Lithium sulfur(Li-S)batteries with high specific capacity and energy density can bring enormous opportunities for the nextgeneration energy storage systems.However,the severe dissolution and shuttle effect of lithium ...Lithium sulfur(Li-S)batteries with high specific capacity and energy density can bring enormous opportunities for the nextgeneration energy storage systems.However,the severe dissolution and shuttle effect of lithium polysulfides(LiPSs)is still the key issue that seriously impedes the development of practical Li-S batteries.Here,polar Co9S8 inlaid carbon nanoboxes(Co9S8@C NBs)have been investigated as cathode host for high-performance Li-S batteries.In this integrated structure,Co9S8 nanocrystals not only provide strong chemisorptive capability for polar LiPSs,but also act as a catalyst to accelerate polysulfide redox reactions;while carbon nanobox with large inner space can offer enough space to relieve the volume expansion and physically confine LiPSs’dissolution.As a result,the S/Co9S8@C NBs cathode exhibits high specific capacity at 1C and the capacity retention was^83%after 400 cycles,corresponding to an average decay rate of only^0.043%per cycle.展开更多
Lithium-sulfur(Li-S)battery has been considered as one of the most promising next generation energy storage technologies for its overwhelming merits of high theoretical specific capacity(1673 m Ah/g),high energy densi...Lithium-sulfur(Li-S)battery has been considered as one of the most promising next generation energy storage technologies for its overwhelming merits of high theoretical specific capacity(1673 m Ah/g),high energy density(2500 Wh/kg),low cost,and environmentally friendliness of sulfur.However,critical drawbacks,including inherent low conductivity of sulfur and Li2S,large volume changes of sulfur cathodes,undesirable shuttling and sluggish redox kinetics of polysulfides,seriously deteriorate the energy density,cycle life and rate capability of Li-S battery,and thus limit its practical applications.Herein,we reviewed the recent developments addressing these problems through iron-based nanomaterials for effective synergistic immobilization as well as conversion reaction kinetics acceleration for polysulfides.The mechanist configurations between different iron-based nanomaterials and polysulfides for entrapment and conversion acceleration were summarized at first.Then we concluded the recent progresses on utilizing various iron-based nanomaterials in Li-S battery as sulfur hosts,separators and cathode interlayers.Finally,we discussed the challenges and perspectives for designing high sulfur loading cathode architectures along with outstanding chemisorption capability and catalytic activity.展开更多
Nickel-rich LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811) cathode material has been widely concerned due to its high voltage,high specific capacity and excellent rate performance,which is considered as one of the most promi...Nickel-rich LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811) cathode material has been widely concerned due to its high voltage,high specific capacity and excellent rate performance,which is considered as one of the most promising cathode materials for the next generation of high-energy-density solid-state lithium batteries.However,serious electro-chemo-mechanical degradation of Nickel-rich cathode during cycling,especially at a high voltage(over 4.5 V),constrains their large-scale application.Here,using the multiphysical simulation,highly-conductive polymer matrix with spontaneous stress-buffering effect was uncovered theoretically for reinforcing the electrochemical performance of composited NCM81 1 cathode through the visualization of uniform concentration distribution of Li-ion coupled with improved stress field inside NCM811 cathode.Thereupon,polyacrylonitrile(PAN) and soft polyvinylidene fluoride(PVDF) were selected as the polymer matrix to fabricate the composited NCM811 cathode(PVDFPAN@NCM811) for improving the electrochemical performance of the solid-state NMC811|Li full cells,which can maintain high capacity over 146.2 mA h g^(-1)after 200 cycles at a high voltage of 4.5 V.Suggestively,designing a multifunctional polymer matrix with high ionic conductivity and mechanical property can buffer the stress and maintain the integrity of the structure,which can be regarded as the door-opening avenue to realize the high electrochemical performance of Ni-rich cathode for solidstate batteries.展开更多
Despite great progress of lithium-sulfur(Li-S)battery performance at the laboratory-level,both key parameters and challenges at cell scales to achieve practical high energy density require high-sulfur-loading cathodes...Despite great progress of lithium-sulfur(Li-S)battery performance at the laboratory-level,both key parameters and challenges at cell scales to achieve practical high energy density require high-sulfur-loading cathodes and lean electrolytes.Herein,a novel carbon foam integrated by hollow carbon bubble nanoreactors with ultrahigh pore volume of 6.9 cm3·g−1 is meticulously designed for ultrahigh sulfur content up to 96 wt.%.Tailoring polysulfide trapping and ion/electron transport kinetics during the charge-discharge process can be achieved by adjusting the wall thickness of hollow carbon bubbles.And a further in-depth understanding of electrochemical reaction mechanism for the cathode is impelled by the in-situ Raman spectroscopy.As a result,the as-prepared cathode delivers high specific capacitances of 1,269 and 695 mAh·g−1 at 0.1 and 5 C,respectively.Furthermore,Li-S pouch cells with high areal sulfur loading of 6.9 mg·cm−2 yield exceptional practical energy density of 382 Wh·kg−1 under lean electrolyte of 3.5µL·mg−1,which demonstrates the great potential for realistic high-energy Li-S batteries.展开更多
Aqueous zinc-ion batteries,due to their high power density,intrinsic safety,low cost,and environmental benign,have attracted tremendous attentions recently.However,their application is severely plagued by the inferior...Aqueous zinc-ion batteries,due to their high power density,intrinsic safety,low cost,and environmental benign,have attracted tremendous attentions recently.However,their application is severely plagued by the inferior energy density and short cycling life,which was mainly ascribed to zinc dendrites,and interfacial side reactions,narrow potential window induced by water decomposition,all of which are highly related with the Zn^(2+)solvation structures in the aqueous electrolytes.Therefore,in this review,we comprehensively summarized the recent development of strategies of regulating Zn^(2+)solvation structures,specially,the effect of zinc salts,nonaqueous co-solvents,and functional additives on the Zn^(2+)solvation structures and the corresponding electrochemical performance of aqueous zinc-ion batteries.Moreover,future perspectives focused on the challenges and possible solutions for design and commercialization of aqueous electrolytes with unique solvation structures are provided.展开更多
Embracing ultrahigh theoretical capacity of 3860 mA h g^(-1)and the lowest reduction potential of-3.04 V(versus standard hydrogen electrode),lithium(Li) is considered as the "holy grail" material for pursuin...Embracing ultrahigh theoretical capacity of 3860 mA h g^(-1)and the lowest reduction potential of-3.04 V(versus standard hydrogen electrode),lithium(Li) is considered as the "holy grail" material for pursuing higher energy density,of which application has been challenged due to the unstable interface caused by the non-uniform electrodeposition as well as high chemical activity.Operating at higher temperature can be recommended to uniform electrodeposition of Li metal.Nevertheless,the intrinsic side-reaction between Li metal anode and electrolyte is inevitably aggravated and thus fosters the failure of Li metal anode rapidly with uneven electrodeposition.Here,a kind of temperature-tolerated ionic liquid(1-methyl-3-ethylimidazole bis(fluorosulfo nyl)imide/lithium bis(trifluoromethylsulfo nyl)imide,EF/LT)based electrolyte that matrixed with poly(vinylidene fluoride-hexafluoropropylene) was designed to maintain the interfacial stabilization of Li metal due to the weak interfacial reaction and uniform electrodeposition at high temperature of 80℃.It is the matter that the 660-h cycle with lower polarization is achieved with EF/LT-based electrolyte at temperature of 80 ℃ and the full cell embraces outstanding cyclic performance,without capacity fading within 100 cycles.Delighting,a door for practical application of Li metal anode for higher energy density as the carbon neutrality progresses in the blooming human society has been opened gradually.展开更多
S@C-Co-N nanoporous carbon co-doped with cobalt and nitrogen as the cathode of lithium-sulfur battery are prepared. The synthetic route is carried out via the carbonization of metal organic frameworks polyhedron ZIF-6...S@C-Co-N nanoporous carbon co-doped with cobalt and nitrogen as the cathode of lithium-sulfur battery are prepared. The synthetic route is carried out via the carbonization of metal organic frameworks polyhedron ZIF-67, followed by the heat treatment with sulfur. The SEM images suggest that C-Co-N composite maintains almost the same size and polyhedron shape of ZIF-67. The XRD pattern confirms the existence of cobalt element. As cathode for lithium-sulfur battery, the S@C-Co-N composite delivers a reversible capacity of 916.6 mAh?g?1 at the initial cycle and 460.5 mAh?g?1 after 500 cycles at 0.5 C, with a capacity fading of 0.09% per cycle.展开更多
基金The authors acknowledge the financial support from the National Postdoctoral Program for Innovation Talents(No.BX201700103)China Postdoctoral Science Foundation funded project(No.2018M633664).
文摘Lithium sulfur(Li-S)batteries with high specific capacity and energy density can bring enormous opportunities for the nextgeneration energy storage systems.However,the severe dissolution and shuttle effect of lithium polysulfides(LiPSs)is still the key issue that seriously impedes the development of practical Li-S batteries.Here,polar Co9S8 inlaid carbon nanoboxes(Co9S8@C NBs)have been investigated as cathode host for high-performance Li-S batteries.In this integrated structure,Co9S8 nanocrystals not only provide strong chemisorptive capability for polar LiPSs,but also act as a catalyst to accelerate polysulfide redox reactions;while carbon nanobox with large inner space can offer enough space to relieve the volume expansion and physically confine LiPSs’dissolution.As a result,the S/Co9S8@C NBs cathode exhibits high specific capacity at 1C and the capacity retention was^83%after 400 cycles,corresponding to an average decay rate of only^0.043%per cycle.
基金financially supported by National Natural Science Foundation of China(Nos.51702362 and 21875282)Natural Science Foundation of Hunan Province(Nos.2022JJ30663,2022JJ40551)+1 种基金Scientific Research Project of National University of Defense Technology(No.ZK19–27)Significant Independent Research Projects for Young Talents of College of Aerospace Science and Engineering,National University of Defense Technology。
文摘Lithium-sulfur(Li-S)battery has been considered as one of the most promising next generation energy storage technologies for its overwhelming merits of high theoretical specific capacity(1673 m Ah/g),high energy density(2500 Wh/kg),low cost,and environmentally friendliness of sulfur.However,critical drawbacks,including inherent low conductivity of sulfur and Li2S,large volume changes of sulfur cathodes,undesirable shuttling and sluggish redox kinetics of polysulfides,seriously deteriorate the energy density,cycle life and rate capability of Li-S battery,and thus limit its practical applications.Herein,we reviewed the recent developments addressing these problems through iron-based nanomaterials for effective synergistic immobilization as well as conversion reaction kinetics acceleration for polysulfides.The mechanist configurations between different iron-based nanomaterials and polysulfides for entrapment and conversion acceleration were summarized at first.Then we concluded the recent progresses on utilizing various iron-based nanomaterials in Li-S battery as sulfur hosts,separators and cathode interlayers.Finally,we discussed the challenges and perspectives for designing high sulfur loading cathode architectures along with outstanding chemisorption capability and catalytic activity.
基金financially supported by the Natural Science Foundation of Hunan Province(2020JJ5653)the National Natural Science Foundation of China(21875282,22102212)+1 种基金the Ministry of Science and Higher Education of the Russian Federation(07515-2022-1150)the National University of Defense Technology Scientific Research Project(ZK20-44)。
文摘Nickel-rich LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811) cathode material has been widely concerned due to its high voltage,high specific capacity and excellent rate performance,which is considered as one of the most promising cathode materials for the next generation of high-energy-density solid-state lithium batteries.However,serious electro-chemo-mechanical degradation of Nickel-rich cathode during cycling,especially at a high voltage(over 4.5 V),constrains their large-scale application.Here,using the multiphysical simulation,highly-conductive polymer matrix with spontaneous stress-buffering effect was uncovered theoretically for reinforcing the electrochemical performance of composited NCM81 1 cathode through the visualization of uniform concentration distribution of Li-ion coupled with improved stress field inside NCM811 cathode.Thereupon,polyacrylonitrile(PAN) and soft polyvinylidene fluoride(PVDF) were selected as the polymer matrix to fabricate the composited NCM811 cathode(PVDFPAN@NCM811) for improving the electrochemical performance of the solid-state NMC811|Li full cells,which can maintain high capacity over 146.2 mA h g^(-1)after 200 cycles at a high voltage of 4.5 V.Suggestively,designing a multifunctional polymer matrix with high ionic conductivity and mechanical property can buffer the stress and maintain the integrity of the structure,which can be regarded as the door-opening avenue to realize the high electrochemical performance of Ni-rich cathode for solidstate batteries.
基金This work was financially supported by National Natural Science Foundation of China(Grant Nos.51702095,51702362,51722503,and 51621004)Natural Science Foundation of Hunan Province,China(Grant No.2018JJ3041)the scientific research project of National University of Defense Technology(Grant Nos.ZK19-27 and ZK17-03-61).
文摘Despite great progress of lithium-sulfur(Li-S)battery performance at the laboratory-level,both key parameters and challenges at cell scales to achieve practical high energy density require high-sulfur-loading cathodes and lean electrolytes.Herein,a novel carbon foam integrated by hollow carbon bubble nanoreactors with ultrahigh pore volume of 6.9 cm3·g−1 is meticulously designed for ultrahigh sulfur content up to 96 wt.%.Tailoring polysulfide trapping and ion/electron transport kinetics during the charge-discharge process can be achieved by adjusting the wall thickness of hollow carbon bubbles.And a further in-depth understanding of electrochemical reaction mechanism for the cathode is impelled by the in-situ Raman spectroscopy.As a result,the as-prepared cathode delivers high specific capacitances of 1,269 and 695 mAh·g−1 at 0.1 and 5 C,respectively.Furthermore,Li-S pouch cells with high areal sulfur loading of 6.9 mg·cm−2 yield exceptional practical energy density of 382 Wh·kg−1 under lean electrolyte of 3.5µL·mg−1,which demonstrates the great potential for realistic high-energy Li-S batteries.
基金supported by Natural Science Foundation of Hunan Province(2023JJ40662)National Defense Science and Technology Key Laboratory Supporting Project(WDZC20235250508)+1 种基金National Natural Science Foundation(22002186)Seed Fund of National University of Defense Technology.
文摘Aqueous zinc-ion batteries,due to their high power density,intrinsic safety,low cost,and environmental benign,have attracted tremendous attentions recently.However,their application is severely plagued by the inferior energy density and short cycling life,which was mainly ascribed to zinc dendrites,and interfacial side reactions,narrow potential window induced by water decomposition,all of which are highly related with the Zn^(2+)solvation structures in the aqueous electrolytes.Therefore,in this review,we comprehensively summarized the recent development of strategies of regulating Zn^(2+)solvation structures,specially,the effect of zinc salts,nonaqueous co-solvents,and functional additives on the Zn^(2+)solvation structures and the corresponding electrochemical performance of aqueous zinc-ion batteries.Moreover,future perspectives focused on the challenges and possible solutions for design and commercialization of aqueous electrolytes with unique solvation structures are provided.
基金financially supported by the Natural Science Foundation of Hunan Province(2020JJ5653)the National Natural Science Foundation of China(21875282,22102212)+1 种基金the National University of Defense Technology Scientific Research Project(ZK20-44)financial support from the Ministry of Science and Higher Education of the Russian Federation(075-15-2022-1150)。
文摘Embracing ultrahigh theoretical capacity of 3860 mA h g^(-1)and the lowest reduction potential of-3.04 V(versus standard hydrogen electrode),lithium(Li) is considered as the "holy grail" material for pursuing higher energy density,of which application has been challenged due to the unstable interface caused by the non-uniform electrodeposition as well as high chemical activity.Operating at higher temperature can be recommended to uniform electrodeposition of Li metal.Nevertheless,the intrinsic side-reaction between Li metal anode and electrolyte is inevitably aggravated and thus fosters the failure of Li metal anode rapidly with uneven electrodeposition.Here,a kind of temperature-tolerated ionic liquid(1-methyl-3-ethylimidazole bis(fluorosulfo nyl)imide/lithium bis(trifluoromethylsulfo nyl)imide,EF/LT)based electrolyte that matrixed with poly(vinylidene fluoride-hexafluoropropylene) was designed to maintain the interfacial stabilization of Li metal due to the weak interfacial reaction and uniform electrodeposition at high temperature of 80℃.It is the matter that the 660-h cycle with lower polarization is achieved with EF/LT-based electrolyte at temperature of 80 ℃ and the full cell embraces outstanding cyclic performance,without capacity fading within 100 cycles.Delighting,a door for practical application of Li metal anode for higher energy density as the carbon neutrality progresses in the blooming human society has been opened gradually.
文摘S@C-Co-N nanoporous carbon co-doped with cobalt and nitrogen as the cathode of lithium-sulfur battery are prepared. The synthetic route is carried out via the carbonization of metal organic frameworks polyhedron ZIF-67, followed by the heat treatment with sulfur. The SEM images suggest that C-Co-N composite maintains almost the same size and polyhedron shape of ZIF-67. The XRD pattern confirms the existence of cobalt element. As cathode for lithium-sulfur battery, the S@C-Co-N composite delivers a reversible capacity of 916.6 mAh?g?1 at the initial cycle and 460.5 mAh?g?1 after 500 cycles at 0.5 C, with a capacity fading of 0.09% per cycle.
