Abstract
Boosting the hydrogen evolution reaction (HER) process with highly efficient non-noble metal catalysts is crucial for hydrogen-powered fuel cells. Pyrite-type NiSe2 is one of the most promising HER catalysts due to its inexpensive cost and good conductivity, although its intrinsic activity is moderate. Using a plasma etching method on a carbon cloth substrate material, we created a large number of selenium vacancies on NiSe2 nanosheets (NiSe2-VSe/CC). With a low overpotential of 91 mV and a Tafel slope of 91 mV dec–1 at 10 mA cm–2, as well as a durability of 20 h at high current (100 mA cm–2), the NiSe2-VSe/CC demonstrates superior HER performance for its catalytic activity and long-term stability. Cross-validated by measurement analyses and density functional theory calculations, the introduction of vacancies reduces the resistivity of NiSe2 and optimizes its hydrogen adsorption energy (GH*) and water adsorption energy (GH2O*). Based on defect engineering, this study proposes an approach to designing improved electrocatalysts for alkaline HER.
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