Synergistically Regulating the Electronic Structure of CoS by Cation and Anion Dual‐Doping for Efficient Overall Water Splitting

Precisely regulating the electronic construction of the reactive center is an essential method to improve the electrocatalysis, but achieving efficient multifunctional characteristics remains a challenge. Herein, CoS sample dual-doped by Cu and F atoms, as bifunctional electrocatalyst, is designed and synthesized for water electrolysis. According to the experimental results, Cu atom doping can perform primary electronic adjustment and obtain bifunctional properties, and then the electronic structure is adjusted for the second time to achieve an optimal state by introducing F atom. Meanwhile, this dual-doping strategy will result in lattice distortion and expose more active sites. As expected, dual-doped Cu-F-CoS show the brilliant electrocatalytic activity, revealing ultralow overpotentials (59 mV for HER, 213 mV for OER) at 10 mA cm-2 in alkaline electrolyte. Besides, it also exhibits distinguished water electrolysis activity with cell voltage as low as 1.52 V at 10 mA cm-2 . Our work can provide an atomic-level perception for adjusting the electronic construction of reactive sites by means of dual-doping engineering and put forward a contributing path for the electrocatalysts with multifunctional designing.