Water induced ultrathin Mo2C nanosheets with high-density grain boundaries for enhanced hydrogen evolution

Yang Yang, Yumin Qian, Zhaoping Luo, Haijing Li, Lanlan Chen, Xumeng Cao, Shiqiang Wei, Bo Zhou, Zhenhua Zhang, Shuai Chen, Wenjun Yan, Juncai Dong, Li Song, Wenhua Zhang, Renfei Feng, Jigang Zhou, Kui Du, Xiuyan Li, Xian-Ming Zhang () and Xiujun Fan ()
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Yang Yang: Shanxi University
Yumin Qian: Beijing Institute of Technology, Haidian
Zhaoping Luo: Chinese Academy of Sciences
Haijing Li: Chinese Academy of Sciences
Lanlan Chen: University of Science and Technology of China
Xumeng Cao: Chinese Academy of Sciences
Shiqiang Wei: University of Science and Technology of China
Bo Zhou: Beijing University of Technology
Zhenhua Zhang: Hangzhou Dianzi University
Shuai Chen: Chinese Academy of Sciences
Wenjun Yan: Chinese Academy of Sciences
Juncai Dong: Chinese Academy of Sciences
Li Song: University of Science and Technology of China
Wenhua Zhang: University of Science and Technology of China
Renfei Feng: Canadian Light Source
Jigang Zhou: Canadian Light Source
Kui Du: Chinese Academy of Sciences
Xiuyan Li: Chinese Academy of Sciences
Xian-Ming Zhang: Shanxi University
Xiujun Fan: Shanxi University

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Grain boundary controlling is an effective approach for manipulating the electronic structure of electrocatalysts to improve their hydrogen evolution reaction performance. However, probing the direct effect of grain boundaries as highly active catalytic hot spots is very challenging. Herein, we demonstrate a general water-assisted carbothermal reaction strategy for the construction of ultrathin Mo2C nanosheets with high-density grain boundaries supported on N-doped graphene. The polycrystalline Mo2C nanosheets are connected with N-doped graphene through Mo–C bonds, which affords an ultra-high density of active sites, giving excellent hydrogen evolution activity and superior electrocatalytic stability. Theoretical calculations reveal that the dz2 orbital energy level of Mo atoms is controlled by the MoC3 pyramid configuration, which plays a vital role in governing the hydrogen evolution activity. The dz2 orbital energy level of metal atoms exhibits an intrinsic relationship with the catalyst activity and is regarded as a descriptor for predicting the hydrogen evolution activity.

Date: 2022
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DOI: 10.1038/s41467-022-34976-1

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