Tuning Binding Strength of Multiple Intermediates towards Efficient pH‐universal Electrocatalytic Hydrogen Evolution by Mo8O26‐NbNxOy Heterocatalysts

Abstract

AbstractDeveloping efficient and robust hydrogen evolution reaction (HER) catalysts for scalable and sustainable hydrogen production through electrochemical water splitting is strategic and challenging. Herein, heterogeneous Mo8O26‐NbNxOy supported on N‐doped graphene (defined as Mo8O26‐NbNxOy/NG) is synthesized by controllable hydrothermal reaction and nitridation process. The O‐exposed Mo8O26 clusters covalently confined on NbNxOy nanodomains provide a distinctive interface configuration and appropriate electronic structure, where fully exposed multiple active sites give excellent HER performance beyond commercial Pt/C catalyst in pH‐universal electrolytes. Theoretical studies reveal that the Mo8O26‐NbNxOy interface with electronic reconstruction affords near‐optimal hydrogen adsorption energy and enhanced initial H2O adsorption. Furthermore, the terminal O atoms in Mo8O26 clusters cooperate with Nb atoms to promote the initial H2O adsorption, and subsequently reduce the H2O dissociation energy, accelerating the entire HER kinetics.