Single Tungsten Atoms Supported on MOF-Derived N-Doped Carbon for Robust Electrochemical Hydrogen Evolution

Wenxing Chen; Jiajing Pei; Chun-Ting He; Jiawei Wan; Hanlin Ren; Yu Wang; Juncai Dong; Konglin Wu; Weng-Chon Cheong; Junjie Mao; Xusheng Zheng; Wensheng Yan; Zhongbin Zhuang; Chen Chen; Qing Peng; Dingsheng Wang; Yadong Li

doi:10.1002/adma.201800396

Single Tungsten Atoms Supported on MOF-Derived N-Doped Carbon for Robust Electrochemical Hydrogen Evolution

Adv Mater. 2018 Jul;30(30):e1800396. doi: 10.1002/adma.201800396. Epub 2018 Jun 10.

Authors

Wenxing Chen^{1

2}, Jiajing Pei³, Chun-Ting He⁴, Jiawei Wan¹, Hanlin Ren¹, Yu Wang⁵, Juncai Dong⁶, Konglin Wu¹, Weng-Chon Cheong¹, Junjie Mao¹, Xusheng Zheng⁷, Wensheng Yan⁷, Zhongbin Zhuang³, Chen Chen¹, Qing Peng¹, Dingsheng Wang¹, Yadong Li¹

Affiliations

¹ Department of Chemistry, Tsinghua University, Beijing, 100084, China.
² Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China.
³ 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.
⁴ MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou, 510275, China.
⁵ Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204, China.
⁶ Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.
⁷ National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, China.

PMID: 29888491
DOI: 10.1002/adma.201800396

Abstract

Tungsten-based catalysts are promising candidates to generate hydrogen effectively. In this work, a single-W-atom catalyst supported on metal-organic framework (MOF)-derived N-doped carbon (W-SAC) for efficient electrochemical hydrogen evolution reaction (HER), with high activity and excellent stability is reported. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption fine structure (XAFS) spectroscopy analysis indicate the atomic dispersion of the W species, and reveal that the W₁ N₁ C₃ moiety may be the favored local structure for the W species. The W-SAC exhibits a low overpotential of 85 mV at a current density of 10 mA cm^-2 and a small Tafel slope of 53 mV dec^-1 , in 0.1 m KOH solution. The HER activity of the W-SAC is almost equal to that of commercial Pt/C. Density functional theory (DFT) calculation suggests that the unique structure of the W₁ N₁ C₃ moiety plays an important role in enhancing the HER performance. This work gives new insights into the investigation of efficient and practical W-based HER catalysts.

Keywords: N-doped carbon; electrocatalysts; hydrogen evolution reaction; metal-organic frameworks; single W atoms.