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Isoelectric Si Heteroatoms as Electron Traps for N2 Fixation and Activation
Advanced Functional Materials ( IF 19.0 ) Pub Date : 2020-09-16 , DOI: 10.1002/adfm.202005779
Guang‐Yao Zhai 1 , Dong Xu 1 , Shi‐Nan Zhang 1 , Zhong‐Hua Xue 1 , Hui Su 1 , Qiu‐Ying Yu 1 , Hong‐Hui Wang 1 , Xiu Lin 1 , Yun‐Xiao Lin 1 , Lu‐Han Sun 1 , Xin‐Hao Li 1 , Jie‐Sheng Chen 1
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Doping the host materials with either electron‐rich heteroatoms or electron‐deficient heteroatoms have been applied as a straightforward and main‐stream method to modify the electronic structures and boost the electrochemical activity for various reactions, including nitrogen reduction reactions (NRR). As the third type of dopants, isoelectric heteroatoms (exemplified with Si atoms in carbon framework in this work) have been designed as highly efficient active centers for NRR. As the same group element with a different size and electronegativity to carbon support, the isoelectric Si heteroatom (Iso‐e Si) creates localized singularities with a lone orbital that can act as an electron trap for pre‐adsorbed N2 molecules through coulomb interaction and thus facilitates the following activation process for NRR. Iso‐e Si atom thus functions as a special type of metal‐free single atom‐based electrocatalyst to largely boost the faradaic efficiency of pristine carbon support for NRR by a factor of 12, giving a remarkably high turnover frequency value of 0.52 h−1, comparable to atomically dispersed transition metal‐based electrocatalysts.

中文翻译:

等电硅杂原子作为电子阱,用于固氮和活化

用富电子杂原子或缺电子杂原子掺杂主体材料已被用作一种直接且主流的方法,以修饰电子结构并提高各种反应(包括氮还原反应(NRR))的电化学活性。作为第三类掺杂剂,等电杂原子(在这项工作中以碳框架中的Si原子为例)已被设计为NRR的高效活性中心。作为具有不同大小和对碳载体的电负性的同一族元素,等电硅杂原子(Iso-e Si)产生具有孤轨道的局部奇异点,该孤点可以充当预吸附N 2的电子陷阱分子通过库仑相互作用,从而促进了随后的NRR激活过程。因此,Iso-e Si原子作为一种特殊的不含金属的单原子基电催化剂,可将NRR的原始碳载体的法拉第效率提高12倍,从而产生非常高的周转频率值0.52 h -1,与原子分散的过渡金属基电催化剂相当。
更新日期:2020-09-16
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