期刊
ADVANCED SCIENCE
卷 6, 期 10, 页码 -出版社
WILEY
DOI: 10.1002/advs.201900119
关键词
chemical doping; electrochemical water splitting; graphene edge; noble metal-free catalysts; scanning electrochemical cell microscopy
资金
- JST-PRESTO Creation of Innovative Core Technology for Manufacture and Use of Energy Carriers from Renewable Energy [JPMJPR1541, JPMJPR1444, JPMJPR14FA]
- JSPS [JP18H04477, JP17H06460]
- JSPS KAKENHI [JP18K14174, JP16K17855, JP16H02280, JP18H03858, JP16H06042, JP17K19135, JP15H05422, JP15K13263, JP16H00885]
- World Premier International Research Center Initiative (WPI), MEXT, Japan
- NIMS microstructural characterization platform and Molecule AMP
- Material Synthesis Platform as a program of Nanotechnology Platform Project, MEXT, Japan
- University of Tsukuba Basic Research Support Program Type S
- Iwatani Naoji Foundation
- Intelligent Cosmos Academic Foundation
Carbon-based metal-free catalysts for the hydrogen evolution reaction (HER) are essential for the development of a sustainable hydrogen society. Identification of the active sites in heterogeneous catalysis is key for the rational design of low-cost and eff icient catalysts. Here, by fabricating holey graphene with chemically dopants, the atomic-level mechanism for accelerating HER by chemical dopants is unveiled, through elemental mapping with atomistic characterizations, scanning electrochemical cell microscopy (SECCM), and density functional theory (DFT) calculations. It is found that the synergetic effects of two important factors-edge structure of graphene and nitrogen/phosphorous codoping-enhance HER activity. SECCM evidences that graphene edges with chemical dopants are electrochemically very active. Indeed, DFT calculation suggests that the pyridinic nitrogen atom could be the catalytically active sites. The HER activity is enhanced due to phosphorus dopants, because phosphorus dopants promote the charge accumulations on the catalytically active nitrogen atoms. These findings pave a path for engineering the edge structure of graphene in graphene-based catalysts.
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