Reaction-induced regioselective reconstruction of Ni-doped Ce(OH)3/CeO2 enables exceptional activity and selectivity for reverse water-shift reaction

Wenbin Li, Bing Liu, Qing Guo, Wenjie Guo, Sai Zhang () and Yongquan Qu ()
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Wenbin Li: Northwestern Polytechnical University
Bing Liu: Jiangnan University
Qing Guo: Northwestern Polytechnical University
Wenjie Guo: Northwestern Polytechnical University
Sai Zhang: Northwestern Polytechnical University
Yongquan Qu: Northwestern Polytechnical University

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract Reconstruction of catalysts by reaction environments represents a viable approach to create highly performed active sites. Herein, we develop a reaction-induced regioselective reconstruction of Ni-doped Ce(OH)3/CeO2 nanorods to form dual-active sites composed of carburized Ni clusters and frustrated Lewis pairs (FLPs), delivering exceptional activity, selectivity and stability for reverse water-gas shift reaction. Ni aggregation in the Ce(OH)3 region, coupled with in-situ carbonization by catalytically generated CO during reaction, induces the formation of the carburized Ni clusters, which effectively promoted H2 dissociation. Additionally, Ni doping in the CeO2 region and Ce(OH)3-to-CeO2 phase transition introduce more oxygen vacancies and thereby generated FLPs in CeO2, which facilitate CO2 adsorption and subsequent hydrogenation by spilled *H species from the carburized Ni clusters. Weak CO adsorption on both the carburized Ni clusters and FLPs significantly suppresses the methanation side-reaction. This reaction-induced regioselective reconstruction strategy provides a new avenue for designing highly performed catalysts.

Date: 2025
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DOI: 10.1038/s41467-025-62771-1

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