Structural and Chemical Evolution of an Inverse CeOx/Cu Catalyst under CO2 Hydrogenation: Tunning Oxide Morphology to Improve Activity and Selectivity

Moncada, Jorge; Chen, Xiaobo; Deng, Kaixi; Wang, Yuxi; Xu, Wenqian; Marinkovic, Nebojsa; Zhou, Guangwen; Martínez-Arias, Arturo; Rodriguez, José A.

doi:10.1021/acscatal.3c04222

Title: Structural and Chemical Evolution of an Inverse CeO_x/Cu Catalyst under CO₂ Hydrogenation: Tunning Oxide Morphology to Improve Activity and Selectivity

Journal Article · 09 November 2023 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.3c04222 · OSTI ID:2217092

^[1]; Chen, Xiaobo ^[2]; Deng, Kaixi ^[3]; Wang, Yuxi ^[3]; Xu, Wenqian ^[4];

^[5];

^[2];

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Brookhaven National Laboratory (BNL), Upton, NY (United States)
State Univ. of New York (SUNY), Binghamton, NY (United States)
Stony Brook Univ., NY (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Columbia Univ., New York, NY (United States)
Consejo Superior de Investigaciones Cientificas (CSIC), Madrid (Spain)
Brookhaven National Laboratory (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)

Small nanoparticles of ceria deposited on a powder of CuO display a very high selectivity for the production of methanol via CO₂ hydrogenation. CeO₂/CuO catalysts with ceria loadings of 5%, 20%, and 50% were investigated. Among these, the system with 5% CeO_x showed the best catalytic performance at temperatures between 200 and 350 °C. The evolution of this system under reaction conditions was studied using a combination of environmental transmission electron microscopy (E-TEM), in situ X-ray absorption spectroscopy (XAS), and time-resolved X-ray diffraction (TR-XRD). For 5% CeO_x/Cu, the in situ studies pointed to a full conversion of CuO into metallic copper, with a complete transformation of Ce⁴⁺ into Ce³⁺. Images from E-TEM showed drastic changes in the morphology of the catalyst when it was exposed to H₂, CO₂, and CO₂/H₂ mixtures. Under a CO₂/H₂ feed, there was a redispersion of the ceria particles that was detected by E-TEM and in situ TR-XRD. Finally, these morphological changes were made possible by the inverse oxide/metal configuration and facilitate the binding and selective conversion of CO₂ to methanol.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704; SC0012335; AC02-06CH11357

OSTI ID:: 2217092

Report Number(s):: BNL-225004-2023-JAAM

Journal Information:: ACS Catalysis, Vol. 13, Issue 23; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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03 NATURAL GAS
cerium oxide
copper oxide
hydrogen
CO2 hydrogenation
carbon dioxide
methanol synthesis
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ceria
copper
in situ characterization
microscopy

Title: Structural and Chemical Evolution of an Inverse CeOx/Cu Catalyst under CO2 Hydrogenation: Tunning Oxide Morphology to Improve Activity and Selectivity

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References (42)

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Title: Structural and Chemical Evolution of an Inverse CeO_x/Cu Catalyst under CO₂ Hydrogenation: Tunning Oxide Morphology to Improve Activity and Selectivity