Hydrogen evolution by a metal-free electrocatalyst.
Electrocatalytic reduction of water to molecular hydrogen via the hydrogen evolution reaction may provide a sustainable energy supply for the future, but its commercial application is hampered by the use of precious platinum catalysts. All alternatives to platinum thus far are based on nonprecious metals, and, to our knowledge, there is no report about a catalyst for electrocatalytic hydrogen evolution beyond metals. Here we couple graphitic-carbon nitride with nitrogen-doped graphene to produce a metal-free hybrid catalyst, which shows an unexpected hydrogen evolution reaction activity with comparable overpotential and Tafel slope to some of well-developed metallic catalysts. Experimental observations in combination with density functional theory calculations reveal that its unusual electrocatalytic properties originate from an intrinsic chemical and electronic coupling that synergistically promotes the proton adsorption and reduction kinetics.
1] School of Chemical Engineering, University of Adelaide, Adelaide, South Australia 5005, Australia [2] Australian Institute for Bioengineering and Nanotechnology, University of Queensland, Brisbane, Queensland 4072, Australia [3].
Yao
Y
Zheng
1] School of Chemical Engineering, University of Adelaide, Adelaide, South Australia 5005, Australia [2].
Yan
Y
Jiao
Physical Sciences and Engineering Division, King Abdullah University of Science and Technology, Thuwal 23955-6900, Kingdom of Saudi Arabia.
Yihan
Y
Zhu
Institute for Frontier Materials, Deakin University, Waurn Ponds, Victoria 3216, Australia.
Lu Hua
LH
Li
Physical Sciences and Engineering Division, King Abdullah University of Science and Technology, Thuwal 23955-6900, Kingdom of Saudi Arabia.
Yu
Y
Han
Institute for Frontier Materials, Deakin University, Waurn Ponds, Victoria 3216, Australia.
Ying
Y
Chen
School of Chemistry, Physics and Mechanical Engineering, Queensland University of Technology, Brisbane, Queensland 4001, Australia.
Aijun
A
Du
Department of Chemistry and Biochemistry, Kent State University, Kent, Ohio 44242, USA.
Mietek
M
Jaroniec
School of Chemical Engineering, University of Adelaide, Adelaide, South Australia 5005, Australia.
Shi Zhang
SZ
Qiao
D002384:Catalysis; D004563:Electrochemistry / Q000379:methods*; D006108:Graphite / Q000737:chemistry; D006859:Hydrogen / Q000737:chemistry*; D007700:Kinetics; D046529:Microscopy, Electron, Transmission; D015394:Molecular Structure; D009570:Nitriles / Q000737:chemistry; D009584:Nitrogen / Q000737:chemistry; D056951:Photoelectron Spectroscopy; D014867:Water / Q000737:chemistry*; D056928:X-Ray Absorption Spectroscopy
D009570:Nitriles; D014867:Water; C011206:cyanogen; D006108:Graphite; D006859:Hydrogen; D009584:Nitrogen