Reaction-induced regioselective reconstruction of Ni-doped Ce(OH)3/CeO2 enables exceptional activity and selectivity for reverse water-shift reaction
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Reconstruction of catalysts by reaction environments represents a viable approach to create highly performed active sites. Herein, we developed a reaction-induced regioselective reconstruction of Ni-doped Ce(OH) 3 /CeO 2 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 of Ni by catalytically generated CO during reaction, induced the formation of the carburized Ni clusters, which effectively promoted H 2 dissociation. Additionally, Ni doping in the CeO 2 region and Ce(OH) 3 -to-CeO 2 phase transition introduced more oxygen vacancies and thereby generated FLPs in CeO 2 , which facilitated CO 2 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 suppressed the methanation side-reaction. This reaction-induced regioselective reconstruction strategy provides a new avenue for designing highly performed catalysts.
