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Vacancy engineering plays vital role in the design of high‐performance electrocatalysts. Here, we introduced coupled cation‐vacancy pairs in Ni‐doped CoSe to achieve boosted hydrogen evolution reaction (HER) activity through a facile topochemical intercalation approach. Adjacent Co vacancy pairs and heteroatom Ni doping contribute together for the upshift of the Se 4pz orbital, which induces larger...
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