Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts

Matsubu, John C.; Zhang, Shuyi; DeRita, Leo; Marinkovic, Nebojsa S.; Chen, Jingguang G.; Graham, George W.; Pan, Xiaoqing; Christopher, Phillip

doi:10.1038/NCHEM.2607

Title: Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts

Journal Article · Mon Sep 19 00:00:00 EDT 2016 · Nature Chemistry

DOI:https://doi.org/10.1038/NCHEM.2607· OSTI ID:1358016

Matsubu, John C. ^[1]; Zhang, Shuyi ^[2]; DeRita, Leo ^[1]; Marinkovic, Nebojsa S. ^[3]; Chen, Jingguang G. ^[4]; Graham, George W. ^[2]; Pan, Xiaoqing ^[5]; Christopher, Phillip ^[6]

University of California, Riverside, CA (United States). Department of Chemical and Environmental Engineering
University of California, Irvine, CA (United States). Department of Chemical Engineering and Materials Science; Univ. of Michigan, Ann Arbor, MI (United States). Department of Materials Science and Engineering
Columbia Univ., New York, NY (United States). Department of Chemical Engineering,
Columbia Univ., New York, NY (United States). Department of Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department
University of California, Irvine, CA (United States). Department of Chemical Engineering and Materials Science and Department of Physics and Astronomy
University of California, Riverside, CA (United States). Department of Chemical and Environmental Engineering, Program in Materials Science, and UCR Center for Catalysis

The optimization of supported metal catalysts predominantly focuses on engineering the metal site, for which physical insights based on extensive theoretical and experimental contributions have enabled the rational design of active sites. Although it is well known that supports can influence the catalytic properties of metals, insights into how metal–support interactions can be exploited to optimize metal active-site properties are lacking. Here in this paper, we utilize in situ spectroscopy and microscopy to identify and characterize a support effect in oxide-supported heterogeneous Rh catalysts. This effect is characterized by strongly bound adsorbates (HCO_x) on reducible oxide supports (TiO₂ and Nb₂O₅) that induce oxygen-vacancy formation in the support and cause HCO_x-functionalized encapsulation of Rh nanoparticles by the support. The encapsulation layer is permeable to reactants, stable under the reaction conditions and strongly influences the catalytic properties of Rh, which enables rational and dynamic tuning of CO₂-reduction selectivity.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; SC0012335; CHE-1301019; CBET-1159240; DMR-0723032

OSTI ID:: 1358016

Report Number(s):: BNL-113828-2017-JA; R&D Project: CO035; KC0302010

Journal Information:: Nature Chemistry, Vol. 9, Issue 2; ISSN 1755-4330

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 510 works

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