An Efficient Multifunctional Soluble Catalyst for Li-O_(2) Batteries  

作　　者：Shuochao Xing Zhengcai Zhang Yaying Dou Minghui Li Jing Wu Zhang Zhang Zhen Zhou 

机构地区：[1]Interdisciplinary Research Center for Sustainable Energy Science and Engineering(IRC4SE2),School of Chemical Engineering,Zhengzhou University,Zhengzhou 450001 [2]Key Laboratory of Advanced Energy Materials Chemistry,Ministry of Education,College of Chemistry,Nankai University,Tianjin 300071

出　　处：《CCS Chemistry》2024年第7期1810-1820,共11页中国化学会会刊（英文）

基　　金：supported by the National Natural Science Foundation of China (NSFC;grant no.22202182).

摘　　要：Aprotic lithium-oxygen(Li-O_(2))batteries have a high theoretical energy density,but they face challenges such as cathode blockage,high charge overpotential,and poor cycling stability.These are caused by sluggish reaction kinetics and severe parasitic reactions.Enhancing the performance of Li-O_(2) batteries necessitates the development of efficient catalysts.These catalysts not only augment both the oxygen reduction reaction(ORR)and the oxygen evolution reaction(OER)but also inhibit undesirable parasitic reactions.In this work,we demonstrated for the first time a multifunctional soluble catalyst of iridium(III)acetylacetonate(Ir(acac)_(3))that could speed up oxygen electrochemistry.Ir(acac)_(3) regulated the ORR pathway and the reactivity of superoxide radical species by forming a reversible intermediate complex(Ir(acac)_(3)-O_(2)^(−)).During charging,Ir(acac)_(3) acted as a redox mediator and aided in Li_(2)O_(2) decomposition by reacting with superoxide intermediates.Moreover,as demonstrated by operando UV-visible spectroscopy,the lower charge potential significantly reduced the generation of highly reactive singlet oxygen(^(1)O_(2))intermediates.As a result,the Ir(acac)_(3)-mediated Li-O_(2) battery showed low overpotential,large capacity,and stable cyclability.This study offers a new approach to achieving efficient Li-O_(2) batteries and provides an opportunity to suppress parasitic reactions.

关 键 词：Li-O_(2)battery soluble catalyst superoxide species ORGANOMETALLICS singlet oxygen 

分 类 号：O64[理学—物理化学]