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Heterogeneous Spin States in Ultrathin Nanosheets Induce Subtle Lattice Distortion To Trigger Efficient Hydrogen Evolution

Liu, Youwen, Hua, Xuemin, Xiao, Chong, Zhou, Tengfei, Huang, Pengcheng, Guo, Zaiping, Pan, Bicai, Xie, Yi·2016·Journal of the American Chemical Society

Abstract

The exploration of efficient nonprecious metal eletrocatalysis of the hydrogen evolution reaction (HER) is an extraordinary challenge for future applications in sustainable energy conversion. The family of first-row-transition-metal dichalcogenides has received a small amount of research, including the active site and dynamics, relative to their extraordinary potential. In response, we developed a strategy to achieve synergistically active sites and dynamic regulation in first-row-transition-metal dichalcogenides by the heterogeneous spin states incorporated in this work. Specifically, taking the metallic Mn-doped pyrite CoSe2 as a self-adaptived, subtle atomic arrangement distortion to provide additional active edge sites for HER will occur in the CoSe2 atomic layers with Mn incorporated into the primitive lattice, which is visually verified by HRTEM. Synergistically, the density functional theory simulation results reveal that the Mn incorporation lowers the kinetic energy barrier by promoting H-H bond formation on two adjacently adsorbed H atoms, benefiting H2 gas evolution. As a result, the Mn-doped CoSe2 ultrathin nanosheets possess useful HER properties with a low overpotential of 174 mV, an unexpectedly small Tafel slope of 36 mV/dec, and a larger exchange current density of 68.3 μA cm(-2). Moreover, the original concept of coordinated regulation presented in this work can broaden horizons and provide new dimensions in the design of newly highly efficient catalysts for hydrogen evolution.

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Metadata

Authors
Liu, Y., Hua, X., Xiao, C., Zhou, T., Huang, P., Guo, Z., Pan, B., & Xie, Y.
Venue
Journal of the American Chemical Society
Published
2016-04-08
Volume
138
Issue
15
Pages
5087-5092
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
OpenAlex
W2340565403
Cited by
425
References
19
FWCI
15.73
Type
journal article
Language
en
Open access
closed
Funders
  • Ministry of Education of the People's Republic of China (WK2060190027, WK2340000063)
  • National Natural Science Foundation of China (11321503, 21331005, 21401182, 91422303, U1532265)
  • National Basic Research Program of China (2015CB932302)
  • Youth Innovation Promotion Association of the Chinese Academy of Sciences (2016392)
  • The Key Laboratory of Neutron Physics (CAEP 2014DB02)

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CoChat. (2026). Citation check: Heterogeneous Spin States in Ultrathin Nanosheets Induce Subtle Lattice Distortion To Trigger Efficient Hydrogen Evolution. https://app.cochat.ai/papers/10.1021/jacs.6b00858
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Liu, Y., Hua, X., Xiao, C., Zhou, T., Huang, P., Guo, Z., Pan, B., & Xie, Y. (2016). Heterogeneous Spin States in Ultrathin Nanosheets Induce Subtle Lattice Distortion To Trigger Efficient Hydrogen Evolution. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.6b00858

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