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Title: Hybrid Ultra-Microporous Materials for Selective Xenon Adsorption and Separation

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [1];  [2];  [2];  [3];  [2];  [2];  [4];  [2];  [5];  [3]
  1. Physical and Computational Science Directorate, Pacific Northwest National Laboratory, Richland WA 99352 USA; Chemistry Department, Faculty of Science, Alexandria University, P.O.Box 426 Ibrahimia Alexandria 21321 Egypt
  2. Department of Chemistry, University of South Florida, 4202 East Fowler Ave., CHE205 Tampa FL 33620 USA
  3. Physical and Computational Science Directorate, Pacific Northwest National Laboratory, Richland WA 99352 USA
  4. X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, Argonne IL 60439 USA
  5. Department of Chemical & Environmental Sciences, University of Limerick, Limerick Republic of Ireland

The demand for Xe/Kr separation continues to grow due to the industrial significance of high-purity Xe gas. Current separation processes rely on energy intensive cryogenic distillation. Therefore, there is a need to develop less energy intensive alternatives such as physisorptive separation using porous materials. Here we show that an underexplored class of porous materials called hybrid ultramicroporous materials (HUMs) based upon inorganic and organic building blocks affords new benchmark selectivity for Xe separation from Xe/Kr mixtures. The isostructural materials, CROFOUR-1-Ni and CROFOUR-2-Ni, are coordination networks that exhibit coordinatively saturated metal centres and two distinct types of micropores, one of which is lined by CrO42- (CROFOUR) anions and the other is decorated by the functionalized organic linker. These nets offer unprecedented selectivity towards Xe, and also address processing and stability limitations of existing porous materials. Modelling experiments indicate that the extraordinary selectivity of these nets is tailored by synergy between the pore size, which is just above the kinetic diameter of Xe, and the strong electrostatics afforded by the CrO42- anions. Column breakthrough experiments demonstrate the potential of the practical use of these materials in Xe/Kr separation at low concentrations at the levels relevant to Xe capture from air and in nuclear fuel reprocessing.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Nuclear Energy; USDOE Office of Science - Office of Basic Energy Sciences - Scientific User Facilities Division
DOE Contract Number:
AC02-06CH11357
OSTI ID:
1390959
Journal Information:
Angewandte Chemie (International Edition), Vol. 55, Issue 29; ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English

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