Interface engineering of heterostructural Ni‐Ni0.2Mo0.8N boosts alkaline hydrogen electrocatalysis

Exploring efficient and low-cost bifunctional catalysts for hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR) is highly desirable for the achievement of unitized regenerative fuel cells. Herein, a facile method to prepare hetero-interfacial Ni-Ni0.2Mo0.8N nanosheets with tailored d-center center for efficient alkaline hydrogen electrocatalysis is presented. Mechanism studies indicate that interface engineering can shift down the d-band center of Ni-Ni0.2Mo0.8N nanosheets due to the electron transfer from Ni to Ni0.2Mo0.8N, which weakens the binding strength of reaction intermediates, thereby boosting the catalytic performance. Relative to pure Ni, Ni-Ni0.2Mo0.8N nanosheets show a lower overpotential of 83 mV at -10 mA cm-2 and good stability during 2,000 cycles for HER. Meanwhile, Ni-Ni0.2Mo0.8N nanosheets exhibit an improved exchange current density for HOR with a 10.2-fold enhancement in comparison with that of pure Ni. This work provides valuable insight into the reasonable design of efficient energy-related electrocatalysts based on the tailoring of d-band center by interface engineering.