Constructing Reactive Micro‐Environment in Basal Plane of MoS2 for pH‐Universal Hydrogen Evolution Catalysis

Abstract MoS 2 represents a promising catalyst for the hydrogen evolution reaction (HER) in water splitting, but the inefficient catalytic activity in a pH‐universal environment is an obstacle to developing practical applications. Boosting and balancing the water dissociation and hydrogen desorption kinetics is crucial in designing high‐performance catalysts for the overall pH range. Herein, it is experimentally demonstrated that cobalt single‐atom doping can effectively construct a reactive CoMoS micro‐environment on the basal plane of MoS 2 and thus alter the uniformity of surface electron density, which is further confirmed by the theoretical results. The reactive micro‐environment consisting of single‐atom Co with the surrounding Mo and S atoms possesses excellent water dissociation and hydrogen desorption kinetics, exhibiting a superior performance of 36 mV at 10 mA cm −2 with a Tafel slope of 33 mV dec −1 in the alkaline condition. Meanwhile, it also shows worthy activity in the acidic (97 mV) and neutral (117 mV) environments. This work provides a facile strategy to improve the HER catalysis of MoS 2 in pH‐universal environments.