Nanoporous Graphene with Single-Atom Nickel Dopants: An Efficient and Stable Catalyst for Electrochemical Hydrogen Production

Single‐atom nickel dopants anchored to three‐dimensional nanoporous graphene can be used as catalysts of the hydrogen evolution reaction (HER) in acidic solutions. In contrast to conventional nickel‐based catalysts and graphene, this material shows superior HER catalysis with a low overpotential of approximately 50 mV and a Tafel slope of 45 mV dec−1 in 0.5 M H2SO4 solution, together with excellent cycling stability. Experimental and theoretical investigations suggest that the unusual catalytic performance of this catalyst is due to sp–d orbital charge transfer between the Ni dopants and the surrounding carbon atoms. The resultant local structure with empty C–Ni hybrid orbitals is catalytically active and electrochemically stable. Single‐atom nickel dopants anchored to three‐dimensional nanoporous graphene show superior catalytic activities towards the hydrogen evolution reaction (HER) in acidic solutions. Experimental and theoretical investigations suggest that the unusual catalytic performance of this catalyst is due to sp–d orbital charge transfer between the Ni dopants and the surrounding carbon atoms.