Toward design of synergistically active carbon-based catalysts for electrocatalytic hydrogen evolution.

Yao Zheng,Yan Jiao,Lu Hua Li,Ying Chen,Mietek Jaroniec,Shi Zhang Qiao,Tan Xing

doi:10.1021/nn501434a

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.

Highlights

Electrocatalytic reduction of water to molecular hydrogen via hydrogen evolution reaction (HER) provides a promising solution to energy supplies in the future
A wide variety of transition metals (Co, Ni, Fe, Mo) and derivative components have been selected as effective candidates; the inherent corrosion and oxidation susceptibility largely limits their utilization in acidic proton-exchange membrane-based electrolysis for sustainable hydrogen production.3À9 On the other hand, various carbon-based materials feature unique advantages for designated catalysis due to their tunable molecular structures, abundance, and strong tolerance to acidic/alkaline environments
To explore the effects of various dopants in graphene toward HER activity, we carried out systematic studies on the electronic properties of differently doped graphene models by density functional theory (DFT) calculations

Summary

Introduction

Electrocatalytic reduction of water to molecular hydrogen via hydrogen evolution reaction (HER) provides a promising solution to energy supplies in the future.

Results

Conclusion