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Title: Recovery of Acid-Gas-Degraded Zeolitic Imidazolate Frameworks by Solvent-Assisted Crystal Redemption (SACRed)

Abstract

The acid stability of zeolitic imidazolate frameworks (ZIFs) is an important issue hindering their application. Acid-gas damage of ZIFs has been considered irreversible. However, we demonstrate here a methodology called solvent-assisted crystal redemption (SACRed) to reverse acid-gas damage to ZIFs with a high degree of structural and functional recovery. For example, post-SACRed ZIF-8 is shown to be structurally and chemically near-identical with the original pristine ZIF-8 that suffered a large loss of surface area, porosity, and crystallinity during acid-gas exposure. We also provide mechanistic insight into the recovery process using deuterium-labeled linkers and 2H NMR spectroscopy. SACRed treatments could allow large extensions in the lifetime of ZIF-based membranes and adsorbents that degrade over time.

Authors:
 [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering
Publication Date:
Research Org.:
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)
OSTI Identifier:
1469889
Grant/Contract Number:  
SC0012577
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 9; Journal Issue: 40; Related Information: UNCAGE-ME partners with Georgia Institute of Technology (lead); Lehigh University; Oak Ridge National Laboratory; University of Alabama; University of Florida; University of Wisconsin; Washington University in St. Louis; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; catalysis (heterogeneous); defects; membrane; carbon capture; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing); MOFs; ZIFs; acid gas; degradation; recovery

Citation Formats

Jayachandrababu, Krishna C., Bhattacharyya, Souryadeep, Chiang, Yadong, Sholl, David S., and Nair, Sankar. Recovery of Acid-Gas-Degraded Zeolitic Imidazolate Frameworks by Solvent-Assisted Crystal Redemption (SACRed). United States: N. p., 2017. Web. doi:10.1021/acsami.7b11686.
Jayachandrababu, Krishna C., Bhattacharyya, Souryadeep, Chiang, Yadong, Sholl, David S., & Nair, Sankar. Recovery of Acid-Gas-Degraded Zeolitic Imidazolate Frameworks by Solvent-Assisted Crystal Redemption (SACRed). United States. doi:10.1021/acsami.7b11686.
Jayachandrababu, Krishna C., Bhattacharyya, Souryadeep, Chiang, Yadong, Sholl, David S., and Nair, Sankar. Tue . "Recovery of Acid-Gas-Degraded Zeolitic Imidazolate Frameworks by Solvent-Assisted Crystal Redemption (SACRed)". United States. doi:10.1021/acsami.7b11686. https://www.osti.gov/servlets/purl/1469889.
@article{osti_1469889,
title = {Recovery of Acid-Gas-Degraded Zeolitic Imidazolate Frameworks by Solvent-Assisted Crystal Redemption (SACRed)},
author = {Jayachandrababu, Krishna C. and Bhattacharyya, Souryadeep and Chiang, Yadong and Sholl, David S. and Nair, Sankar},
abstractNote = {The acid stability of zeolitic imidazolate frameworks (ZIFs) is an important issue hindering their application. Acid-gas damage of ZIFs has been considered irreversible. However, we demonstrate here a methodology called solvent-assisted crystal redemption (SACRed) to reverse acid-gas damage to ZIFs with a high degree of structural and functional recovery. For example, post-SACRed ZIF-8 is shown to be structurally and chemically near-identical with the original pristine ZIF-8 that suffered a large loss of surface area, porosity, and crystallinity during acid-gas exposure. We also provide mechanistic insight into the recovery process using deuterium-labeled linkers and 2H NMR spectroscopy. SACRed treatments could allow large extensions in the lifetime of ZIF-based membranes and adsorbents that degrade over time.},
doi = {10.1021/acsami.7b11686},
journal = {ACS Applied Materials and Interfaces},
number = 40,
volume = 9,
place = {United States},
year = {2017},
month = {9}
}

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