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Title: Energy-based descriptors to rapidly predict hydrogen storage in metal–organic frameworks

Abstract

The low volumetric density of hydrogen is a critical limitation to its use as a transportation fuel. Filling a fuel tank with nanoporous materials, such as metal–organic frameworks (MOFs), could greatly improve the deliverable capacity of these tanks if appropriate materials could be found. Yet, since MOFs can be made from many combinations of metal nodes, organic linkers, and functional groups, the design space of possible MOFs is enormous. Experimental characterization of thousands of MOFs is infeasible, and even conventional molecular simulations can be prohibitively expensive for large databases. In this work, we have developed a data-driven approach to accelerate materials screening and learn structure–property relationships. We report new descriptors for gas adsorption in MOFs derived from the energetics of MOF–guest interactions. Using the bins of an energy histogram as features, we trained a sparse regression model to predict gas uptake in multiple MOF databases to an accuracy within 3 g L -1. The interpretable model parameters indicate that a somewhat weak attraction between hydrogen and the framework is ideal for cryogenic storage and release. Our machine learning method is more than three orders of magnitude faster than conventional molecular simulations, enabling rapid exploration of large numbers of MOFs. Asmore » a case study, we applied the method to screen a database of more than 50 000 experimental MOF structures. We experimentally validated one of the top candidates identified from the accelerated screening, MFU-4l. This material demonstrated a hydrogen deliverable capacity of 47 g L -1 (54 g L -1 simulated) when operating at storage conditions of 77 K, 100 bar and delivery at 160 K, 5 bar.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Publication Date:
Research Org.:
Univ. of Minnesota, Minneapolis, MN (United States). Nanoporous Materials Genome Center
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1508085
Alternate Identifier(s):
OSTI ID: 1481431
Grant/Contract Number:  
SC0008688; FG02-17ER16362
Resource Type:
Accepted Manuscript
Journal Name:
Molecular Systems Design & Engineering
Additional Journal Information:
Journal Volume: 4; Journal Issue: 1; Journal ID: ISSN 2058-9689
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Bucior, Benjamin J., Bobbitt, N. Scott, Islamoglu, Timur, Goswami, Subhadip, Gopalan, Arun, Yildirim, Taner, Farha, Omar K., Bagheri, Neda, and Snurr, Randall Q. Energy-based descriptors to rapidly predict hydrogen storage in metal–organic frameworks. United States: N. p., 2018. Web. doi:10.1039/C8ME00050F.
Bucior, Benjamin J., Bobbitt, N. Scott, Islamoglu, Timur, Goswami, Subhadip, Gopalan, Arun, Yildirim, Taner, Farha, Omar K., Bagheri, Neda, & Snurr, Randall Q. Energy-based descriptors to rapidly predict hydrogen storage in metal–organic frameworks. United States. doi:10.1039/C8ME00050F.
Bucior, Benjamin J., Bobbitt, N. Scott, Islamoglu, Timur, Goswami, Subhadip, Gopalan, Arun, Yildirim, Taner, Farha, Omar K., Bagheri, Neda, and Snurr, Randall Q. Thu . "Energy-based descriptors to rapidly predict hydrogen storage in metal–organic frameworks". United States. doi:10.1039/C8ME00050F.
@article{osti_1508085,
title = {Energy-based descriptors to rapidly predict hydrogen storage in metal–organic frameworks},
author = {Bucior, Benjamin J. and Bobbitt, N. Scott and Islamoglu, Timur and Goswami, Subhadip and Gopalan, Arun and Yildirim, Taner and Farha, Omar K. and Bagheri, Neda and Snurr, Randall Q.},
abstractNote = {The low volumetric density of hydrogen is a critical limitation to its use as a transportation fuel. Filling a fuel tank with nanoporous materials, such as metal–organic frameworks (MOFs), could greatly improve the deliverable capacity of these tanks if appropriate materials could be found. Yet, since MOFs can be made from many combinations of metal nodes, organic linkers, and functional groups, the design space of possible MOFs is enormous. Experimental characterization of thousands of MOFs is infeasible, and even conventional molecular simulations can be prohibitively expensive for large databases. In this work, we have developed a data-driven approach to accelerate materials screening and learn structure–property relationships. We report new descriptors for gas adsorption in MOFs derived from the energetics of MOF–guest interactions. Using the bins of an energy histogram as features, we trained a sparse regression model to predict gas uptake in multiple MOF databases to an accuracy within 3 g L-1. The interpretable model parameters indicate that a somewhat weak attraction between hydrogen and the framework is ideal for cryogenic storage and release. Our machine learning method is more than three orders of magnitude faster than conventional molecular simulations, enabling rapid exploration of large numbers of MOFs. As a case study, we applied the method to screen a database of more than 50 000 experimental MOF structures. We experimentally validated one of the top candidates identified from the accelerated screening, MFU-4l. This material demonstrated a hydrogen deliverable capacity of 47 g L-1 (54 g L-1 simulated) when operating at storage conditions of 77 K, 100 bar and delivery at 160 K, 5 bar.},
doi = {10.1039/C8ME00050F},
journal = {Molecular Systems Design & Engineering},
number = 1,
volume = 4,
place = {United States},
year = {2018},
month = {11}
}

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