Rational Design of Single Molybdenum Atoms Anchored on N‐Doped Carbon for Effective Hydrogen Evolution Reaction

• Published in: Angewandte Chemie International Edition Vol. 56; no. 50; pp. 16086 - 16090
• Main Authors: Chen, Wenxing, Pei, Jiajing, He, Chun‐Ting, Wan, Jiawei, Ren, Hanlin, Zhu, Youqi, Wang, Yu, Dong, Juncai, Tian, Shubo, Cheong, Weng‐Chon, Lu, Siqi, Zheng, Lirong, Zheng, Xusheng, Yan, Wensheng, Zhuang, Zhongbin, Chen, Chen, Peng, Qing, Wang, Dingsheng, Li, Yadong
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 11.12.2017
• Edition: International ed. in English
• Subjects: Aberration; Atomic structure; Carbon; Catalysis; Catalysts; Density functional theory; electrocatalysis; Electrochemistry; Fine structure; hydrogen evolution reaction; Hydrogen evolution reactions; Metals; Molybdenum; N-doped carbon; Nitrogen; Scanning transmission electron microscopy; single atoms; Spectroscopy; Transmission electron microscopy; Ultrastructure; N-doped carbon; single atoms; electrocatalysis; hydrogen evolution reaction; molybdenum
• ISSN: 1433-7851; 1521-3773; 1521-3773
• DOI: 10.1002/anie.201710599

The highly efficient electrochemical hydrogen evolution reaction (HER) provides a promising pathway to resolve energy and environment problems. An electrocatalyst was designed with single Mo atoms (Mo‐SAs) supported on N‐doped carbon having outstanding HER performance. The structure of the catalyst was probed by aberration‐corrected scanning transmission electron microscopy (AC‐STEM) and X‐ray absorption fine structure (XAFS) spectroscopy, indicating the formation of Mo‐SAs anchored with one nitrogen atom and two carbon atoms (Mo1N1C2). Importantly, the Mo1N1C2 catalyst displayed much more excellent activity compared with Mo2C and MoN, and better stability than commercial Pt/C. Density functional theory (DFT) calculation revealed that the unique structure of Mo1N1C2 moiety played a crucial effect to improve the HER performance. This work opens up new opportunities for the preparation and application of highly active and stable Mo‐based HER catalysts. Single Mo atoms dispersed on N‐doped carbon was prepared as a catalyst. It showed high catalytic activity and stability for the hydrogen evolution reaction (HER), and its structure was characterized by electronic microscopy and XAFS measurements. The unique catalytic properties for HER were investigated by DFT calculations.