The d-orbital regulation of isolated manganese sites for enhanced oxygen evolution  

作　　者：Xue Bai Jingyi Han Xiaodi Niu Jingqi Guan 

机构地区：[1]Institute of Physical Chemistry,College of Chemistry,Jilin University,2519 Jiefang Road,Changchun 130021,China [2]College of Food Science and Engineering,Jilin University,Changchun 130062,China

出　　处：《Nano Research》2023年第8期10796-10802,共7页纳米研究（英文版）

基　　金：supported by the National Natural Science Foundation of China(No.22075099);the Natural Science Foundation of Jilin Province(No.20220101051JC);the Education Department of Jilin Province(No.JJKH20220967KJ)。

摘　　要：Developing transition metal-nitrogen-carbon materials(M-N-C)as electrocatalysts for the oxygen evolution reaction(OER)is significant for low-cost energy conversion systems.Further d-orbital adjustment of M center in M-N-C is beneficial to the improvement of OER performance.Herein,we synthesize a single-Mn-atom catalyst based on carbon skeleton(Mn_(1)-N_(2)S_(2)C_(x))with isolated Mn-N_(2)S_(2)sites,which exhibits high alkaline OER activity(η10=280 mV),low Tafel slope(44 mV·dec^(−1)),and excellent stability.Theoretical calculations reveal the pivotal function of isolated Mn-N_(2)S_(2)sites in promoting OER,including the adsorption kinetics of intermediates and activation mechanism of active sites.The doping of S causes the increase in both charge density and work function of active Mn center,and ortho-Mn_(1)-N_(2)S_(2)C_(x)expresses the fastest OER kinetics due to the asymmetric plane.

关 键 词：dual-heteroatom coordination Mn1-N_(2)S_(2)C_(x) oxygen evolution reaction(OER) single-atom catalyst theoretical calculation 

分 类 号：O64[理学—物理化学]