Low-Temperature Restructuring of CeO2-Supported Ru Nanoparticles Determines Selectivity in CO2 Catalytic Reduction

Aitbekova, Aisulu; Wu, Liheng; Wrasman, Cody J.; Boubnov, Alexey; Hoffman, Adam S.; Goodman, Emmett D.; Bare, Simon R.; Cargnello, Matteo

doi:10.1021/jacs.8b07615

Low-Temperature Restructuring of CeO₂-Supported Ru Nanoparticles Determines Selectivity in CO₂ Catalytic Reduction

Journal Article · Tue Sep 25 00:00:00 EDT 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.8b07615· OSTI ID:1484844

Aitbekova, Aisulu ^[1]; Wu, Liheng ^[2]; Wrasman, Cody J. ^[1]; Boubnov, Alexey ^[3]; Hoffman, Adam S. ^[3]; Goodman, Emmett D. ^[1]; Bare, Simon R. ^[3]; ^[1]

Stanford Univ., Stanford, CA (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

CO₂ reduction to higher value products is a promising way to produce fuels and key chemical building blocks while reducing CO₂ emissions. The reaction at atmospheric pressure mainly yields CH₄ via methanation and CO via the reverse water-gas shift (RWGS) reaction. Describing catalyst features that control the selectivity of these two pathways is important to determine the formation of specific products. At the same time, identification of morphological changes occurring to catalysts under reaction conditions can be crucial to tune their catalytic performance. In this contribution we investigate the dependency of selectivity for CO₂ reduction on the size of Ru nanoparticles (NPs) and on support. We find that even at rather low temperatures (210 °C), oxidative pretreatment induces redispersion of Ru NPs supported on CeO₂ and leads to a complete switch in the performance of this material from a well-known selective methanation catalyst to an active and selective RWGS catalyst. By utilizing in situ X-ray absorption spectroscopy, we demonstrate that the low-temperature redispersion process occurs via decomposition of the metal oxide phase with size-dependent kinetics, producing stable single-site RuO_x/CeO₂ species strongly bound to the CeO₂ support that are remarkably selective for CO production. Furthermore, these results show that reaction selectivity can be heavily dependent on catalyst structure and that structural changes of the catalyst can occur even at low temperatures and can go unseen in materials with less defined structures.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1484844

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 42 Vol. 140; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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