Dual Graphitic-N Doping in a Six-Membered C-Ring of Graphene-Analogous Particles Enables an Efficient Electrocatalyst for the Hydrogen Evolution Reaction.
Zhiyu LinYang YangMengsi LiHao HuangWei HuLing ChengWensheng YanZhiwu YuKaitian MaoGuoliang XiaJian LuPeng JiangKang YangRuirui ZhangPengping XuChanglai WangLin HuQianwang ChenPublished in: Angewandte Chemie (International ed. in English) (2019)
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.
Keyphrases
- density functional theory
- solid state
- molecular dynamics
- room temperature
- visible light
- metal organic framework
- carbon nanotubes
- walled carbon nanotubes
- high resolution
- ionic liquid
- machine learning
- reduced graphene oxide
- deep learning
- mass spectrometry
- genome wide
- molecular dynamics simulations
- transition metal
- contrast enhanced