Homologous CoP/NiCoP Heterostructure on N‐Doped Carbon for Highly Efficient and pH‐Universal Hydrogen Evolution Electrocatalysis

Abstract Hydrogen evolution electrocatalysts can achieve sustainable hydrogen production via electrocatalytic water splitting; however, designing highly active and stable noble‐metal‐free hydrogen evolution electrocatalysts that perform as efficiently as Pt catalysts over a wide pH range is a challenging task. Herein, a new 2D cobalt phosphide/nickelcobalt phosphide (CoP/NiCoP) hybrid nanosheet network is proposed, supported on an N‐doped carbon (NC) matrix as a highly efficient and durable pH‐universal hydrogen evolution reaction (HER) electrocatalyst. It is derived from topological transformation of corresponding layer double hydroxides and graphitic carbon nitride. This 2D CoP/NiCoP/NC catalyst exhibits versatile HER electroactivity with very low overpotentials of 75, 60, and 123 mV in 1 m KOH, 0.5 m H 2 SO 4 , and 1 m PBS electrolytes, respectively, delivering a current density of 10 mA cm −2 for HER. Such impressive HER performance of the hybrid electrocatalyst is mainly attributed to the collective effects of electronic structure engineering, strong interfacial coupling between CoP and NiCoP in heterojunction, an enlarged surface area/exposed catalytic active sites due to the 2D morphology, and conductive NC support. This method is believed to provide a basis for the development of efficient 2D electrode materials with various electrochemical applications.