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Title: Structure and Thermodynamic Stability of Zeolitic Imidazolate Framework Surfaces

Abstract

Extensive efforts over the last several decades have focused on the possibility of “crystal engineering” metal–organic framework (MOF) materials with bulk properties tailored toward specific applications. However, beyond their bulk structure, MOF interfaces and surfaces can also play an important role in governing the materials properties relevant to many applications, including both interfacial mass and/or charge transport. We presently examine the diversity of stable surface structures/terminations of zeolitic imidazolate frameworks (ZIFs), a subclass of MOFs, under a variety of conditions that are characteristic of either gas-phase, “post-synthetic” conditions (relevant to many MOF applications) or solution-phase conditions (typical of those used during MOF synthesis). We construct surface phase diagrams to predict the most stable ZIF surface terminations as a function of external parameters (including temperature, adsorbate pressures, and pH), making explicit comparison against prior experimental observations, when possible. Overall, we find that the resulting phase diagrams can be used to explain the results of prior experimental studies of ZIF terminations across a variety of conditions and provide important insights into the factors that govern the structure of ZIF interfaces.

Authors:
 [1]; ORCiD logo [1]
  1. Univ. of Wisconsin, Madison, WI (United States)
Publication Date:
Research Org.:
UW-Madison
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Wisconsin Alumni Research Foundation; Wisconsin Institutes for Discovery; National Science Foundation (NSF)
Contributing Org.:
UW-Madison Center for High Throughput Computing (CHTC)
OSTI Identifier:
1657503
Grant/Contract Number:  
SC0014059
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 124; Journal Issue: 2; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Free energy; Solvation; Metal organic frameworks; Solvents; Phase diagrams

Citation Formats

Weng, Tingting, and Schmidt, J. R.. Structure and Thermodynamic Stability of Zeolitic Imidazolate Framework Surfaces. United States: N. p., 2019. Web. https://doi.org/10.1021/acs.jpcc.9b10124.
Weng, Tingting, & Schmidt, J. R.. Structure and Thermodynamic Stability of Zeolitic Imidazolate Framework Surfaces. United States. https://doi.org/10.1021/acs.jpcc.9b10124
Weng, Tingting, and Schmidt, J. R.. Thu . "Structure and Thermodynamic Stability of Zeolitic Imidazolate Framework Surfaces". United States. https://doi.org/10.1021/acs.jpcc.9b10124. https://www.osti.gov/servlets/purl/1657503.
@article{osti_1657503,
title = {Structure and Thermodynamic Stability of Zeolitic Imidazolate Framework Surfaces},
author = {Weng, Tingting and Schmidt, J. R.},
abstractNote = {Extensive efforts over the last several decades have focused on the possibility of “crystal engineering” metal–organic framework (MOF) materials with bulk properties tailored toward specific applications. However, beyond their bulk structure, MOF interfaces and surfaces can also play an important role in governing the materials properties relevant to many applications, including both interfacial mass and/or charge transport. We presently examine the diversity of stable surface structures/terminations of zeolitic imidazolate frameworks (ZIFs), a subclass of MOFs, under a variety of conditions that are characteristic of either gas-phase, “post-synthetic” conditions (relevant to many MOF applications) or solution-phase conditions (typical of those used during MOF synthesis). We construct surface phase diagrams to predict the most stable ZIF surface terminations as a function of external parameters (including temperature, adsorbate pressures, and pH), making explicit comparison against prior experimental observations, when possible. Overall, we find that the resulting phase diagrams can be used to explain the results of prior experimental studies of ZIF terminations across a variety of conditions and provide important insights into the factors that govern the structure of ZIF interfaces.},
doi = {10.1021/acs.jpcc.9b10124},
journal = {Journal of Physical Chemistry. C},
number = 2,
volume = 124,
place = {United States},
year = {2019},
month = {12}
}

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