Polyethylene oxide(PEO)-based electrolytes are considered as one of the most promising solid-state elec-trolytes for next-generation lithium batteries with high safety and energy density;however,the draw-backs such as insufficient ion conductance,mechanical strength and electrochemical stability hinder their applications in metallic lithium batteries.To enhance their overall properties,flexible and thin com-posite polymer electrolyte(CPE)membranes with 3D continuous aramid nanofiber(ANF)-Li1.4Al0.4Ti1.6(PO4)3(LATP)nanoparticle hybrid frameworks are facilely prepared by filling PEO-LiTFSI in the 3D nanohybrid scaffolds via a solution infusion way.The construction of the 3D continuous nanohybrid networks can effectively inhibit the PEO crystallization,facilitate the lithium salt dissociation and meanwhile increase the fast-ion transport in the continuous LATP electrolyte phase,and thus greatly improving the ionic conductivity(～3 times that of the pristine one).With the integration of the 3D con-tinuity and flexibility of the 3D ANF networks and the thermostability of the LATP phase,the CPE mem-branes also show a wider electrochemical window(～5.0 V vs.4.3 V),higher tensile strength(～4-10 times that of the pristine one)and thermostability,and better lithium dendrite resistance capability.Furthermore,the CPE-based LiFePO4/Li cells exhibit superior cycling stability(133 mAh/g after 100 cycles at 0.3 C)and rate performance(100 mAh/g at 1 C)than the pristine electrolyte-based cell(79 and 29 mAh/g,respectively).This work offers an important CPE design criteria to achieve comprehensively-upgraded solid-state electrolytes for safe and high-energy metal battery applications.

State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources,School of New Energy,North China Electric Power University,Beijing 102206,China

[1]Lehao Liu;Dongmei Zhang;Tianrong Yang;Weihao Hu;Xianglong Meng;Jinshan Mo;Wenyan Hou;Qianxiao Fan;Kai Liu;Bing Jiang;Lihua Chu;Meicheng Li-.Flexible ion-conducting membranes with 3D continuous nanohybrid networks for high-performance solid-state metallic lithium batteries)[J].能源化学,2022(12):360-368

4Ti1,tinuity

Flexible,conducting,membranes,continuous,nanohybrid,networks,performance,solid,state,metallic,lithium,batteries,Polyethylene,oxide,PEO,electrolytes,considered,one,promising,next,generation,safety,energy,density,however,draw,backs,such,insufficient,conductance,mechanical,strength,electrochemical,hinder,their,applications,To,enhance,overall,properties,flexible,thin,posite,polymer,CPE,aramid,nanofiber,ANF,Li1,4Al0,LATP,nanoparticle,frameworks,facilely,prepared,by,filling,LiTFSI,scaffolds,via,solution,infusion,way,construction,can,effectively,inhibit,crystallization,facilitate,salt,dissociation,meanwhile,increase,fast,transport,phase,thus,greatly,improving,ionic,conductivity,times,that,pristine,With,integration,flexibility,thermostability,also,show,wider,window,higher,tensile,better,dendrite,resistance,capability,Furthermore,LiFePO4,cells,exhibit,superior,cycling,mAh,after,cycles,rate,than,respectively,This,offers,important,design,criteria,achieve,comprehensively,upgraded,battery

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