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Delocalized Spin States in 2D Atomic Layers Realizing Enhanced Electrocatalytic Oxygen Evolution
Advanced Materials ( IF 27.4 ) Pub Date : 2017-06-08 , DOI: 10.1002/adma.201701687
Shichuan Chen 1 , Zhixiong Kang 1 , Xin Hu 2 , Xiaodong Zhang 1 , Hui Wang 1 , Junfeng Xie 1 , XuSheng Zheng 3 , Wensheng Yan 3 , Bicai Pan 1 , Yi Xie 1
Advanced Materials ( IF 27.4 ) Pub Date : 2017-06-08 , DOI: 10.1002/adma.201701687
Shichuan Chen 1 , Zhixiong Kang 1 , Xin Hu 2 , Xiaodong Zhang 1 , Hui Wang 1 , Junfeng Xie 1 , XuSheng Zheng 3 , Wensheng Yan 3 , Bicai Pan 1 , Yi Xie 1
Affiliation
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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.
中文翻译：
实现增强的电催化氧放出的2D原子层中的离域自旋态
过渡金属基化合物的电催化活性与金属原子的自旋态密切相关。然而，调节催化剂自旋态的方式仍然有限，并且自旋态与催化活性之间的潜在关系仍然不清楚。在这里，第一次，通过服用镍II例如，基于基团的化合物没有高或低的自旋态，表明它们的自旋态可以在向原子层引入结构变形后发生离域化。Ni原子的离域自旋态不仅可以提供高电导率，而且可以在系统的活性位点和反应中间体之间提供低吸附能。不出所料，与相应的大块样品相比，具有结构变形的镍硫属元素化物超薄纳米片在电催化氧释放方面显示出显着增强的活性。这项工作通过调节自旋态，为设计过渡金属基化合物中的高级电催化剂建立了新途径。
更新日期：2017-06-08
中文翻译：
实现增强的电催化氧放出的2D原子层中的离域自旋态
过渡金属基化合物的电催化活性与金属原子的自旋态密切相关。然而，调节催化剂自旋态的方式仍然有限，并且自旋态与催化活性之间的潜在关系仍然不清楚。在这里，第一次，通过服用镍II例如，基于基团的化合物没有高或低的自旋态，表明它们的自旋态可以在向原子层引入结构变形后发生离域化。Ni原子的离域自旋态不仅可以提供高电导率，而且可以在系统的活性位点和反应中间体之间提供低吸附能。不出所料，与相应的大块样品相比，具有结构变形的镍硫属元素化物超薄纳米片在电催化氧释放方面显示出显着增强的活性。这项工作通过调节自旋态，为设计过渡金属基化合物中的高级电催化剂建立了新途径。
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