Scalable preparation of asymmetrical bilayer sulfide/halide electrolyte membranes for all-solid-state batteries with high voltage  

作　　者：Shenghao JING Yanchen LIU Yang LU Hanzhou LIU Yang LIU Siliang LIU Zongliang ZHANG Fangyang LIU 

机构地区：[1]School of Metallurgy and Environment,Central South University,Changsha,410083,China [2]Engineering Research Centre of Advanced Battery Materials,Ministry of Education,Changsha,410083,China [3]Hunan Provincial Key Laboratory of Nonferrous Value-added Metallurgy,Changsha,410083,China [4]National Energy Metal Resources and New Materials Key Laboratory,Changsha,410083,China [5]Hunan Energy Frontiers New Materials Technology Co.,Ltd.,Changsha,410208,China

出　　处：《Science China(Technological Sciences)》2025年第3期97-109,共13页中国科学(技术科学英文版)

基　　金：financially supported by Hunan Provincial Key R&D Project(Grant No.2023GK2016);the National Key Research and Development Program of China(Grant No.2023YFC2909100);the National Natural Science Foundation of China(Grant Nos.52304376 and 22109084)。

摘　　要：All-solid-state batteries(ASSBs)are considered to be the most promising candidates for improving battery safety and energy density.Sulfide electrolytes have a narrow electrochemical window,which hinders their applications coupled with high-voltage cathodes.Halide electrolytes with high-voltage endurance can help solve this problem.Herein,the combination of spraying and slurry-coating methods was adopted as a practical route to process a free-standing Li_(6)PS_5Cl(LPSCl)asymmetrical electrolyte membrane(19.23Ωcm~2,75μm)decorated with a 10μm Li_(3)In Cl_(6)(LICl)layer.The LICl-LPSCl asymmetrical electrolyte membranes enhanced the high-voltage stabilities to match those of LiNi_(0.83)Co_(0.11)Mn_(0.06)O_(2)(NCM811)and Li_(1.2)Ni_(0.13)Co_(0.13)Mn_(0.54)O_(2)(LRMO)cathodes.The NCM811|LICl-LPSCl|n Si ASSB achieved an initial coulombic efficiency(ICE)of 85.13%and a capacity retention of 77.16%after 200 cycles.Compared with the LPSCl membrane,the LICl-LPSCl membrane displayed high stability with the LRMO cathode as the charging cut-off voltage increased to 4.7 V,which improved the initial charge capacity from 143 to 270 mAh g^(-1)and achieved stable cycling of 160 m Ah g^(-1)at 0.5 C.Additionally,we attempted continuous LICl-LPSCl membrane production and utilized the product to fabricate a pouch-type ASSB based on LRMO.The fabrication of the LICl-LPSCl electrolyte membrane demonstrated its potential for controllable and industryadaptable applications in ASSBs.

关 键 词：all-solid-state batteries halide electrolyte sulfide electrolyte high-voltage asymmetrical 

分 类 号：TM912[电气工程—电力电子与电力传动] TB383.2[一般工业技术—材料科学与工程]