Steam‐Assisted Selective CO 2 Hydrogenation to Ethanol over Ru−In Catalysts

Zhou, Chengshuang; Aitbekova, Aisulu; Liccardo, Gennaro; Oh, Jinwon; Stone, Michael L.; McShane, Eric J.; Werghi, Baraa; Nathan, Sindhu; Song, Chengyu; Ciston, Jim; Bustillo, Karen C.; Hoffman, Adam S.; Hong, Jiyun; Perez‐Aguilar, Jorge; Bare, Simon R.; Cargnello, Matteo

doi:10.1002/ange.202406761

Title: Steam‐Assisted Selective CO ₂ Hydrogenation to Ethanol over Ru−In Catalysts

Journal Article · 04 September 2024 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.202406761 · OSTI ID:2530488

^[1]; Aitbekova, Aisulu ^[2]; Liccardo, Gennaro ^[3]; Oh, Jinwon ^[4]; Stone, Michael L. ^[1];

^[1]; Werghi, Baraa ^[5]; Nathan, Sindhu ^[1]; Song, Chengyu ^[6];

^[6]; Bustillo, Karen C. ^[6]; Hoffman, Adam S. ^[7]; Hong, Jiyun ^[7]; Perez‐Aguilar, Jorge ^[7]; Bare, Simon R. ^[7];

^[3]

Department of Chemical Engineering Stanford University Stanford California 94305 United States
Applied Physics and Materials Science California Institute of Technology Pasadena California 91125 United States
Department of Chemical Engineering Stanford University Stanford California 94305 United States, SUNCAT Center for Interface Science and Catalysis Stanford University Stanford California 94305 United States
Department of Materials Science and Engineering Stanford University Stanford California 94305 United States
Department of Chemical Engineering Stanford University Stanford California 94305 United States, SUNCAT Center for Interface Science and Catalysis Stanford University Stanford California 94305 United States, SLAC National Accelerator Laboratory 2575 Sand Hill Road Menlo Park California 94305 United States
National Center for Electron Microscopy Facility Molecular Foundry Lawrence Berkeley National Lab Berkeley California 94720 United States
SLAC National Accelerator Laboratory 2575 Sand Hill Road Menlo Park California 94305 United States

Abstract Multicomponent catalysts can be designed to synergistically combine reaction intermediates at interfacial active sites, but restructuring makes systematic control and understanding of such dynamics challenging. We here unveil how reducibility and mobility of indium oxide species in Ru‐based catalysts crucially control the direct, selective conversion of CO ₂ to ethanol. When uncontrolled, reduced indium oxide species occupy the Ru surface, leading to deactivation. With the addition of steam as a mild oxidant and using porous polymer layers to control In mobility, Ru−In ₂ O ₃ interface sites are stabilized, and ethanol can be produced with superior overall selectivity (70 %, rest CO). Our work highlights how engineering of bifunctional active ensembles enables cooperativity and synergy at tailored interfaces, which unlocks unprecedented performance in heterogeneous catalysts.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515

OSTI ID:: 2530488

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 41 Vol. 136; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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