. Mihye Kong, Yongmoon Lee, G. Diego Gatta, Yongjae Lee. Comparative compressional behavior of chabazite with Li+, Na+, Ag+, K+, Rb+, and Cs+ as extra-framework cations. American Mineralogist 2018, 103 (2) , 207-215.
    6. Jae Hwan Yang, Hwan-Seo Park, Yung-Zun Cho. Immobilization of Cs-trapping ceramic filters within glass-ceramic waste forms. Annals of Nuclear Energy 2017, 110 , 1121-1126.
    7. Jae Hwan Yang, Ahreum Han, Joo Young Yoon, Hwan-Seo Park, Yung-Zun Cho. A new route to the stable capture and final immobilization of radioactive cesium. Journal of Hazardous Materials 2017, 339 , 73-81.
    8. Kai Landskron. High Pressure Chemistry. 2016, 1-45.
    9. Junhyuck Im, Yongmoon Lee, Douglas A. Blom, Thomas Vogt, Yongjae Lee. High-pressure and high-temperature transformation of Pb( ii )-natrolite to Pb( ii )-lawsonite. Dalton Transactions 2016, 45 (4) , 1622-1630.

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