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Machine Learning the Quantum-Chemical Properties of Metal–Organic Frameworks for Accelerated Materials Discovery with a New Electronic Structure Database

preprint
submitted on 29.10.2020, 03:28 and posted on 29.10.2020, 19:00 by Andrew Rosen, Shaelyn Iyer, Debmalya Ray, Zhenpeng Yao, Alan Aspuru-Guzik, Laura Gagliardi, Justin Notestein, Randall Q. Snurr

Metal–organic frameworks (MOFs) are a widely investigated class of crystalline solids with tunable structures that make it possible to impart specific chemical functionality tailored for a given application. However, the enormous number of possible MOFs that can be synthesized makes it difficult to determine which materials would be the most promising candidates, especially for applications governed by electronic structure properties that are often computationally demanding to simulate and time-consuming to probe experimentally. Here, we have developed the first publicly available quantum-chemical database for MOFs (the “QMOF database”), which consists of properties derived from density functional theory (DFT) for over 14,000 experimentally synthesized MOFs. Throughout this study, we demonstrate how this new database can be used to identify MOFs with targeted electronic structure properties. As a proof-of-concept, we use the QMOF database to evaluate the performance of several machine learning models for the prediction of DFT-computed band gaps and find that crystal graph convolutional neural networks are capable of achieving superior predictive performance, making it possible to circumvent computationally expensive quantum-chemical calculations. We also show how unsupervised learning methods can aid the discovery of otherwise subtle structure–property relationships using the computational findings in this work. We conclude by highlighting several MOFs with low band gaps, a challenging task given the electronically insulating nature of most MOF structures. The data and predictive models generated in this work, as well as the database of MOF structures, should be highly useful to other researchers interested in the predictive design and discovery of MOFs for the many applications dictated by quantum-chemical phenomena.

Funding

National Defense Science and Engineering Graduate Fellowship

Nanoporous Materials Genome Center (DE-FG02-17ER16362)

History

Email Address of Submitting Author

rosen@u.northwestern.edu

Institution

Northwestern University

Country

United States

ORCID For Submitting Author

0000-0002-0141-7006

Declaration of Conflict of Interest

R.Q.S. has a financial interest in the start-up company NuMat Technologies, which is seeking to commercialize metal−organic frameworks.

Exports