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<p>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)<sub>3</sub>/CeO<sub>2</sub> 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)<sub>3</sub> region, coupled with in-situ carbonization by catalytically generated CO during reaction, induces the formation of the carburized Ni clusters, which effectively promoted H<sub>2</sub> dissociation. Additionally, Ni doping in the CeO<sub>2</sub> region and Ce(OH)<sub>3</sub>-to-CeO<sub>2</sub> phase transition introduce more oxygen vacancies and thereby generated FLPs in CeO<sub>2</sub>, which facilitate CO<sub>2</sub> 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.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月8日

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  • Wenbin Li,
  • Bing Liu,
  • Qing Guo,
  • Wenjie Guo,
  • Sai Zhang,
  • Yongquan Qu

摘要

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.