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

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          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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          Author and article information

          Journal
          J. Am. Chem. Soc.
          Journal of the American Chemical Society
          American Chemical Society (ACS)
          1520-5126
          0002-7863
          Apr 20 2016
          : 138
          : 15
          Affiliations
          [1 ] Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, University of Science & Technology of China , Hefei, Anhui 230026, P. R. China.
          [2 ] Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials (AIIM), and School of Mechanical, Materials and Mechatronics Engineering, University of Wollongong , North Wollongong, NSW 2500, Australia.
          Article
          10.1021/jacs.6b00858
          27018462
          d30539af-2225-4c28-804a-8a87bd5ba410
          History

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