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
Popularization of lithium-sulfur batteries(LSBs) is still hindered by shuttle effect and volume expansion.Herein, a new modularized sulfur storage strategy is proposed to solve above problems and accomplished via empl...Popularization of lithium-sulfur batteries(LSBs) is still hindered by shuttle effect and volume expansion.Herein, a new modularized sulfur storage strategy is proposed to solve above problems and accomplished via employing 100% space utilization host material of cobalt loaded carbon nanoparticles derived from ZIF-67. The modular dispersed storage of sulfur not only greatly increases the proportion of active sulfur,but also inhibits the occurrence of volume expansion. Meanwhile, 100% space utilization host material can greatly improve the conductivity of the cathode, provide a larger electrolyte wetting interface and effectively suppress the shuttle effect. Moreover, loaded cobalt particles have high catalytic activity for electrochemical reaction and can effectively improve the redox kinetics. The cell with new cathode host material carbonized at 650 ℃(ZIF-67(650 ℃)) exhibits superior rate performance and can maintain a high specific capacity of 950 m Ah/g after 100 cycles at 0.2 C, showing a good cycle stability.展开更多
Lithium-sulfur batteries(LSBs) hold great potential for large-scale electrochemical energy storage applications. Currently, the shuttle of soluble lithium polysulfide(LiPSs) intermediates with sluggish conversion kine...Lithium-sulfur batteries(LSBs) hold great potential for large-scale electrochemical energy storage applications. Currently, the shuttle of soluble lithium polysulfide(LiPSs) intermediates with sluggish conversion kinetics and random deposition of Li2S have severely degraded the capacity, rate and cycling performances of LSBs, preventing their practical applications. In this work, ultrathin MoSe2 nanosheets with active edge sites were successfully grown on both internal and external surfaces of hollow carbon spheres with mesoporous walls(MCHS). The resulting MoSe2@MCHS composite acted as a novel functional reservoir for Li PSs with high chemical affinity and effectively mediated their fast redox conversion during charge/discharge as elucidated by experimental observations and first-principles density functional theory(DFT) calculations. The as-fabricated Li-S cells delivered high capacity, superior rate and excellent cyclability. The current work presents new insights on the delicate design and fabrication of novel functional composite electrode materials for rechargeable batteries with emerging applications.展开更多
Lithium-sulfur(Li-S)batteries have been regarded as the candidate for the next-generation energy storage system due to the high theoretical specific capacity(1675 m Ah/g), energy density(2600 Wh/kg)and the abundance o...Lithium-sulfur(Li-S)batteries have been regarded as the candidate for the next-generation energy storage system due to the high theoretical specific capacity(1675 m Ah/g), energy density(2600 Wh/kg)and the abundance of elemental sulfur, but the application of Li-S batteries is impeded by a series of problems. Recently, all-solid-state Li-S batteries(ASSLSBs) have drawn great attention because many drawbacks such as safety issues caused by metallic lithium anodes and organic liquid electrolytes can be overcome through the use of solid-state electrolytes(SEs). However, not only the problems brought by sulfur cathodes still exist, but more trouble arouses from the interfaces between SEs and cathodes, hampering the practical application of ASSLSBs. Therefore, in order to deal with the problems, enormous endeavors have been done on ASSLSB cathodes during the past few decades, including engineering of cathode active materials, cathode host materials, cathode binder materials and cathode structures. In this review, the electrochemical mechanism and existing problems of ASSLSBs are briefly introduced. Subsequently, the strategies for developing cathode materials and designing cathode structures are presented. Then there follows a brief discussion of SE problems and expectations, and finally, the challenges and perspectives of ASSLSBs are summarized.展开更多
Lithium–sulfur(Li–S)battery is attracting increasing interest for its potential in low-cost high-density energy storage.However,it has been a persistent challenge to simultaneously realize high energy density and lo...Lithium–sulfur(Li–S)battery is attracting increasing interest for its potential in low-cost high-density energy storage.However,it has been a persistent challenge to simultaneously realize high energy density and long cycle life.Herein,we report a synergistic strategy to exploit a unique nitrogen-doped three-dimensional graphene aerogel as both the lithium anode host to ensure homogeneous lithium plating/stripping and mitigate lithium dendrite formation and the sulfur cathode host to facilitate efficient sulfur redox chemistry and combat undesirable polysulfide shuttling effect,realizing Li–S battery simultaneously with ultrahigh energy density and long cycle life.The as-demonstrated polysulfide-based device delivers a high areal capacity of 7.5 mAh/cm^(2)(corresponds to 787 Wh/L)and an ultralow capacity fading of 0.025%per cycle over 1000 cycles at a high current density of 8.6 mA/cm^(2).Our findings suggest a novel strategy to scale up the superior electrochemical property of every microscopic unit to a macroscopic-level performance that enables simultaneously high areal energy density and long cycling stability that are critical for practical Li–S batteries.展开更多
Sodium-ion batteries are promising for large-scale energy storage due to sodium's low cost and infinite abundance. The most popular cathodes for sodium-ion batteries, i.e., the layered sodium-containing oxides, us...Sodium-ion batteries are promising for large-scale energy storage due to sodium's low cost and infinite abundance. The most popular cathodes for sodium-ion batteries, i.e., the layered sodium-containing oxides, usually exhibit reversible host rearrangement between P-type and O-type stacking upon charge/discharge. Herein we demonstrate that such host rearrangement is unfavorable and can be suppressed by introducing transition-metal ions into sodium layers. The electrode with stabilized P3-type stacking delivers superior rate capability, high energy efficiency, and excellent cycling performance. Owing to the cation-mixing nature, it performs the lowest lattice strain among all reported cathodes for sodium-ion batteries. Our findings highlight the significance of a stable host for sodium-ion storage and moreover underline the fundamental distinction in material design strategy between lithium-and sodium-ion batteries.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supported by the National Natural Science Foundation of China (No.52173255)the Opening Project of the Jiangsu Key Laboratory for Chemistry of Low-Dimensional Materials (No.JSKC20021)the Collaborative Innovation Center for Advanced Micro/nanomaterials and Equipment (Co-constructed by Jiangsu Province and Ministry of Education)。
文摘Popularization of lithium-sulfur batteries(LSBs) is still hindered by shuttle effect and volume expansion.Herein, a new modularized sulfur storage strategy is proposed to solve above problems and accomplished via employing 100% space utilization host material of cobalt loaded carbon nanoparticles derived from ZIF-67. The modular dispersed storage of sulfur not only greatly increases the proportion of active sulfur,but also inhibits the occurrence of volume expansion. Meanwhile, 100% space utilization host material can greatly improve the conductivity of the cathode, provide a larger electrolyte wetting interface and effectively suppress the shuttle effect. Moreover, loaded cobalt particles have high catalytic activity for electrochemical reaction and can effectively improve the redox kinetics. The cell with new cathode host material carbonized at 650 ℃(ZIF-67(650 ℃)) exhibits superior rate performance and can maintain a high specific capacity of 950 m Ah/g after 100 cycles at 0.2 C, showing a good cycle stability.
基金financially supported by the National Natural Science Foundation of China (51302204, 21902122)Postdoctoral Science Foundation of China (2019M652723)+2 种基金Hunan Provincial Science and Technology Plan Project (No.2017TP1001)Program for Changjiang Scholars and Innovative Research Team in University (IRT_15R52)Hubei Provincial Department of Education for the “Chutian Scholar” program。
文摘Lithium-sulfur batteries(LSBs) hold great potential for large-scale electrochemical energy storage applications. Currently, the shuttle of soluble lithium polysulfide(LiPSs) intermediates with sluggish conversion kinetics and random deposition of Li2S have severely degraded the capacity, rate and cycling performances of LSBs, preventing their practical applications. In this work, ultrathin MoSe2 nanosheets with active edge sites were successfully grown on both internal and external surfaces of hollow carbon spheres with mesoporous walls(MCHS). The resulting MoSe2@MCHS composite acted as a novel functional reservoir for Li PSs with high chemical affinity and effectively mediated their fast redox conversion during charge/discharge as elucidated by experimental observations and first-principles density functional theory(DFT) calculations. The as-fabricated Li-S cells delivered high capacity, superior rate and excellent cyclability. The current work presents new insights on the delicate design and fabrication of novel functional composite electrode materials for rechargeable batteries with emerging applications.
基金supported by the National Natural Science Foundation of China (Nos. 51874110 and 51604089)Natural Science Foundation of Heilongjiang Province (No. LH2021B011)Open Project of State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology (No. QA202138)。
文摘Lithium-sulfur(Li-S)batteries have been regarded as the candidate for the next-generation energy storage system due to the high theoretical specific capacity(1675 m Ah/g), energy density(2600 Wh/kg)and the abundance of elemental sulfur, but the application of Li-S batteries is impeded by a series of problems. Recently, all-solid-state Li-S batteries(ASSLSBs) have drawn great attention because many drawbacks such as safety issues caused by metallic lithium anodes and organic liquid electrolytes can be overcome through the use of solid-state electrolytes(SEs). However, not only the problems brought by sulfur cathodes still exist, but more trouble arouses from the interfaces between SEs and cathodes, hampering the practical application of ASSLSBs. Therefore, in order to deal with the problems, enormous endeavors have been done on ASSLSB cathodes during the past few decades, including engineering of cathode active materials, cathode host materials, cathode binder materials and cathode structures. In this review, the electrochemical mechanism and existing problems of ASSLSBs are briefly introduced. Subsequently, the strategies for developing cathode materials and designing cathode structures are presented. Then there follows a brief discussion of SE problems and expectations, and finally, the challenges and perspectives of ASSLSBs are summarized.
基金This work was financially supported by Scientific ResearchStart-up Funds of Tsinghua SIGS(Grant NumberQD2021018C to L.P.)the National Natural Science Founda-tion of China(Grant Numbers 20231710015 , 22209096 to L.P.)+2 种基金GuangDong Basic and Applied Basic ResearchFoundation(No.2023A1515010059 to L.P.)ShenzhenFundamental Research Program(No.JCYJ20220530143003008 to L.P.)C.Z.acknowledges the financial supportfrom the National Natural Science Foundation of China(Grant Number 51472031)
文摘Lithium–sulfur(Li–S)battery is attracting increasing interest for its potential in low-cost high-density energy storage.However,it has been a persistent challenge to simultaneously realize high energy density and long cycle life.Herein,we report a synergistic strategy to exploit a unique nitrogen-doped three-dimensional graphene aerogel as both the lithium anode host to ensure homogeneous lithium plating/stripping and mitigate lithium dendrite formation and the sulfur cathode host to facilitate efficient sulfur redox chemistry and combat undesirable polysulfide shuttling effect,realizing Li–S battery simultaneously with ultrahigh energy density and long cycle life.The as-demonstrated polysulfide-based device delivers a high areal capacity of 7.5 mAh/cm^(2)(corresponds to 787 Wh/L)and an ultralow capacity fading of 0.025%per cycle over 1000 cycles at a high current density of 8.6 mA/cm^(2).Our findings suggest a novel strategy to scale up the superior electrochemical property of every microscopic unit to a macroscopic-level performance that enables simultaneously high areal energy density and long cycling stability that are critical for practical Li–S batteries.
基金The financial support from the National Basic Research Program of China(2014CB932300)Natural Science Foundation of Jiangsu Province of China(BK20170630)+1 种基金NSF of China(21633003 and 51602144)sponsored by the JST-CREST ‘‘Phase Interface Science for Highly Efficient Energy Utilization",JST(Japan)
文摘Sodium-ion batteries are promising for large-scale energy storage due to sodium's low cost and infinite abundance. The most popular cathodes for sodium-ion batteries, i.e., the layered sodium-containing oxides, usually exhibit reversible host rearrangement between P-type and O-type stacking upon charge/discharge. Herein we demonstrate that such host rearrangement is unfavorable and can be suppressed by introducing transition-metal ions into sodium layers. The electrode with stabilized P3-type stacking delivers superior rate capability, high energy efficiency, and excellent cycling performance. Owing to the cation-mixing nature, it performs the lowest lattice strain among all reported cathodes for sodium-ion batteries. Our findings highlight the significance of a stable host for sodium-ion storage and moreover underline the fundamental distinction in material design strategy between lithium-and sodium-ion batteries.
