Reduction‐induced metal/oxide interfacial sites for selective CO 2 hydrogenation

Xie, Zhenhua; Hwang, Sooyeon; Chen, Jingguang G.

doi:10.1002/smm2.1201

Title: Reduction‐induced metal/oxide interfacial sites for selective CO ₂ hydrogenation

Journal Article · 28 March 2023 · SmartMat

DOI: https://doi.org/10.1002/smm2.1201 · OSTI ID:1963969

Xie, Zhenhua ^[1]; Hwang, Sooyeon ^[2];

^[1]

Department of Chemical Engineering Columbia University New York New York USA, Chemistry Division Brookhaven National Laboratory Upton New York USA
Center for Functional Nanomaterials Brookhaven National Laboratory Upton New York USA

Abstract The interfacial structures of bimetallic‐derived catalysts play an important role in promoting the activation of reactants such as CO ₂ . In particular, both the physical property (e.g., local bonding environment) and the electronic property (e.g., oxidation state) can evolve from their native states under different environments, such as upon reduction and during the catalytic reaction. Hence, taking the CO ₂ hydrogenation reaction over Rh‐based catalysts as a case study, the present work compares the interfacial structures in tuning the selectivity toward CH ₄ or CO. The combination of ex situ and in situ characterization reveals two representative interfacial structures: the Rh/CeO _x interface formed over Rh/CeO ₂ is active and selective to produce CH ₄ (~95%) by following a formate‐mediated pathway; in comparison, the InO _x /Rh interface derived after reduction is active for CO ₂ activation and enables a redox mechanism for the exclusive formation of CO (~100%). This work provides insights into the environment‐induced structural evolution at the metal−oxide interfaces, as well as the role of distinct interfacial active sites in tuning the selectivity of CO ₂ hydrogenation.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

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

Grant/Contract Number:: SC0012653; SC0012704

OSTI ID:: 1963969

Report Number(s):: BNL-224456-2023-JAAM; GRP-COCAFP-2; e1201

Journal Information:: SmartMat, Journal Name: SmartMat Journal Issue: 4 Vol. 4; ISSN 2688-819X

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

Country of Publication:: China

Language:: English

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Title: Reduction‐induced metal/oxide interfacial sites for selective CO ₂ hydrogenation