Single-Atom-Layer Catalysis in a MoS2 Monolayer Activated by Long-Range Ferromagnetism for the Hydrogen Evolution Reaction: Beyond Single-Atom Catalysis

Hengli Duan, Chao Wang, Guinan Li, Hao Tan, Wei Hu, Liang Cai, Wei Liu, Na Li, Qianqian Ji, Yao Wang, Ying Lu, Wensheng Yan*, Fengchun Hu, Wenhua Zhang, Zhihu Sun*, Zeming Qi, Li Song, Shiqiang Wei*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

88 Scopus citations

Abstract

Single-atom-layer catalysts with fully activated basal-atoms will provide a solution to the low loading-density bottleneck of single-atom catalysts. Herein, we activate the majority of the basal sites of monolayer MoS2, by doping Co ions to induce long-range ferromagnetic order. This strategy, as revealed by in situ synchrotron radiation microscopic infrared spectroscopy and electrochemical measurements, could activate more than 50 % of the originally inert basal-plane S atoms in the ferromagnetic monolayer for the hydrogen evolution reaction (HER). Consequently, on a single monolayer of ferromagnetic MoS2 measured by on-chip micro-cell, a current density of 10 mA cm−2 could be achieved at the overpotential of 137 mV, corresponding to a mass activity of 28, 571 Ag−1, which is two orders of magnitude higher than the multilayer counterpart. Its exchange current density of 75 μA cm−2 also surpasses most other MoS2-based catalysts. Experimental results and theoretical calculations show the activation of basal plane S atoms arises from an increase of electronic density around the Fermi level, promoting the H adsorption ability of basal-plane S atoms.

Original languageEnglish (US)
Pages (from-to)7251-7258
Number of pages8
JournalAngewandte Chemie - International Edition
Volume60
Issue number13
DOIs
StatePublished - Mar 22 2021

Bibliographical note

Funding Information:
This work was financially supported by the National Natural Science Foundation of China (Grants No. 11975234, 11775225, U1632263, U1732148, 11604341 and 21533007), the Foundation for Innovative Research Groups of the National Natural Science Foundation of China (11621063), Users with Excellence Program of Hefei Science Center CAS (2019 HSC‐UE002, 2020HSC‐UE002, 2020HSC‐CIP013), and Postdoctoral Science Foundation of China (2020TQ0316 and 2019M662202). The authors would like to thank BSRF, SSRF and NSRL for the synchrotron beamtime. This work was partially carried out at the USTC Center for Micro and Nanoscale Research and Fabrication, and we thank Dianfa Zhou for his help on micro/nano devices fabrication.

Publisher Copyright:
© 2021 Wiley-VCH GmbH

Keywords

  • ferromagnetism
  • hydrogen evolution reaction
  • MoS
  • single-atom-layer catalysis
  • XAFS

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

Fingerprint

Dive into the research topics of 'Single-Atom-Layer Catalysis in a MoS2 Monolayer Activated by Long-Range Ferromagnetism for the Hydrogen Evolution Reaction: Beyond Single-Atom Catalysis'. Together they form a unique fingerprint.

Cite this