K2xSn4-xS8-x (x = 0.65-1): A new metal sulfide for rapid and selective removal of Cs+, Sr2+ and UO2 2+ ions

Debajit Sarma, Christos D. Malliakas, K. S. Subrahmanyam, Saiful M. Islam, Mercouri G Kanatzidis

Research output: Contribution to journalArticle

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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. Here 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 UO2 2+ ion exchange properties in varying conditions. 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 UO2 2+. 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 UO2 2+ (2.7 × 104) at neutral pH (7.4, 6.9, 5.7 ppm Cs+, Sr2+ and UO2 2+, respectively; V/m ∼ 1000 mL g-1). KTS-3 exhibits impressive Cs+, Sr2+ and UO2 2+ 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.

Original languageEnglish
Pages (from-to)1121-1132
Number of pages12
JournalChemical Science
Volume7
Issue number2
DOIs
Publication statusPublished - 2016

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Sulfides
Radioactive Waste
Ion exchange
Metals
Ions
Radioisotopes
Potassium
Salts
Uranium
Tin
Industrial wastes
Spent fuels
Nuclear fuels
Vacancies
Diffraction
Crystal structure
Single crystals
Costs

ASJC Scopus subject areas

  • Chemistry(all)

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K2xSn4-xS8-x (x = 0.65-1) : A new metal sulfide for rapid and selective removal of Cs+, Sr2+ and UO2 2+ ions. / Sarma, Debajit; Malliakas, Christos D.; Subrahmanyam, K. S.; Islam, Saiful M.; Kanatzidis, Mercouri G.

In: Chemical Science, Vol. 7, No. 2, 2016, p. 1121-1132.

Research output: Contribution to journalArticle

Sarma, Debajit ; Malliakas, Christos D. ; Subrahmanyam, K. S. ; Islam, Saiful M. ; Kanatzidis, Mercouri G. / K2xSn4-xS8-x (x = 0.65-1) : A new metal sulfide for rapid and selective removal of Cs+, Sr2+ and UO2 2+ ions. In: Chemical Science. 2016 ; Vol. 7, No. 2. pp. 1121-1132.
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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. Here 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 UO2 2+ ion exchange properties in varying conditions. 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) {\AA}, b = 16.882(2) {\AA}, c = 7.375(1) {\AA} 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 UO2 2+. 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 UO2 2+ (2.7 × 104) at neutral pH (7.4, 6.9, 5.7 ppm Cs+, Sr2+ and UO2 2+, respectively; V/m ∼ 1000 mL g-1). KTS-3 exhibits impressive Cs+, Sr2+ and UO2 2+ 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.",
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