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Title: K 2x Sn 4-x S 8-x (x = 0.65–1): a new metal sulfide for rapid and selective removal of Cs + , Sr 2+ and UO 2 2+ ions

Abstract

The fission of uranium produces radionuclides, 137Cs and 90Sr, which are major constituents of spent nuclear fuel. The half-life of 137Cs and 90Sr is nearly 30 years and thus that makes them harmful to human life and the environment. The selective removal of these radionuclides in the presence of high salt concentrations from industrial nuclear waste is necessary for safe storage. We report the synthesis and crystal structure of K2xSn4-xS8-x (x = 0.65–1, KTS-3) a material which exhibits excellent Cs+, Sr2+ and UO22+ ion exchange properties in varying conditions. Furthermore, the compound adopts a layered structure which consists of exchangeable potassium ions sandwiched between infinite layers of octahedral and tetrahedral tin centers. K2xSn4-xS8-x (x = 0.65–1, KTS-3) crystallizes in the monoclinic space group P21/c with cell parameters a = 13.092(3) Å, b = 16.882(2) Å, c = 7.375(1) Å and β = 98.10(1)°. Refinement of the single crystal diffraction data revealed the presence of Sn vacancies in the tetrahedra that are long range ordered. The interlayer potassium ions of KTS-3 can be exchanged for Cs+, Sr2+ and UO22+. KTS-3 exhibits rapid and efficient ion exchange behavior in a broad pH range. The distribution coefficients (Kd) for KTS-3 are high formore » Cs+ (5.5 × 104), Sr2+ (3.9 × 105) and UO22+ (2.7 × 104) at neutral pH (7.4, 6.9, 5.7 ppm Cs+, Sr2+ and UO22+, respectively; V/m ~ 1000 mL g-1). KTS-3 exhibits impressive Cs+, Sr2+ and UO22+ ion exchange properties in high salt concentration and over a broad pH range, which coupled with the low cost, environmentally friendly nature and facile synthesis underscores its potential in treating nuclear waste.« less

Authors:
 [1];  [1];  [1];  [1];  [2]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1352636
Grant/Contract Number:  
AC02-06CH11357; DMR-1410169
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Science
Additional Journal Information:
Journal Volume: 7; Journal Issue: 2; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Sarma, Debajit, Malliakas, Christos D., Subrahmanyam, K. S., Islam, Saiful M., and Kanatzidis, Mercouri G. K 2x Sn 4-x S 8-x (x = 0.65–1): a new metal sulfide for rapid and selective removal of Cs + , Sr 2+ and UO 2 2+ ions. United States: N. p., 2015. Web. doi:10.1039/c5sc03040d.
Sarma, Debajit, Malliakas, Christos D., Subrahmanyam, K. S., Islam, Saiful M., & Kanatzidis, Mercouri G. K 2x Sn 4-x S 8-x (x = 0.65–1): a new metal sulfide for rapid and selective removal of Cs + , Sr 2+ and UO 2 2+ ions. United States. https://doi.org/10.1039/c5sc03040d
Sarma, Debajit, Malliakas, Christos D., Subrahmanyam, K. S., Islam, Saiful M., and Kanatzidis, Mercouri G. Tue . "K 2x Sn 4-x S 8-x (x = 0.65–1): a new metal sulfide for rapid and selective removal of Cs + , Sr 2+ and UO 2 2+ ions". United States. https://doi.org/10.1039/c5sc03040d. https://www.osti.gov/servlets/purl/1352636.
@article{osti_1352636,
title = {K 2x Sn 4-x S 8-x (x = 0.65–1): a new metal sulfide for rapid and selective removal of Cs + , Sr 2+ and UO 2 2+ ions},
author = {Sarma, Debajit and Malliakas, Christos D. and Subrahmanyam, K. S. and Islam, Saiful M. and Kanatzidis, Mercouri G.},
abstractNote = {The fission of uranium produces radionuclides, 137Cs and 90Sr, which are major constituents of spent nuclear fuel. The half-life of 137Cs and 90Sr is nearly 30 years and thus that makes them harmful to human life and the environment. The selective removal of these radionuclides in the presence of high salt concentrations from industrial nuclear waste is necessary for safe storage. We report the synthesis and crystal structure of K2xSn4-xS8-x (x = 0.65–1, KTS-3) a material which exhibits excellent Cs+, Sr2+ and UO22+ ion exchange properties in varying conditions. Furthermore, the compound adopts a layered structure which consists of exchangeable potassium ions sandwiched between infinite layers of octahedral and tetrahedral tin centers. K2xSn4-xS8-x (x = 0.65–1, KTS-3) crystallizes in the monoclinic space group P21/c with cell parameters a = 13.092(3) Å, b = 16.882(2) Å, c = 7.375(1) Å and β = 98.10(1)°. Refinement of the single crystal diffraction data revealed the presence of Sn vacancies in the tetrahedra that are long range ordered. The interlayer potassium ions of KTS-3 can be exchanged for Cs+, Sr2+ and UO22+. KTS-3 exhibits rapid and efficient ion exchange behavior in a broad pH range. The distribution coefficients (Kd) for KTS-3 are high for Cs+ (5.5 × 104), Sr2+ (3.9 × 105) and UO22+ (2.7 × 104) at neutral pH (7.4, 6.9, 5.7 ppm Cs+, Sr2+ and UO22+, respectively; V/m ~ 1000 mL g-1). KTS-3 exhibits impressive Cs+, Sr2+ and UO22+ ion exchange properties in high salt concentration and over a broad pH range, which coupled with the low cost, environmentally friendly nature and facile synthesis underscores its potential in treating nuclear waste.},
doi = {10.1039/c5sc03040d},
journal = {Chemical Science},
number = 2,
volume = 7,
place = {United States},
year = {Tue Oct 27 00:00:00 EDT 2015},
month = {Tue Oct 27 00:00:00 EDT 2015}
}

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