Grafting metal complexes onto amorphous supports: from elementary steps to catalyst site populations via kernel regression

Khan, Salman A.; Vandervelden, Craig A.; Scott, Susannah L.; Peters, Baron

doi:10.1039/c9re00357f

Grafting metal complexes onto amorphous supports: from elementary steps to catalyst site populations via kernel regression

Journal Article · Thu Oct 31 00:00:00 EDT 2019 · Reaction Chemistry & Engineering

DOI:https://doi.org/10.1039/c9re00357f· OSTI ID:1800093

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

Ab initio computational studies have made tremendous progress in describing the behavior of molecular (homogeneous) catalysts and crystalline versions of heterogeneous catalysts, but not for amorphous heterogeneous catalysts. Even widely used industrial amorphous catalysts like atomically dispersed Cr on silica remain poorly understood and largely intractable to computational investigation. The central problems are that (i) the amorphous support presents an unknown quenched disordered structure, (ii) metal atoms attach to various surface grafting sites with different rates, and (iii) the resulting grafted sites have different activation and catalytic reaction kinetics. This study combines kernel regression and importance sampling techniques to efficiently model grafting of metal ions onto a non-uniform ensemble of support environments. Our analysis uses a simple model of the quenched disordered support environment, grafting chemistry, and catalytic activity of the resulting grafted sites.

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), Basic Energy Sciences (BES)

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

OSTI ID:: 1800093

Journal Information:: Reaction Chemistry & Engineering, Journal Name: Reaction Chemistry & Engineering Journal Issue: 1 Vol. 5; ISSN 2058-9883

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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