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Title: Influence of Hydrogen Sulfide Exposure on the Transport and Structural Properties of the Metal–Organic Framework ZIF-8

In this paper, the interaction between hydrogen sulfide and ZIF-8 was studied via structural characterizations and guest molecule diffusion measurements. It was found that hydrogen sulfide reacts with the ZIF-8 external particle surface to form a surface barrier that excludes the uptake of larger molecules (ethanol) and slows down the uptake of smaller molecules (carbon dioxide). Nonetheless, bulk transport properties were unaltered, as supported by pulsed field gradient nuclear magnetic resonance studies. Dispersion-corrected density functional theory calculations revealed that H 2S is consumed by reactions occurring at the ZIF external surface. These reactions result in water and defect formation, both of which were found to be exothermic and independent of both crystallographic facets ({001} and {110}) and surface termination. Finally, we concluded that these surface reactions lead to structural and chemical changes to the ZIF-8 external surface that generate surface barriers to molecular transport.
Authors:
 [1] ; ORCiD logo [2] ; ORCiD logo [3] ;  [4] ; ORCiD logo [3] ; ORCiD logo [2] ; ORCiD logo [1]
  1. Univ. of Florida, Gainesville, FL (United States). Dept. of Chemical Engineering
  2. Univ. of Wisconsin, Madison, WI (United States). Theoretical Chemistry Inst. Dept. of Chemistry
  3. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical and Biomolecular Engineering
  4. Univ. of Florida, Gainesville, FL (United States). National High Magnetic Field Lab.
Publication Date:
Grant/Contract Number:
SC0012577; ECCS-1542174; DMR-1157490
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Name: Journal of Physical Chemistry. C; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
Georgia Inst. of Technology, Atlanta, GA (United States); Univ. of Florida, Gainesville, FL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1428044