Lithium sulfide(Li_(2)S)as a cathode material for lithium-sulfur(Li-S)batteries,one of the most promising advanced batteries in the future,has received tremendous attention in the past decades.However,developing the p...Lithium sulfide(Li_(2)S)as a cathode material for lithium-sulfur(Li-S)batteries,one of the most promising advanced batteries in the future,has received tremendous attention in the past decades.However,developing the practical Li_(2)S cathode confronts challenges of low conductivity for Li-ions and electrons,high sensitivity to environmental moisture,big overpotential barrier to electrochemical activation,and poor cyclability due to the shuttle effect of intermediate species.This article herein reports a simple and effective strategy for making Li_(2)S@Li_(2)S_(2)@Li_(2)S_(6) double-shelled microparticles,which can significantly mitigate these problems.They are synthesized by dissolving Li2S together with S in dimethoxyethane,then drying off the solvent,and finally calcining the collected solid.Compared with pure Li_(2)S,such a double-shell material presents a 26.7% improvement in cycling capacity,0.5 V lower in activation overpotential,and prolonged tolerance in the ambient environment.The density functional theory calculation shows that the performance enhancement lies in the higher stability of Li2S6in contact with moisture and some autocatalytic effect of Li_(2)S_(2)@Li_(2)S_(6).Such a double-shell structure becomes a universal performanceenhancing approach when being combined with other means,such as cathodes composited with catalytic MoS_(2),separators modified with selenium-doped sulfurized-polyacrylonitrile/montmorillonite,electrolytes containing fluorenone additive,and Li anodes coated with a layer of Li_(3)N.The corresponding capacity retention shows up to 80%improvement compared with pure Li_(2)S.展开更多
基金supported by the National Key Research and Development Program of China(2018YFE0111600)the Haihe Laboratory of Sustainable Chemical Transformations(YYJC202104)for financial support。
文摘Lithium sulfide(Li_(2)S)as a cathode material for lithium-sulfur(Li-S)batteries,one of the most promising advanced batteries in the future,has received tremendous attention in the past decades.However,developing the practical Li_(2)S cathode confronts challenges of low conductivity for Li-ions and electrons,high sensitivity to environmental moisture,big overpotential barrier to electrochemical activation,and poor cyclability due to the shuttle effect of intermediate species.This article herein reports a simple and effective strategy for making Li_(2)S@Li_(2)S_(2)@Li_(2)S_(6) double-shelled microparticles,which can significantly mitigate these problems.They are synthesized by dissolving Li2S together with S in dimethoxyethane,then drying off the solvent,and finally calcining the collected solid.Compared with pure Li_(2)S,such a double-shell material presents a 26.7% improvement in cycling capacity,0.5 V lower in activation overpotential,and prolonged tolerance in the ambient environment.The density functional theory calculation shows that the performance enhancement lies in the higher stability of Li2S6in contact with moisture and some autocatalytic effect of Li_(2)S_(2)@Li_(2)S_(6).Such a double-shell structure becomes a universal performanceenhancing approach when being combined with other means,such as cathodes composited with catalytic MoS_(2),separators modified with selenium-doped sulfurized-polyacrylonitrile/montmorillonite,electrolytes containing fluorenone additive,and Li anodes coated with a layer of Li_(3)N.The corresponding capacity retention shows up to 80%improvement compared with pure Li_(2)S.
