It is not enough to develop an ideal hydrogen evolution reaction (HER) electrocatalysts by single strategy. Here, the HER performances are significantly improved by the combined strategies of P and Se binary vacancies and heterostructure engineering, which is rarely explored and remain unclear. As a result, the overpotentials of MoP/MoSe -H heterostructures rich in P and Se binary vacancies are 47 and 110 mV at 10 mA cm in 1 m KOH and 0.
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