High-throughput predictions of metal–organic framework electronic properties: theoretical challenges, graph neural networks, and data exploration

Andrew S. Rosen, Victor Fung, Patrick Huck, Cody T. O’Donnell, Matthew K. Horton, Donald G. Truhlar, Kristin A. Persson, Justin M. Notestein, Randall Q. Snurr

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

With the goal of accelerating the design and discovery of metal–organic frameworks (MOFs) for electronic, optoelectronic, and energy storage applications, we present a dataset of predicted electronic structure properties for thousands of MOFs carried out using multiple density functional approximations. Compared to more accurate hybrid functionals, we find that the widely used PBE generalized gradient approximation (GGA) functional severely underpredicts MOF band gaps in a largely systematic manner for semi-conductors and insulators without magnetic character. However, an even larger and less predictable disparity in the band gap prediction is present for MOFs with open-shell 3d transition metal cations. With regards to partial atomic charges, we find that different density functional approximations predict similar charges overall, although hybrid functionals tend to shift electron density away from the metal centers and onto the ligand environments compared to the GGA point of reference. Much more significant differences in partial atomic charges are observed when comparing different charge partitioning schemes. We conclude by using the dataset of computed MOF properties to train machine-learning models that can rapidly predict MOF band gaps for all four density functional approximations considered in this work, paving the way for future high-throughput screening studies. To encourage exploration and reuse of the theoretical calculations presented in this work, the curated data is made publicly available via an interactive and user-friendly web application on the Materials Project.

Original languageEnglish (US)
Article number112
Journalnpj Computational Materials
Volume8
Issue number1
DOIs
StatePublished - Dec 2022

Bibliographical note

Funding Information:
A.S.R. acknowledges support via a Miller Research Fellowship from the Miller Institute for Basic Research in Science, University of California, Berkeley. P.H., C.T.O., M.K.H., and K.A.P. acknowledge support by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under Contract No. DE-AC02-05-CH11231 (Materials Project program KC23MP). D.G.T. and R.Q.S. acknowledge support from the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences through the Nanoporous Materials Genome Center under Award Number DE-FG02-17ER16362. A.S.R. acknowledges computing support from the Department of Defense High Performance Computing (HPC) Modernization Program via the Mustang HPC environment at the Air Force Research Laboratory and the Onyx HPC environment at the U.S. Army Engineer Research and Development Center.

Publisher Copyright:
© 2022, The Author(s).

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