Revealing interfacial space charge storage of Li^(+)/Na^(+)/K^(+)by operando magnetometry  

原位磁性测试揭示锂/钠/钾离子的界面空间电荷存储

作　　者：Xiangkun Li Jie Su Zhaohui Li Zhiqiang Zhao Fengling Zhang Leqing Zhang Wanneng Ye Qinghao Li Kai Wang Xia Wang Hongsen Li Han Hu Shishen Yan Guo-Xing Miao Qiang Li 李祥琨;宿杰;李召辉;赵志强;张凤玲;张乐清;叶万能;李庆浩;王凯;王霞;李洪森;胡涵;颜世申;苗国兴;李强(College of Physics,University-Industry Joint Center for Ocean Observation and Broadband Communication,State Key Laboratory of Bio-Fibers and Eco-Textiles,Weihai Innovation Research Institute,Qingdao University,Qingdao 266071,China;State Key Laboratory of Heavy Oil Processing,College of Chemical Engineering,China University of Petroleum(East China),Qingdao 266580,China;School of Physics,State Key Laboratory of Crystal Materials,Shandong University,Jinan 250100,China;Department of Electrical and Computer Engineering&Institute for Quantum Computing,University of Waterloo,Ontario N2L 3G1,Canada)

机构地区：[1]College of Physics,University-Industry Joint Center for Ocean Observation and Broadband Communication,State Key Laboratory of Bio-Fibers and Eco-Textiles,Weihai Innovation Research Institute,Qingdao University,Qingdao 266071,China [2]State Key Laboratory of Heavy Oil Processing,College of Chemical Engineering,China University of Petroleum(East China),Qingdao 266580,China [3]School of Physics,State Key Laboratory of Crystal Materials,Shandong University,Jinan 250100,China [4]Department of Electrical and Computer Engineering&Institute for Quantum Computing,University of Waterloo,Ontario N2L 3G1,Canada

出　　处：《Science Bulletin》2022年第11期1145-1153,共9页科学通报（英文版）

基　　金：supported by the National Natural Science Foundation of China(22179066,51804173,and 11674186);the National Science Foundation of Shandong Province(ZR2020MA073);the Science and Technology Board of Qingdao(16-5-1-2jch);Natural Sciences and Engineering Research Council of Canada(NSERC)Discovery grant RGPIN-04178;the Canada First Research Excellence Fund。

摘　　要：Interfacial space charge storage between ionic and electronic conductor is a promising scheme to further improve energy and power density of alkali metal ion batteries(AMIBs).However,the general behavior of space charge storage in AMIBs has been less investigated experimentally,mostly due to the complicated electrochemical behavior and lack of proper characterization techniques.Here,we use operando magnetometry to verify that in FeSe_(2)AMIBs,abundant Li^(+)/Na^(+)/K^(+)(M^(+))can be stored at M_(2)Se phase while electrons accumulate at Fe nanoparticles,forming interfacial space charge layers.Magnetic and dynamics tests further demonstrate that with increasing ionic radius from Li^(+),Na^(+)to K^(+),the reaction kinetics can be hindered,resulting in limited Fe formation and reduced space charge storage capacity.This work lays solid foundation for studying the complex interfacial effect in electrochemical processes and designing advanced energy storage devices with substantial capacity and considerable power density.本文通过先进的实时原位磁性测试成功揭示了碱金属离子电池中的Li^(+)、Na^(+)、K^(+)的界面空间电荷存储机制.磁性测试结果表明,在FeSe_(2)等过渡族金属材料碱金属离子电池体系中,M^(+)(Li^(+)/Na^(+)/K^(+))和自旋极化电子可以分别存储在M2Se和Fe中,即界面空间电荷存储机制.这说明FeSe_(2)碱金属离子电池的储能机制不仅包含嵌入和转化反应,还包括界面空间电荷存储机制.此外,根据Fe/M2Se界面体系中空间电荷存储M^(+)的能力不同,磁学以及动力学测试结果进一步证明了碱金属离子半径是影响空间电荷存储的重要因素.该研究表明磁性测试是研究过渡族金属基材料的储能机制以及电化学过程中复杂界面效应的一种强有力的分析表征手段,为设计具有大存储容量和高功率密度的先进储能装置奠定了坚实的基础.

关 键 词：Operando magnetometry Interfacial space charge storage Alkali metal ions batteries Kinetics FeSe_(2) 

分 类 号：TM912[电气工程—电力电子与电力传动]