Frameworked electrolytes:Ionic transport behavior and high mobility for solid state batteries  

作　　者：Jianguo Sun Hao Yuan Jing Yang Tuo Wang Yulin Gao Qi Zhao Ximeng Liu Haimei Wang Yong-Wei Zhang John Wang 

机构地区：[1]Department of Materials Science and Engineering,National University of Singapore,Singapore,Singapore [2]Institute of High Performance Computing(IHPC),Agency for Science,Technology and Research(A*STAR),Singapore,Singapore [3]ST Engineering Advanced Material Engineering Pte.Ltd.,Singapore,Singapore [4]National University of Singapore(Chongqing)Research Institute,Chongqing Liang Jiang New Area,Chongqing,the People's Republic of China [5]Institute of Materials Research and Engineering(IMRE),Agency for Science,Technology and Research(A*STAR),Singapore,Singapore

出　　处：《InfoMat》2024年第2期76-89,共14页信息材料（英文）

基　　金：Singapore Ministry of Education,Grant/Award Number:A-8000186-01-00;National Research Foundation(NRF)Singapore,Grant/Award Numbers:CRP NRF-CRP26-2021-0003,NRFCRP24-2020-0002;A*STAR SERC CRF Award。

摘　　要：All solid-state batteries(ASSBs)are the holy grails of rechargeable batteries,where extensive searches are ongoing in the pursuit of ideal solid-state electrolytes.Nevertheless,there is still a long way off to the satisfactorily high(enough)ionic conductivity,long-term stability and especially being able to form compatible interfaces with the solid electrodes.Herein,we have explored ionic transport behavior and high mobility in the sub-nano pore networks in the framework structures.Macroscopically,the frameworked electrolyte behaves as a solid,and however in the(sub)-nano scales,the very limited number of solvent molecules in confinement makes them completely different from that in liquid electrolyte.Differentiated from a liquid-electrolyte counterpart,the interactions between the mobile ions and surrounding molecules are subject to dramatic changes,leading to a high ionic conductivity at room temperature with a low activation energy.Li+ions in the sub-nano cages of the network structure are highly mobile and diffuse rather independently,where the rate-limiting step of ions crossing cages is driven by the local concentration gradient and the electrostatic interactions between Li^(+)ions.This new class of frameworked electrolytes(FEs)with both high ionic conductivity and desirable interface with solid electrodes are demonstrated to work with Li-ion batteries,where the ASSB with LiFePO_(4)shows a highly stable electrochemical performance of over 450 cycles at 2℃ at room temperature,with an almost negligible capacity fade of 0.03‰ each cycle.In addition,the FE shows outstanding flexibility and anti-flammability,which are among the key requirements of large-scale applications.

关 键 词：frameworked electrolyte macroscopically solid with 3D ionic channels in sub-nano-scales solid-state battery space confinement of Li ions 

分 类 号：TM912[电气工程—电力电子与电力传动]