MOFs with the Stability for Practical Gas Adsorption Applications Require New Design Rules
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Oh_ACSAMI_2024.pdf
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Accepted version
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7.35 MB
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Author(s)
Oh, Changhwan
Nandy, Aditya
Yue, Shuwen
Kulik, Heather J
Date Issued
October 4, 2024
Journal
ACS Applied Materials & Interfaces
Publisher
American Chemical Society
Citation
Oh, Changhwan, Nandy, Aditya, Yue, Shuwen and Kulik, Heather J. 2024. "MOFs with the Stability for Practical Gas Adsorption Applications Require New Design Rules." ACS Applied Materials & Interfaces, 16 (41).
Version
Author's final manuscript
Abstract
Metal-organic frameworks (MOFs) have been widely studied for their ability to capture and store greenhouse gases. However, most computational discovery efforts study hypothetical MOFs without consideration of their stability, limiting the practical application of novel materials. We overcome this limitation by screening hypothetical ultrastable MOFs that have predicted high thermal and activation stability, as judged by machine learning (ML) models trained on experimental measures of stability. We enhance this set by computing the bulk modulus as a measure of mechanical stability and filter 1102 mechanically robust hypothetical MOFs from a database of ultrastable MOFs (USMOF DB). Grand Canonical Monte Carlo simulations are then employed to predict the gas adsorption properties of these hypothetical MOFs, alongside a database of experimental MOFs. We identify privileged building blocks that lead MOFs in USMOF DB to show exceptional working capacities compared to the experimental MOFs. We interpret these differences by training ML models on CO2 and CH4 adsorption in these databases, showing how poor model transferability between data sets indicates that novel design rules can be derived from USMOF DB that would not have been gathered through assessment of structurally characterized MOFs. We identify geometric features and node chemistry that will enable the rational design of MOFs with enhanced gas adsorption properties in synthetically realizable MOFs.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Materials Science and Engineering
Massachusetts Institute of Technology. Department of Chemistry
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Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
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DOI of Published Version
10.1021/acsami.4c13250
