Sulfur-containing polymer(SCP)is considered as an outstanding cathode material for lithium-sulfur batteries.However,undesirable soluble polysulfides may shuttle in electrolyte,concluding long-chain Li_(2)S_(n)(n>4)...Sulfur-containing polymer(SCP)is considered as an outstanding cathode material for lithium-sulfur batteries.However,undesirable soluble polysulfides may shuttle in electrolyte,concluding long-chain Li_(2)S_(n)(n>4)and short-chain Li2Sn(n≤4),as well as the sluggish conversion kinetics are yet to be solved to enhance the performance of lithium-sulfur batteries.Here Se-doped sulfurized polyaniline with adjusted sulfur-chain-S_(x)-(x≤6)contribute to ensure the absence of long-chain polysulfides,and the skeleton with quinoid imine can endow strongly adsorption towards short-chain polysulfides by the reversible transition between deprotonated/protonated imine(-NH^(+)=and-N=),which offer double insurance against suppressing“shuttle effect”.Furthermore,Se atoms are doped into sulfurized polysulfides to accelerate the redox conversion and take a frontier orbital theory-oriented view into catalytic mechanism.Se-doped sulfurized polyaniline as active materials for lithium-organosulfur batteries delivers good electrochemical performance,including high rate,reversible specific capacity(680 mA h g^(-1)at 0.1 A g^(-1)),and lower capacity decay rate only of 0.15%with near 100%coulomb efficiency during long-term cycle.This work provides a valuable guiding ideology and promising solution for the chemistry-oriented structure design and practical application for lithium-organosulfur batteries.展开更多
基金partly supported by the National Natural Science Foundation of China(51763014 and 52073133)the Key Talent Project Foundation of Gansu Province+3 种基金Joint fund between Shenyang National Laboratory for Materials Science and State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals(18LHPY002)the Incubation Program of Excellent Doctoral Dissertation-Lanzhou University of Technologyexcellent doctoral Program of Gansu Province(22JR5RA240)the Program for Hongliu Distinguished Young Scholars in Lanzhou University of Technology。
文摘Sulfur-containing polymer(SCP)is considered as an outstanding cathode material for lithium-sulfur batteries.However,undesirable soluble polysulfides may shuttle in electrolyte,concluding long-chain Li_(2)S_(n)(n>4)and short-chain Li2Sn(n≤4),as well as the sluggish conversion kinetics are yet to be solved to enhance the performance of lithium-sulfur batteries.Here Se-doped sulfurized polyaniline with adjusted sulfur-chain-S_(x)-(x≤6)contribute to ensure the absence of long-chain polysulfides,and the skeleton with quinoid imine can endow strongly adsorption towards short-chain polysulfides by the reversible transition between deprotonated/protonated imine(-NH^(+)=and-N=),which offer double insurance against suppressing“shuttle effect”.Furthermore,Se atoms are doped into sulfurized polysulfides to accelerate the redox conversion and take a frontier orbital theory-oriented view into catalytic mechanism.Se-doped sulfurized polyaniline as active materials for lithium-organosulfur batteries delivers good electrochemical performance,including high rate,reversible specific capacity(680 mA h g^(-1)at 0.1 A g^(-1)),and lower capacity decay rate only of 0.15%with near 100%coulomb efficiency during long-term cycle.This work provides a valuable guiding ideology and promising solution for the chemistry-oriented structure design and practical application for lithium-organosulfur batteries.