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Toward Design of Synergistically Active Carbon-Based Catalysts for Electrocatalytic Hydrogen Evolution

Yao ZhengAustralian Institute for Bioengineering and Nanotechnology, University of Queensland, Brisbane, Queensland 4072, AustraliaYan JiaoSchool of Chemical Engineering, The University of Adelaide, Adelaide, South Australia 5005, AustraliaLu Hua LiInstitute for Frontier Materials, Deakin University, Waurn Ponds, Victoria 3216, AustraliaTan XingInstitute for Frontier Materials, Deakin University, Waurn Ponds, Victoria 3216, AustraliaYing ChenInstitute for Frontier Materials, Deakin University, Waurn Ponds, Victoria 3216, AustraliaMietek JaroniecDepartment of Chemistry and Biochemistry, Kent State University, Kent, Ohio 44240, United StatesShi‐Zhang QiaoSchool of Chemical Engineering, The University of Adelaide, Adelaide, South Australia 5005, Australia
2014en
ABI

Abstract

Replacement of precious Pt catalyst with cost-effective alternatives would be significantly beneficial for hydrogen production via electrocatalytic hydrogen evolution reaction (HER). All candidates thus far are exclusively metallic catalysts, which suffer inherent corrosion and oxidation susceptibility during acidic proton-exchange membrane electrolysis. Herein, based on theoretical predictions, we designed and synthesized nitrogen (N) and phosphorus (P) dual-doped graphene as a nonmetallic electrocatalyst for sustainable and efficient hydrogen production. The N and P heteroatoms could coactivate the adjacent C atom in the graphene matrix by affecting its valence orbital energy levels to induce a synergistically enhanced reactivity toward HER. As a result, the dual-doped graphene showed higher electrocatalytic HER activity than single-doped ones and comparable performance to some of the traditional metallic catalysts.

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