Surface-supported cluster catalysis: Ensembles of metastable states run the show

Zandkarimi, Borna; Alexandrova, Anastassia N.

doi:10.1002/wcms.1420

Title: Surface-supported cluster catalysis: Ensembles of metastable states run the show

Journal Article · Tue May 28 00:00:00 EDT 2019 · Wiley Interdisciplinary Reviews: Computational Molecular Science

DOI:https://doi.org/10.1002/wcms.1420· OSTI ID:1594588

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Univ. of California, Los Angeles, CA (United States)

Abstract It has recently been shown that the dynamic behavior of surface‐supported nanocluster catalysts in realistic reaction conditions defies conventional models used in catalysis. This opens new doors in catalysis by giving more leverage in catalyst design, but also requires a major revision of the understanding of how dynamic heterogeneous catalytic interfaces operate, as well as of the computational approaches of catalyst modeling, and experimental methods of catalyst characterization. Major aspects of the new paradigm include the collective action of many catalyst states that form a statistical ensemble in reaction conditions, the catalytic activity and selectivity being driven by rare and metastable catalyst states, reaction thermodynamics and kinetics being controlled by different states of the catalyst, broken scaling relationships, non‐Arrhenius behaviors, and catalyst dynamic restructuring being an essential part of the reaction mechanism. For computation, this complexity means the departure from the standard density functional theory calculations of reaction mechanisms on a single catalyst structure. For experiment, it calls for the development of operando characterization tools with the per‐site resolution and the ability to find the minority sites that govern the catalytic activity. For catalyst design, the goal becomes the creation of the catalyst state (geometric and electronic) that might not be present in the as‐prepared catalyst, but would develop in the reaction conditions and would have the desired activity then. While cluster catalysts are the most dramatic in their dynamic fluxionality, other amorphous interfaces also exhibit some of it, and thus are also subject to similar paradigm revision. This article is categorized under: Structure and Mechanism > Reaction Mechanisms and Catalysis

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Research Organization:: Univ. of California, Los Angeles, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR)

Grant/Contract Number:: SC0019152

OSTI ID:: 1594588

Alternate ID(s):: OSTI ID: 1518493

Journal Information:: Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 9, Issue 6; ISSN 1759-0876

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 34 works

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Sn-modification of Pt ₇ /alumina model catalysts: Suppression of carbon deposition and enhanced thermal stability Li, Guangjing; Zandkarimi, Borna; Cass, Ashley C. The Journal of Chemical Physics, Vol. 152, Issue 2 https://doi.org/10.1063/1.5129686	journal	January 2020

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