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

90 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

Keywords

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

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

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