Dynamic Interconversion of Metal Active Site Ensembles in Zeolite Catalysis

Krishna, Siddarth H.; Jones, Casey B.; Gounder, Rajamani

doi:10.1146/annurev-chembioeng-092120-010920

Title: Dynamic Interconversion of Metal Active Site Ensembles in Zeolite Catalysis

Journal Article · Wed Apr 07 00:00:00 EDT 2021 · Annual Review of Chemical and Biomolecular Engineering

DOI:https://doi.org/10.1146/annurev-chembioeng-092120-010920· OSTI ID:1835589

Krishna, Siddarth H. ^[1]; Jones, Casey B. ^[1]; Gounder, Rajamani ^[1]

Purdue Univ., West Lafayette, IN (United States)

Catalysis science is founded on understanding the structure, number, and reactivity of active sites. Kinetic models that consider active sites to be static and noninteracting entities are routinely successful in describing the behavior of heterogeneous catalysts. Yet, active site ensembles often restructure in response to their external environment and even during steady-state catalytic turnover, sometimes requiring non-mean-field kinetic treatments to describe distance-dependent interactions among sites. Such behavior is being recognized more frequently in modern catalysis research, with the advent of experimental methods to quantify turnover rates with increasing precision, an expanding arsenal of operando characterization tools, and computational descriptions of atomic structure and motion at chemical potentials and timescales increasingly relevant to reaction conditions. This review focuses on dynamic changes to metal active site ensembles on zeolite supports, which are silica-based crystalline materials substituted with Al that generate binding sites for isolated and low-nuclearity metal site ensembles. Metal sites can become solvated and mobilized during reaction, facilitating interactions among sites that change their nuclearity and function. Such intersite communication can be regulated by the zeolite support, resulting in non-single-site and potentially non-mean-field kinetic behavior arising from mechanisms of catalytic action that combine elements of those canonically associated with homogeneous and heterogeneous catalysis. Here, we discuss recent literature examples that document dynamic active site behavior in metal-zeolites and outline methodologies to identify and interpret such behavior. We conclude with our outlook on future research directions to develop this evolving branch of catalysis science and harness it for practical applications.

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Research Organization:: Purdue Univ., West Lafayette, IN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: SC0019026; AC02-06CH11357

OSTI ID:: 1835589

Journal Information:: Annual Review of Chemical and Biomolecular Engineering, Vol. 12, Issue 1; ISSN 1947-5438

Publisher:: Annual ReviewsCopyright Statement

Country of Publication:: United States

Language:: English

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