Modulating the dynamic change of catalysts is significant for understanding the mechanism and exploiting better electrocatalysts but remains challenging in oxygen evolution reaction (OER). Herein, ceria-promoted reconstruction of Ni-X (X = S, P, and O) is investigated to unravel the correlation between the reconstructed surface and the OER performance, which further guides the design of prominent electrocatalysts. Interfacial CeO 2 promotes the in situ reconfiguration of Ni-X via strengthening hydroxyl adsorption, generating highly active CeO 2 -NiOOH interfaces. Moreover, rich oxygen vacancies formed after breaking Ni-S/P bonds and leaching S/P anions render Ni 3 S 2 and Ni 2 P superior to NiO with the same CeO 2 modification, highlighting another dependence on pre-catalyst materials chemistry. Theoretical analysis further confirms that the co-presence of CeO 2 -NiOOH interfaces and oxygen vacancies can harmoniously regulate intermediate chemisorption toward favorable OER kinetics. As a proof of concept, CeO 2 -modified Ni 3 S 2 exhibits low overpotentials of 251 and 364 mV at the current densities of 10 and 100 mA cm −2 in 1.0 M KOH, respectively, performing among the best of recently reported Ni-based counterparts.
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