As a clean and promising hydrogen production process, the electrochemical hydrogen evolution reaction (HER) is particularly important. However, its electrocatalytic activity is usually limited by the acid or base environment of the electrolyte. To achieve efficient conversion in energy storage, developing cost-effective nonprecious HER electrocatalysts at all pH values is highly required. Herein, defect-rich porous CoS 1.097 /MoS 2 hybrid microspheres are synthesized via a one-step sulfurization method. As expected, the optimal pH-universal CoS 1.097 /MoS 2 HER electrocatalyst shows overpotentials of 228, 249, and 341 mV at −10 mA cm −2 and small Tafel slopes of 59, 75, and 85 mV dec −1 in 0.5 M H 2 SO 4 , 1.0 M KOH, and 0.1 M PBS electrolyte, respectively. Furthermore, the CoS 1.097 /MoS 2 also presents outstanding HER catalytic stability in a 21 h stability test. The outstanding performance of CoS 1.097 /MoS 2 can be ascribed to the synergetic interplay of CoS 1.097 and MoS 2 , with abundant defects and a hierarchically ordered interconnected micro/mesoporous structure.
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