Active Site Identification and Interfacial Design of a MoP/N-Doped Carbon Catalyst for Efficient Hydrogen Evolution Reaction
Mengting Lin, Ruihu Lu, Wen Luo, Nuo Xu, Yan Zhao, Liqiang Mai
Abstract
Systematic research on potential active sites, in particular, the intrinsic mechanism between the nitrogen-doped carbon (NC) and transition metal phosphides (TMPs) is of great significance to boost the development of hydrogen evolution reaction (HER) catalysts. In this work, we designed a reliable scheme to verify the interaction of a molybdenum phosphide/NC (MoP/NC) catalyst derived from theoretical calculations. According to our screening calculations of 19 feasible active sites on MoP/NC, interface engineering of MoP/NC was proved to provide an electronic transfer from the Mo layer to the graphene layer, thereby activating N-doped graphene serve as active sites. Furthermore, the sp2 or sp3 H-adsorption patterns could effectively adjust the adsorption strength, which promotes the HER catalytic activity. Meanwhile, to confirm the calculated results, an ultrathin N-doped carbon-coated MoP globular material (MoP/NC) was constructed, whose catalytic performance greatly surpasses that of the MoP material in both acid and alkaline media. These findings deepen the understanding of the intrinsic mechanism of functional carbon-incorporated TMPs and provide scientific guidance for the interface design of an efficient HER electrocatalyst.