Nickel single atom-decorated carbon nanosheets as multifunctional electrocatalyst supports toward efficient alkaline hydrogen evolution

Abstract Tailoring catalysts with balanced adsorption capabilities toward multiple reaction intermediates is highly desirable for complex electrocatalytic reactions, but rather challenging. Here, Ni single atom-decorated carbon nanosheets are developed as multifunctional supports for engineering heterostructured electrocatalysts toward hydrogen evolution in alkaline media. The Ni single atoms (Ni–N4) are actively dedicated to cleaving the H–OH bonds as well as facilitating Had spillover to metallic Pt sites. For the case of supported Pt electrocatalysts, a Pt/PtOx configuration is generated at the heterointerface via Pt–O–C (Ni) interfacial bonding, with oxidized Pt species located at the interface and metallic Pt formed in the near-interface area. Further, the oxidized Pt species are also active for boosting the water dissociation step. These findings not only open up a new avenue toward the development of multifunctional catalyst supports but also demonstrate the importance of regulating interface chemistry of heterostructured electrocatalysts at atomic level.