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Adv Mater. 2017 Aug;29(30). doi: 10.1002/adma.201701687. Epub 2017 Jun 8.

Delocalized Spin States in 2D Atomic Layers Realizing Enhanced Electrocatalytic Oxygen Evolution.

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Hefei National Laboratory for Physical Science at the Microscale, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, 230026, P. R. China.
College of Chemistry and Chemical Engineering, Xinjiang Normal University, Urumqi, Xinjiang, 830054, P. R. China.
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, P. R. China.


The electrocatalytic activity of transition-metal-based compounds is strongly related to the spin states of metal atoms. However, the ways for regulation of spin states of catalysts are still limited, and the underlying relationship between the spin states and catalytic activities remains unclear. Herein, for the first time, by taking NiII -based compounds without high or low spin states for example, it is shown that their spin states can be delocalized after introducing structural distortion to the atomic layers. The delocalized spin states for Ni atoms can provide not only high electrical conductivity but also low adsorption energy between the active sites and reaction intermediates for the system. As expected, the ultrathin nanosheets of nickel-chalcogenides with structural distortions show dramatically enhanced activity in electrocatalytic oxygen evolution compared to their corresponding bulk samples. This work establishes new way for the design of advanced electrocatalysts in transition-metal-based compounds via regulation of spin states.


2D materials; electrocatalysis; oxygen evolution; spin states


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