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Dual Graphitic‐N Doping in a Six‐Membered C‐Ring of Graphene‐Analogous Particles Enables an Efficient Electrocatalyst for the Hydrogen Evolution Reaction
Author(s) -
Lin Zhiyu,
Yang Yang,
Li Mengsi,
Huang Hao,
Hu Wei,
Cheng Ling,
Yan Wensheng,
Yu Zhiwu,
Mao Kaitian,
Xia Guoliang,
Lu Jian,
Jiang Peng,
Yang Kang,
Zhang Ruirui,
Xu Pengping,
Wang Changlai,
Hu Lin,
Chen Qianwang
Publication year - 2019
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201908210
Subject(s) - overpotential , graphene , electrocatalyst , xanes , tafel equation , catalysis , density functional theory , materials science , ring (chemistry) , chemistry , nanotechnology , computational chemistry , electrochemistry , organic chemistry , spectral line , physics , electrode , astronomy
Abstract Graphene‐based materials still exhibit poor electrocatalytic activities for the hydrogen evolution reaction (HER) although they are considered to be the most promising electrocatalysts. We fabricated a graphene‐analogous material displaying exceptional activity towards the HER under acidic conditions with an overpotential (57 mV at 10 mA cm −2 ) and Tafel slope (44.6 mV dec −1 ) superior to previously reported graphene‐based materials, and even comparable to the state‐of‐the art Pt/C catalyst. X‐ray absorption near‐edge structure (XANES) and solid‐state NMR studies reveal that the distinct feature of its structure is dual graphitic‐N doping in a six‐membered carbon ring. Density functional theory (DFT) calculations show that the unique doped structure is beneficial for the activation of C−H bonds and to make the carbon atom bonded to two graphitic N atoms an active site for the HER.