Activating the hydrogen evolution reaction in low-dimensional carbon by partial hydrogenation: Role of the hybrid sp^(2) -sp^(3) orbital interface

Developing highly efficient catalyst for the hydrogen evolution reaction(HER)and understanding their mecha-nism is crucial for establishing the hydrogen economy.Carbon-based materials are particularly attractive as HER catalysts because of their abundance and morphological variety.Herein,using density functional theory(DFT)calculations,we propose for the first time a virtual interface consisting of sp^(2) and sp^(3) orbitals of carbon,for acti-vating the intrinsically inert low-dimensional carbon toward the HER.This hybrid orbital interface is generated by pre-adsorbed hydrogen introduced by the partial hydrogenation of these low-dimensional carbon materials(C_(60),carbon nanotubes and graphene).The pre-adsorbed hydrogen can activate adjacent carbon atoms to become active sites for the HER.The best performance among these sites is comparable to that of the commercial Pt/C catalyst.Given that the partial hydrogenation of low-dimensional carbon has been experimentally realized,our work provides a simple yet novel concept for HER catalyst design.