Rational composite design is highly important for the development of high-performance composite polymer electrolytes(CPEs)for solid-state lithium(Li)metal batteries.In this work,Li closo-borohydride,Li_(2)B_(12)H_(12)...Rational composite design is highly important for the development of high-performance composite polymer electrolytes(CPEs)for solid-state lithium(Li)metal batteries.In this work,Li closo-borohydride,Li_(2)B_(12)H_(12),is introduced to poly(vinylidene fluoride)-Li-bis-(trifluoromethanesulfonyl)imide(PVDF-LiTFSI)with a bound N-methyl pyrrolidone plasticizer to form a novel CPE.This CPE shows superb Li^(+)conduction properties,as evidenced by its conductivity of 1.43×10^(-4) S cm^(-1) and Li^(+)transference number of 0.34 at 25℃.Density functional theory calculations reveal that Li_(2)B_(12)H_(12),which features electron-deficient multicenter bonds,can facilitate the dissociation of LiTFSI and enhance the immobilization of TFSI to improve the Li^(+)conduction properties of the CPE.Moreover,the fabricated CPE exhibits excellent electrochemical,thermal,and mechanical stability.The addition of Li_(2)B_(12)H_(12) can help form a protective layer at the anode/electrolyte interface,thereby preventing unwanted reactions.The above benefits of the fabricated CPE contribute to the high compatibility of the electrode.Symmetric Li cells can be stably cycled at 0.2mA cm^(-2) for over 1200 h,and Li||LiFePO_(4) cells can deliver a reversible specific capacity of 140mAh g^(-1) after 200 cycles at 1C at 25℃ with a capacity retention of 98%.展开更多
基金supported by the National Natural Science Foundation of China(51971146 and 51971147)the Major Program for the Scientific Research Innovation Plan of Shanghai Education Commission(2019-01-07-00-07-E00015)+3 种基金Shanghai Outstanding Academic Leaders PlanGuangxi Key Laboratory of Information Materials(Guilin University of Electronic Technology,201017-K)Shanghai Rising-Star Program(20QA1407100)the General Program of Natural Science Foundation of Shanghai(20ZR1438400).
文摘Rational composite design is highly important for the development of high-performance composite polymer electrolytes(CPEs)for solid-state lithium(Li)metal batteries.In this work,Li closo-borohydride,Li_(2)B_(12)H_(12),is introduced to poly(vinylidene fluoride)-Li-bis-(trifluoromethanesulfonyl)imide(PVDF-LiTFSI)with a bound N-methyl pyrrolidone plasticizer to form a novel CPE.This CPE shows superb Li^(+)conduction properties,as evidenced by its conductivity of 1.43×10^(-4) S cm^(-1) and Li^(+)transference number of 0.34 at 25℃.Density functional theory calculations reveal that Li_(2)B_(12)H_(12),which features electron-deficient multicenter bonds,can facilitate the dissociation of LiTFSI and enhance the immobilization of TFSI to improve the Li^(+)conduction properties of the CPE.Moreover,the fabricated CPE exhibits excellent electrochemical,thermal,and mechanical stability.The addition of Li_(2)B_(12)H_(12) can help form a protective layer at the anode/electrolyte interface,thereby preventing unwanted reactions.The above benefits of the fabricated CPE contribute to the high compatibility of the electrode.Symmetric Li cells can be stably cycled at 0.2mA cm^(-2) for over 1200 h,and Li||LiFePO_(4) cells can deliver a reversible specific capacity of 140mAh g^(-1) after 200 cycles at 1C at 25℃ with a capacity retention of 98%.
