The notorious"shuttle effect"of polysulfide during charge-discharge process induces grievous capacity fading,while the sluggish polysulfide conversion kinetics significantly hinders the development of practi...The notorious"shuttle effect"of polysulfide during charge-discharge process induces grievous capacity fading,while the sluggish polysulfide conversion kinetics significantly hinders the development of practically viable lithium-sulfur(Li-S)batteries.In this study,a novel ZIF-7@carbon composite with ZIF-7 sheets vertically rooted on carbon cloth was developed as multifunctional interlayer to address these issues.The composite shows directional layered structure with outstanding compactness,and thus can provide massive active sites for accelerated redox reactions.The pore channels are perpendicular to the square surface,resulting in extremely high utilization of one-dimensional channels.Therefore,this structure can not only maintain the structural stability during the charge-discharge process by providing enough space for volume expansion,but also contribute to efficient exposure and utilization of active sites for the physical/chemical adsorption and catalytic conversion of polysulfide.As a result,Li-S batteries with the as-developed interlayer deliver a considerable areal capacity of 4.75 mAh cm^(-2) at an elevated sulfur loading of 5.5 mg cm^(-2),and an impressive cyclability with an extremely low capacity-fading rate of merely 0.04%per cycle over 500 cycles at 1 C.展开更多
Lithium-sulfur(Li-S)batteries hold great promises to serve as next-generation energy storage devices because of their high theoretical energy density and environmental benignity.However,the shuttle effect of the solub...Lithium-sulfur(Li-S)batteries hold great promises to serve as next-generation energy storage devices because of their high theoretical energy density and environmental benignity.However,the shuttle effect of the soluble lithium polysulfides(LiPS)and intrinsic insulating nature of sulfur lead to low sulfur utilization and coulombic efficiency,leading to poor cycling performance.The impeded charge transportation and retard LiPS catalytic conversion also endows the Li-S batteries with sluggish redox reaction,leading to unsatisfied rate capability.In this study,Co-based MOF material ZIF-67 is used as the precursor to prepare Co nano-dots decorated three-dimensional graphene aerogel as sulfur immobilizer.This porous architecture establishes a highly conductive interconnected framework for fast charge/mass transportation.The exposed Co nano-dots serve as active sites to strongly trap LiPS,which endows CoNDs@G with low decomposition energy barrier for fast LiPS conversion reaction and promote the completely Li2 S catalytic transformation.Li-S cells based on the Co-NDs@G cathode exhibits excellent cyclability and a high capacity retention rate of 91.1%in 100 cycles.This strategy offers a new direction to design sulfur immobilizer for accelerated LiPS conversion kinetics of Li-S batteries.展开更多
基金the financial support from the Outstanding Young Talents Project of Hebei High Education Institutions(BJ2019013)the Natural Science Foundation of Hebei Province(B2019202289,B2019202199)+1 种基金the National Natural Science Foundation of China(No.21908039)the “Hundred Talents Program”of Hebei Province(E2019050013)。
文摘The notorious"shuttle effect"of polysulfide during charge-discharge process induces grievous capacity fading,while the sluggish polysulfide conversion kinetics significantly hinders the development of practically viable lithium-sulfur(Li-S)batteries.In this study,a novel ZIF-7@carbon composite with ZIF-7 sheets vertically rooted on carbon cloth was developed as multifunctional interlayer to address these issues.The composite shows directional layered structure with outstanding compactness,and thus can provide massive active sites for accelerated redox reactions.The pore channels are perpendicular to the square surface,resulting in extremely high utilization of one-dimensional channels.Therefore,this structure can not only maintain the structural stability during the charge-discharge process by providing enough space for volume expansion,but also contribute to efficient exposure and utilization of active sites for the physical/chemical adsorption and catalytic conversion of polysulfide.As a result,Li-S batteries with the as-developed interlayer deliver a considerable areal capacity of 4.75 mAh cm^(-2) at an elevated sulfur loading of 5.5 mg cm^(-2),and an impressive cyclability with an extremely low capacity-fading rate of merely 0.04%per cycle over 500 cycles at 1 C.
基金the financial support from the Natural Science Foundation of Hebei Province(B2020202069)。
文摘Lithium-sulfur(Li-S)batteries hold great promises to serve as next-generation energy storage devices because of their high theoretical energy density and environmental benignity.However,the shuttle effect of the soluble lithium polysulfides(LiPS)and intrinsic insulating nature of sulfur lead to low sulfur utilization and coulombic efficiency,leading to poor cycling performance.The impeded charge transportation and retard LiPS catalytic conversion also endows the Li-S batteries with sluggish redox reaction,leading to unsatisfied rate capability.In this study,Co-based MOF material ZIF-67 is used as the precursor to prepare Co nano-dots decorated three-dimensional graphene aerogel as sulfur immobilizer.This porous architecture establishes a highly conductive interconnected framework for fast charge/mass transportation.The exposed Co nano-dots serve as active sites to strongly trap LiPS,which endows CoNDs@G with low decomposition energy barrier for fast LiPS conversion reaction and promote the completely Li2 S catalytic transformation.Li-S cells based on the Co-NDs@G cathode exhibits excellent cyclability and a high capacity retention rate of 91.1%in 100 cycles.This strategy offers a new direction to design sulfur immobilizer for accelerated LiPS conversion kinetics of Li-S batteries.