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

Wenxing Chen; Jiajing Pei; Chun-Ting He; Jiawei Wan; Hanlin Ren; Youqi Zhu; Yu Wang; Juncai Dong; Shubo Tian; Weng-Chon Cheong; Siqi Lu; Lirong Zheng; Xusheng Zheng; Wensheng Yan; Zhongbin Zhuang; Chen Chen; Qing Peng; Dingsheng Wang; Yadong Li

doi:10.1002/anie.201710599

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

Angew Chem Int Ed Engl. 2017 Dec 11;56(50):16086-16090. doi: 10.1002/anie.201710599. Epub 2017 Nov 15.

Authors

Wenxing Chen¹, Jiajing Pei², Chun-Ting He³, Jiawei Wan¹, Hanlin Ren¹, Youqi Zhu¹, Yu Wang⁴, Juncai Dong⁵, Shubo Tian¹, Weng-Chon Cheong¹, Siqi Lu², Lirong Zheng⁵, Xusheng Zheng⁶, Wensheng Yan⁶, Zhongbin Zhuang², Chen Chen¹, Qing Peng¹, Dingsheng Wang¹, Yadong Li¹

Affiliations

¹ Department of Chemistry, Tsinghua University, Beijing, 100084, China.
² State Key Lab of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China.
³ MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou, 510275, China.
⁴ Shanghai Synchrontron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai, 201800, China.
⁵ Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, China.
⁶ National Synchrotron Radiation Laboratory (NSRL), University of Science and Technology of China, Hefei, Anhui, 230029, China.

PMID: 29076292
DOI: 10.1002/anie.201710599

Abstract

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 (Mo₁ N₁ C₂ ). Importantly, the Mo₁ N₁ C₂ catalyst displayed much more excellent activity compared with Mo₂ C and MoN, and better stability than commercial Pt/C. Density functional theory (DFT) calculation revealed that the unique structure of Mo₁ N₁ C₂ 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.

Keywords: N-doped carbon; electrocatalysis; hydrogen evolution reaction; molybdenum; single atoms.

Publication types

Research Support, Non-U.S. Gov't