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

Abstract

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:
Research Org.:
Georgia Inst. of Technology, Atlanta, GA (United States); Univ. of Florida, Gainesville, FL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1428044
Grant/Contract Number:  
SC0012577; ECCS-1542174; DMR-1157490
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 13; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Dutta, Akshita, Tymi?ska, Nina, Zhu, Guanghui, Collins, James, Lively, Ryan P., Schmidt, J. R., and Vasenkov, Sergey. Influence of Hydrogen Sulfide Exposure on the Transport and Structural Properties of the Metal–Organic Framework ZIF-8. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.8b00798.
Dutta, Akshita, Tymi?ska, Nina, Zhu, Guanghui, Collins, James, Lively, Ryan P., Schmidt, J. R., & Vasenkov, Sergey. Influence of Hydrogen Sulfide Exposure on the Transport and Structural Properties of the Metal–Organic Framework ZIF-8. United States. doi:10.1021/acs.jpcc.8b00798.
Dutta, Akshita, Tymi?ska, Nina, Zhu, Guanghui, Collins, James, Lively, Ryan P., Schmidt, J. R., and Vasenkov, Sergey. Fri . "Influence of Hydrogen Sulfide Exposure on the Transport and Structural Properties of the Metal–Organic Framework ZIF-8". United States. doi:10.1021/acs.jpcc.8b00798.
@article{osti_1428044,
title = {Influence of Hydrogen Sulfide Exposure on the Transport and Structural Properties of the Metal–Organic Framework ZIF-8},
author = {Dutta, Akshita and Tymi?ska, Nina and Zhu, Guanghui and Collins, James and Lively, Ryan P. and Schmidt, J. R. and Vasenkov, Sergey},
abstractNote = {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 H2S 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.},
doi = {10.1021/acs.jpcc.8b00798},
journal = {Journal of Physical Chemistry. C},
number = 13,
volume = 122,
place = {United States},
year = {Fri Mar 09 00:00:00 EST 2018},
month = {Fri Mar 09 00:00:00 EST 2018}
}

Journal Article:
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