TY - JOUR
T1 - Chalcogenide aerogels as sorbents for noble gases (Xe, Kr)
AU - Subrahmanyam, Kota S.
AU - Spanopoulos, Ioannis
AU - Chun, Jaehun
AU - Riley, Brian J.
AU - Thallapally, Praveen K.
AU - Trikalitis, Pantelis N.
AU - Kanatzidis, Mercouri G.
N1 - Funding Information:
This work was funded in part by the US Department of Energy Office of Nuclear Energy through a Nuclear Energy University Partnership (NEUP) grant. Pacific Northwest National Laboratory is operated by the U.S. Department of Energy under Contract Number DE-AC05-76RL01830. This research has been cofinanced by the European Union and Greek national funds through the Operational Program “Education and Lifelong Learning” of the National Strategic Reference Framework (NSRF) Research Funding Program: ARISTEIA II 4862.
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/10/4
Y1 - 2017/10/4
N2 - High-surface-area molybdenum sulfide (MoSx) and antimony sulfide (SbSx) chalcogels were studied for Xe/Kr gas separation. The intrinsic soft Lewis basic character of the chalcogel framework is a unique property among the large family of porous materials and lends itself to a potential new approach toward the selective separation of Xe over Kr. Among these chalcogels, MoSx shows the highest Xe and Kr uptake, reaching 0.69 mmol g-1 (1.05 mmol cm-3) and 0.28 mmol g-1 (0.42 mmol cm-3) respectively, at 273 K and 1 bar. The corresponding isosteric heat of adsorption at zero coverage (Qst 0) is 22.8 and 18.6 kJ mol-1 and both are the highest among the selected chalcogels. The IAST (10:90) Xe/Kr selectivity at 273 K for MoSx is 6.0, whereas for SbSx chalcogels, it varies in the range 2.0-2.8. The higher formal charge of molybdenum, Mo4+, in MoSx versus that of antimony, Sb3+, in SbSx coupled with its larger atomic size could induce higher polarizability in the MoSx framework and therefore higher Xe/Kr selectivity.
AB - High-surface-area molybdenum sulfide (MoSx) and antimony sulfide (SbSx) chalcogels were studied for Xe/Kr gas separation. The intrinsic soft Lewis basic character of the chalcogel framework is a unique property among the large family of porous materials and lends itself to a potential new approach toward the selective separation of Xe over Kr. Among these chalcogels, MoSx shows the highest Xe and Kr uptake, reaching 0.69 mmol g-1 (1.05 mmol cm-3) and 0.28 mmol g-1 (0.42 mmol cm-3) respectively, at 273 K and 1 bar. The corresponding isosteric heat of adsorption at zero coverage (Qst 0) is 22.8 and 18.6 kJ mol-1 and both are the highest among the selected chalcogels. The IAST (10:90) Xe/Kr selectivity at 273 K for MoSx is 6.0, whereas for SbSx chalcogels, it varies in the range 2.0-2.8. The higher formal charge of molybdenum, Mo4+, in MoSx versus that of antimony, Sb3+, in SbSx coupled with its larger atomic size could induce higher polarizability in the MoSx framework and therefore higher Xe/Kr selectivity.
KW - Aerogels
KW - Chalcogenide
KW - Nuclear remediation
KW - Porous materials
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U2 - 10.1021/acsami.6b15896
DO - 10.1021/acsami.6b15896
M3 - Article
C2 - 28157282
AN - SCOPUS:85027723139
SN - 1944-8244
VL - 9
SP - 33389
EP - 33394
JO - ACS applied materials & interfaces
JF - ACS applied materials & interfaces
IS - 39
ER -