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Single‐Atom‐Layer Catalysis in a MoS 2 Monolayer Activated by Long‐Range Ferromagnetism for the Hydrogen Evolution Reaction: Beyond Single‐Atom Catalysis
Author(s) -
Duan Hengli,
Wang Chao,
Li Guinan,
Tan Hao,
Hu Wei,
Cai Liang,
Liu Wei,
Li Na,
Ji Qianqian,
Wang Yao,
Lu Ying,
Yan Wensheng,
Hu Fengchun,
Zhang Wenhua,
Sun Zhihu,
Qi Zeming,
Song Li,
Wei Shiqiang
Publication year - 2021
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202014968
Subject(s) - overpotential , monolayer , ferromagnetism , fermi level , atom (system on chip) , chemistry , hydrogen , catalysis , materials science , atomic physics , condensed matter physics , nanotechnology , electrochemistry , electrode , physics , organic chemistry , quantum mechanics , computer science , embedded system , electron , biochemistry
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 MoS 2 , 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 MoS 2 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 MoS 2 ‐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.