Tandem Co–O dual sites on halloysite with promoted reaction kinetics for sulfur reduction  

作　　者：Qiang Zhang Yinyin Qian Ji-Jun Zou Ruijie Gao Huaming Yang 

机构地区：[1]Engineering Research Center of Nano-Geomaterials of Ministry of Education,China University of Geosciences,Wuhan 430074,Hubei,China [2]Hunan Key Laboratory of Mineral Materials and Application,School of Minerals Processing and Bioengineering,Central South University,Changsha 410083,Hunan,China [3]Faculty of Materials Science and Chemistry,China University of Geosciences,Wuhan 430074,Hubei,China [4]Key Laboratory for Green Chemical Technology of the Ministry of Education,School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China [5]Key Laboratory of Functional Geomaterials in China Nonmetallic Minerals Industry,China University of Geosciences,Wuhan 430074,Hubei,China

出　　处：《Journal of Energy Chemistry》2022年第12期486-493,I0013,共9页能源化学（英文版）

基　　金：supported by the National Science Fund for Distinguished Young Scholars(51225403);the National Natural Science Foundation of China(52042403);the National Postdoctoral Program for Innovative Talents(BX2021276);the China Postdoctoral Science Foundation(2020M682519);the Strategic Priority Research Program of Central South University(ZLXD2017005);the“CUG Scholar"Scientific Research Funds at China University of Geosciences(Wuhan)(Project No.20222020110)。

摘　　要：Facilitating sulfur reduction reaction(SRR)is a promising pathway to tackle the polysulfide shuttle effect and enhance the electrochemical performance of lithium-sulfur(Li-S)batteries.Catalysts with a solo active site can reduce a reaction barrier of a certain transition-intermediate,but the linear scaling relationship between multi-intermediates still obstructs overall SRR.Herein,we construct tandem Co–O dual sites with accelerating SRR kinetics by loading highly dispersed cobalt sulfide clusters on halloysite.This catalyst features Co with upshifted d-orbital and O with downshifted p-orbital,which cooperatively adsorb long-chain polysulfide and dissociate an S–S bond,thus achieving both optimal adsorption–desorption strength and reduced conversion energy barrier of multi-intermediates in SRR.The Li-S coin batteries using the electrocatalyst endows a high specific capacity of 1224.3 m Ah g^(-1)at 0.2 C after 200cycles,and enhances cycling stability with a low-capacity decay rate of 0.03%per cycle at 1 C after1000 cycles.Moreover,the strategy of the tandem Co–O dual sites is further verified in a practical Li-S pouch battery that realizes 1014.1 m Ah g^(-1)for 100 cycles,which opens up a novel avenue for designing electrocatalysts to accelerate multi-step reactions.

关 键 词：Sulfur reduction reaction Dual catalytic site ORBIT Li-S battery 

分 类 号：TM912[电气工程—电力电子与电力传动] TQ426[化学工程]