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

• Published in: ACS nano Vol. 8; no. 5; pp. 5290 - 5296
• Main Authors: Zheng, Yao, Jiao, Yan, Li, Lu Hua, Xing, Tan, Chen, Ying, Jaroniec, Mietek, Qiao, Shi Zhang
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 27-05-2014
• Subjects: Catalysis; Catalysts; Electrocatalysts; Energy levels; Graphene; Hydrogen evolution; Hydrogen production; Nanostructure; metal-free catalysis; synergistic catalysis; hydrogen evolution; dual-doped graphene; theoretical prediction
• ISSN: 1936-0851; 1936-086X
• DOI: 10.1021/nn501434a

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.