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Title: Chalcogenide Aerogels as Sorbents for Noble Gases (Xe, Kr)

Abstract

High surface MoSx and SbSx chalcogels were studied for Xe/Kr gas separation. The intrinsic soft character of the chalcogel framework is a unique property among the large family of porous materials and offers a potential new approach towards 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 (Qst0) 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 while for SbSx chalcogels 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.

Authors:
 [1]; ORCiD logo [2];  [3];  [3];  [3];  [2]; ORCiD logo [1]
  1. Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
  2. Department of Chemistry, University of Crete, Voutes, 71003 Heraklion, Greece
  3. Pacific Northwest National Laboratory, Richland, Washington 99352, United States
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1406757
Report Number(s):
PNNL-SA-121769
Journal ID: ISSN 1944-8244; 600305000
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: ACS Applied Materials and Interfaces; Journal Volume: 9; Journal Issue: 39
Country of Publication:
United States
Language:
English

Citation Formats

Subrahmanyam, Kota S., Spanopoulos, Ioannis, Chun, Jaehun, Riley, Brian J., Thallapally, Praveen K., Trikalitis, Pantelis N., and Kanatzidis, Mercouri G.. Chalcogenide Aerogels as Sorbents for Noble Gases (Xe, Kr). United States: N. p., 2017. Web. doi:10.1021/acsami.6b15896.
Subrahmanyam, Kota S., Spanopoulos, Ioannis, Chun, Jaehun, Riley, Brian J., Thallapally, Praveen K., Trikalitis, Pantelis N., & Kanatzidis, Mercouri G.. Chalcogenide Aerogels as Sorbents for Noble Gases (Xe, Kr). United States. doi:10.1021/acsami.6b15896.
Subrahmanyam, Kota S., Spanopoulos, Ioannis, Chun, Jaehun, Riley, Brian J., Thallapally, Praveen K., Trikalitis, Pantelis N., and Kanatzidis, Mercouri G.. Fri . "Chalcogenide Aerogels as Sorbents for Noble Gases (Xe, Kr)". United States. doi:10.1021/acsami.6b15896.
@article{osti_1406757,
title = {Chalcogenide Aerogels as Sorbents for Noble Gases (Xe, Kr)},
author = {Subrahmanyam, Kota S. and Spanopoulos, Ioannis and Chun, Jaehun and Riley, Brian J. and Thallapally, Praveen K. and Trikalitis, Pantelis N. and Kanatzidis, Mercouri G.},
abstractNote = {High surface MoSx and SbSx chalcogels were studied for Xe/Kr gas separation. The intrinsic soft character of the chalcogel framework is a unique property among the large family of porous materials and offers a potential new approach towards 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 (Qst0) 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 while for SbSx chalcogels 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.},
doi = {10.1021/acsami.6b15896},
journal = {ACS Applied Materials and Interfaces},
number = 39,
volume = 9,
place = {United States},
year = {Fri Feb 03 00:00:00 EST 2017},
month = {Fri Feb 03 00:00:00 EST 2017}
}