Importance learning estimator for the site-averaged turnover frequency of a disordered solid catalyst

Vandervelden, Craig A.; Khan, Salman A.; Peters, Baron

doi:10.1063/5.0037450

Importance learning estimator for the site-averaged turnover frequency of a disordered solid catalyst

Journal Article · Sun Dec 27 23:00:00 EST 2020 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0037450· OSTI ID:1849456

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Univ. of California, Santa Barbara, CA (United States). Dept. of Chemical Engineering; Univ. of Illinois at Urbana-Champaign, IL (United States)
Univ. of California, Santa Barbara, CA (United States). Dept. of Chemical Engineering
Univ. of Illinois at Urbana-Champaign, IL (United States). Chemical and Biomolecular Engineering; Univ. of Illinois at Urbana-Champaign, IL (United States). Dept. of Chemistry

For disordered catalysts such as atomically dispersed “single-atom” metals on amorphous silica, the active sites inherit different properties from their quenched-disordered local environments. The observed kinetics are site-averages, typically dominated by a small fraction of highly active sites. Standard sampling methods require expensive ab initio calculations at an intractable number of sites to converge on the siteaveraged kinetics. We present a new method that efficiently estimates the site-averaged turnover frequency (TOF). The new estimator uses the same importance learning algorithm [Vandervelden et al., React. Chem. Eng. 5, 77 (2020)] that we previously used to compute the siteaveraged activation energy. We demonstrate the method by computing the site-averaged TOF for a simple disordered lattice model of an amorphous catalyst. The results show that with the importance learning algorithm, the site-averaged TOF and activation energy can now be obtained concurrently with orders of magnitude reduction in required ab initio calculations.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of California, Santa Barbara, CA (United States); Univ. of Kansas, Lawrence, KS (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: FG02-03ER15467; SC0019488

OSTI ID:: 1849456

Alternate ID(s):: OSTI ID: 1752972

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 24 Vol. 153; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Importance learning estimator for the site-averaged turnover frequency of a disordered solid catalyst

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