Acid Gas Stability of Zeolitic Imidazolate Frameworks: Generalized Kinetic and Thermodynamic Characteristics

Bhattacharyya, Souryadeep; Han, Rebecca; Kim, Wun -Gwi; Chiang, Yadong; Jayachandrababu, Krishna C.; Hungerford, Julian T.; Dutzer, Michael R.; Ma, Chen; Walton, Krista S.; Sholl, David S.; Nair, Sankar

doi:10.1021/acs.chemmater.8b01394

Title: Acid Gas Stability of Zeolitic Imidazolate Frameworks: Generalized Kinetic and Thermodynamic Characteristics

Journal Article · Tue May 29 00:00:00 EDT 2018 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.8b01394· OSTI ID:1439424

Bhattacharyya, Souryadeep ^[1]; Han, Rebecca ^[1]; Kim, Wun -Gwi ^[1]; Chiang, Yadong ^[1]; Jayachandrababu, Krishna C. ^[1]; Hungerford, Julian T. ^[1]; Dutzer, Michael R. ^[1]; Ma, Chen ^[1]; Walton, Krista S. ^[1]; Sholl, David S. ^[1]; Nair, Sankar ^[1]

Georgia Inst. of Technology, Atlanta, GA (United States)

Here, acid gases such as SO₂ and CO₂ are present in many environments in which the use of nanoporous metal-organic frameworks (MOFs) is envisaged. Among metal-organic frameworks, zeolitic imidazolate frameworks (ZIFs) have been extensively explored as membranes or adsorbents. However, there is little systematic knowledge of the effects of acid gas exposure on the structure of ZIFs, in particular the mechanistic aspects of ZIF degradation by acid gases as well as the effects of ZIF crystal topology and linker composition on their stability. Here we present a generalized and quantitative investigation of the kinetic and thermodynamic acid gas stability of a diverse range of ZIF materials. The stability of 16 ZIFs (of SOD, RHO, ANA, and GME topologies) under different environments – humid air, liquid water, and acid gases CO₂ and SO₂ (dry, humid, and aqueous) – are investigated by a suite of experimental and computational methods. The kinetics of ZIF degradation under exposure to humid SO₂ is studied in detail, and effective rate constants for acid gas degradation of ZIFs are reported for the first time. Remarkably, the kinetics of degradation of the diverse ZIFs correlate strongly with the linker pKa and ZIF water adsorption in a manner contrary to that expected from previous predictions in the literature. Furthermore, we find that the material ZIF-71 (RHO topology) shows much higher stability relative to the other ZIFs in humid SO₂ and CO₂ environments.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME); Georgia Institute of Technology, Atlanta, GA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012577

OSTI ID:: 1439424

Journal Information:: Chemistry of Materials, Vol. 30, Issue 12; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 59 works

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