Sodium-oxygen batteries(Na-O_(2))have attracted extensive attention as promising energy storage systems due to their high energy density and low cost.Redox mediators are often employed to improve Na-O_(2) battery perf...Sodium-oxygen batteries(Na-O_(2))have attracted extensive attention as promising energy storage systems due to their high energy density and low cost.Redox mediators are often employed to improve Na-O_(2) battery performance,however,their effect on the formation mechanism of the oxygen reduction product(NaO_(2))is still unclear.Here,we have investigated the formation mechanism of NaO_(2) during the discharge process in the presence of a redox mediator with the help of atomic/nano-scale in-situ characterization tools used in concert(e.g.atomic force microscope,electrochemical quartz crystal microbalance(EQCM)and laser nano-particle analyzer).As a result,real-time observations on different time scales show that by shuttling electrons to the electrolyte,the redox mediator enables formation of NaO_(2) in the solution-phase instead of within a finite region near the electrode surface.These findings provide new fundamental insights on the understanding of Na-O_(2) batteries and new consequently perspectives on designing high performance metal-O_(2) batteries and other related functions.展开更多
A functional interlayer based on two-dimensional(2D)porous modified vermiculite nanosheets(PVS)was obtained by acid-etching vermiculite nanosheets.The as-obtained 2D porous nanosheets exhibited a high specific surface...A functional interlayer based on two-dimensional(2D)porous modified vermiculite nanosheets(PVS)was obtained by acid-etching vermiculite nanosheets.The as-obtained 2D porous nanosheets exhibited a high specific surface area of 427 m^(2)·g^(-1)and rich surface active sites,which help restrain polysulfides(LiPSs)through good physi-cal and chemical adsorption,while simultaneously accelerating the nucleation and dissolution kinetics of Li_(2)S,effec-tively suppressing the shuttle effect.The assembled lithium-sulfur batteries(LSBs)employing the PVS-based inter-layer delivered a high initial discharge capacity of 1386 mAh·g^(-1)at 0.1C(167.5 mAh·g^(-1)),long-term cycling stabil-ity,and good rate property.展开更多
Developing effective heterostructure strategies to mitigate the shuttling effect and accelerate lithium polysulfide(Li PS)conversion remains a critical challenge in lithium–sulfur(Li–S)batteries.Here,we report the f...Developing effective heterostructure strategies to mitigate the shuttling effect and accelerate lithium polysulfide(Li PS)conversion remains a critical challenge in lithium–sulfur(Li–S)batteries.Here,we report the first carbon–free VO_(2)–VS_(2)heterostructure material synthesized via in situ sulfurization,applied as a modifier on a commercial polypropylene(PP)separator(denoted as VO_(2)–VS_(2)@PP).The as–prepared VO_(2)–VS_(2)nanorods synergistically combine the high absorptivity of VO_(2)with the efficient catalytic properties of VS_(2),simultaneously enhancing Li PS anchoring and promoting its conversion.We systematically investigate the influence of material composition on battery performance,leveraging these functional attributes,Li–S cells incorporating VO_(2)–VS_(2)@PP exhibit exceptional cycle stability(over 500cycles at 1C),impressive rate performance(807 m Ah.g^(–1)at 5C),desirable reversibility(49.9%capacity retention after 300 cycles at 5C)and exceptional pouch cell performance(3.65 m Ah.cm^(–2)after 50 stable cycles at 0.1C).This study underscores the potential of tailored heterostructures in realizing high–performance Li–S batteries,offering new insights for next–generation energy storage solutions.展开更多
Lithium-sulfur batteries(LSBs)are considered as the most promising energy storage technologies owing to their large theoretical energy density(2500Wh/kg)and specific capacity(1675 mAh/g).However,the heavy shuttle effe...Lithium-sulfur batteries(LSBs)are considered as the most promising energy storage technologies owing to their large theoretical energy density(2500Wh/kg)and specific capacity(1675 mAh/g).However,the heavy shuttle effect of polysulfides and the growth of lithium dendrites greatly hinder their further development and commercial application.In this paper,cobalt-molybdenum bimetallic carbides heterostructure(Co_(6)Mo_(6)C_(2)@Co@NC)was successfully prepared through chemical etching procedure of ZIF-67 precursor with sodium molybdate and the subsequent high temperature annealing process.The obtained dodecahedral Co_(6)Mo_(6)C_(2)@Co@NC with hollow and porous structure provides large specific surface area and plentiful active sites,which speeds up the chemisorption and catalytic conversion of polysulfides,thus mitigating the shuttle effect of polysulfides and the generation of lithium dendrites.When applied as the LSBs separator modifier layer,the cell with modified separator present excellent rate capability and durable cycling stability.In particular,the cell with Co_(6)Mo_(6)C_(2)@Co@NC/PP separator can maintain the high capacity of 738 mAh/g at the current density of 2 C and the specific capacity of 782.6 mAh/g after 300 cycles at 0.5 C,with the coulombic efficiency(CE)near to 100%.Moreover,the Co_(6)Mo_(6)C_(2)@Co@NC/PP battery exhibits the impressive capacity of 431 mAh/g in high sulfur loading(4.096 mg/cm^(2))at 0.5 C after 200 cycles.This work paves the way for the development of bimetallic carbides heterostructure multifunctional catalysts for durable Li-S battery applications and reveals the synergistic regulation of polysulfides and lithium dendrites through the optimization of the structure and composition.展开更多
Lithium-sulfur batteries(LSBs)have attracted widespread attention due to their high theoretical energy density.However,the dissolution of long-chain polysulfides into the electrolyte(the“shuttle effect”)leads to rap...Lithium-sulfur batteries(LSBs)have attracted widespread attention due to their high theoretical energy density.However,the dissolution of long-chain polysulfides into the electrolyte(the“shuttle effect”)leads to rapid capacity decay.Therefore,finding suitable materials to mitigate the shuttle effect of polysulfides is crucial for enhancing the electrochemical performance of lithium-sulfur batteries.In this study,LSBs’separator is modified with Ni_(3)V_(2)O_(8)nanoparticles@carboxylated carbon nanotubes(Ni_(3)V_(2)O_(8)@CNTs)composite.There are abundant oxygen vacancies in Ni_(3)V_(2)O_(8)@CNTs composite which plays a synergistic effect on shuttle effect.The Ni_(3)V_(2)O_(8)can tightly anchor soluble polysulfides through oxygen vacancies,while the CNTs not only facilitate the transport of ions and electrons but also weaken the migration of polysulfides,limiting shuttle effect.As a result,the cycling stability of LSBs using Ni_(3)V_(2)O_(8)@CNTs-modified separator has been significantly improved(with a capacity decay rate of only 0.0334%after 1500 cycles at 4.0C).This study proposes a strategy to design modified separator for high-performance LSBs.展开更多
Lithium-sulfur batteries(LSBs)have attracted the attention of more and more researchers due to the advantages of high energy density,environmental friendliness,and low production cost.However,the low electronic conduc...Lithium-sulfur batteries(LSBs)have attracted the attention of more and more researchers due to the advantages of high energy density,environmental friendliness,and low production cost.However,the low electronic conductivity of active material and shuttling effect of lithium polysulfides(LiPSs)limit the commercial development of LSBs.To solve these problems,we design a core-shell composite with nitrogen-doped carbon(NC)and two types of selenides(FeSe_(2)-NC@ZnSe-NC).The FeSe_(2)-NC@ZnSe-NC has a strong adsorption capacity,and can effectively adsorb LiPSs.At the same time,it also effectively alleviates the shuttling effect of LiPSs,and improves the utilization of the active substance during the charge/discharge reaction processes.The mechanism involved in FeSe_(2)-NC@ZnSe-NC is demonstrated by both experiments and density-functional theory(DFT)calculations.The electrochemical test results indicate that LSB with S/FeSe_(2)-NC@ZnSe-NC delivers an initial discharge capacity of 1260 mAh·g^(-1)at 0.2C.And after 500 cycles at 1C,the capacity decay rate per cycle is 0.031%,and the capacity retention rate is 85%.The FeSe_(2)-NC@ZnSe-NC core-shell structure verifies a rational strategy to construct an electrode material for high-performance LSBs.展开更多
Lithium–sulfur(Li–S)batteries are supposed to be one of the most potential next-generation batteries owing to their high theoretical capacity and low cost.Nevertheless,the shuttle effect of firm multi-step two-elect...Lithium–sulfur(Li–S)batteries are supposed to be one of the most potential next-generation batteries owing to their high theoretical capacity and low cost.Nevertheless,the shuttle effect of firm multi-step two-electron reaction between sulfur and lithium in liquid electrolyte makes the capacity much smaller than the theoretical value.Many methods were proposed for inhibiting the shuttle effect of polysulfide,improving corresponding redox kinetics and enhancing the integral performance of Li–S batteries.Here,we will comprehensively and systematically summarize the strategies for inhibiting the shuttle effect from all components of Li–S batteries.First,the electrochemical principles/mechanism and origin of the shuttle effect are described in detail.Moreover,the efficient strategies,including boosting the sulfur conversion rate of sulfur,confining sulfur or lithium polysulfides(LPS)within cathode host,confining LPS in the shield layer,and preventing LPS from contacting the anode,will be discussed to suppress the shuttle effect.Then,recent advances in inhibition of shuttle effect in cathode,electrolyte,separator,and anode with the aforementioned strategies have been summarized to direct the further design of efficient materials for Li–S batteries.Finally,we present prospects for inhibition of the LPS shuttle and potential development directions in Li–S batteries.展开更多
Metal sulfides are a class of promising anode materials for sodium-ion batteries(SIBs)owing to their high theoretical specific capacity.Nevertheless,the reactant products(polysulfides)could dissolve into electrolyte,s...Metal sulfides are a class of promising anode materials for sodium-ion batteries(SIBs)owing to their high theoretical specific capacity.Nevertheless,the reactant products(polysulfides)could dissolve into electrolyte,shuttle across separator,and react with sodium anode,leading to severe capacity loss and safety concerns.Herein,for the first time,gallium(Ga)-based liquid metal(LM)alloy is incorporated with MoS_(2)nanosheets to work as an anode in SIBs.The electron-rich,ultrahigh electrical conductivity,and self-healing properties of LM endow the heterostructured MoS_(2)-LM with highly improved conductivity and electrode integrity.Moreover,LM is demonstrated to have excellent capability for the adsorption of polysulfides(e.g.,Na_(2)S,Na_(2)S_(6),and S_(8))and subsequent catalytic conversion of Na_(2)S.Consequently,the MoS_(2)-LM electrode exhibits superior ion diffusion kinetics and long cycling performance in SIBs and even in lithium/potassium-ion battery(LIB/PIB)systems,far better than those electrodes with conventional binders(polyvinylidene difluoride(PVDF)and sodium carboxymethyl cellulose(CMC)).This work provides a unique material design concept based on Ga-based liquid metal alloy for metal sulfide anodes in rechargeable battery systems and beyond.展开更多
Metal organic frameworks(MOFs)are crystalline materials with three-dimensional porous network structure.They are obtained by self-assembly of coordinate bond with metal ions as the nodes and organic ligands as the con...Metal organic frameworks(MOFs)are crystalline materials with three-dimensional porous network structure.They are obtained by self-assembly of coordinate bond with metal ions as the nodes and organic ligands as the connecting chains.MOFs have attracted extensive attention from researchers over the years due to their clear pore and rich topological structure.As the typical powder materials,a specific separator manufacturing process must be possessed when incorporating MOFs into lithium sulfur batteries separator.This mini review summarized the manufacturing process of MOFs separator for LSBs in recent years,and summed up the effects and mechanisms of separators prepared by various separator-forming processes on the performance of LSBs,the potential for industrialization of different separator manufacturing processes is also mentioned briefly.展开更多
Metal-iodine batteries have attracted widespread attention due to their long cycle life,high energy density,remarkable charging capability and low self-discharge rate.Nevertheless,this development is hampered by the c...Metal-iodine batteries have attracted widespread attention due to their long cycle life,high energy density,remarkable charging capability and low self-discharge rate.Nevertheless,this development is hampered by the challenges of the iodine cathode and metal anode,including the hydrogen evolution reaction(HER),sluggish kinetics,shuttle effect of polyiodine ion at the cathode and dendrite formation,corrosion and passivation at the anode.This review summarizes recent developments in metaliodine batteries,including zinc-iodine batteries,lithiumiodine batteries,sodium-iodine batteries,etc.The challenges in the cathode,anode,electrolyte and separator of metal-iodine batteries are discussed,along with the corresponding design and synthesis strategies and specific methods to improve the electrochemical performance.Selecting appropriate cathode hosts,constructing surface protective layers,adding anode additives,making threedimensional anode designs and employing better electrolytes and functional separators to obstruct the production and shuttling of polyiodine ions are highlighted.Finally,future guidelines and directions for the development of metal-iodine batteries are proposed.展开更多
Lithium-selenium(Li-Se)batteries have attracted increasing attention as one of the next-generation battery systems due to much higher electronic conductivity and comparable volumetric capacity of Se compared to the po...Lithium-selenium(Li-Se)batteries have attracted increasing attention as one of the next-generation battery systems due to much higher electronic conductivity and comparable volumetric capacity of Se compared to the popular sulfur cathode.However,its practical application still faces great challenges,especially the rapid capacity decay triggered by the loss of active Se species.A comprehensive review to uncover the in-depth failure mechanism and provide targeted solutions to promote the stable operation of Li-Se batteries is urgently needed.This review systematically summarizes the strategies in the new perspective,focusing on the optimization of Se utilization in Li-Se batteries by keeping a high Se maintenance in the cathode and accelerating the electrochemical kinetics of lithium polyselenides(LiPSe)conversion.On the basis of stru ctural design and Li_(2)Se active material introduction to accommodate volume expansion,blocking s huttle transport of LiPSe by physical/chemical adsorption,bonding Se with polymers or cathode electrolyte interphase(CEI)construction,and catalytic design to accelerate the conversion of LiPSe,different strategies for improving the utilization of Se have been evaluated and discussed.To address the inevitable loss of Se,prospects on inactive Se reactivation and Li protection are detailedly proposed and analyzed referring to the chemistry and corrosion science.Additionally,the perspectives on the future design and comprehensive parameter evaluations for the optimization of Li-Se batteries are recommended.This review comprehensively explains the causes and solutions of capacity fading and provides potential efforts for lifespan expansion of batteries,shedding light on the future development of Li-Se batteries.展开更多
Iodine is widely used in aqueous zinc batteries(ZBs)due to its abundant resources,low cost,and active redox reactions.In addition to the active material in zinc-iodine batteries,iodine also plays an important role in ...Iodine is widely used in aqueous zinc batteries(ZBs)due to its abundant resources,low cost,and active redox reactions.In addition to the active material in zinc-iodine batteries,iodine also plays an important role in other ZBs,such as regulating the electrochemical behavior of zinc ions,promoting the reaction kinetic and reversibility of other redox pairs,catalytic behaviors related to iodine reactions,coupling with other halogen ions,shuttle behaviors of polyiodides,etc.However,there is currently a lack of comprehensive discussion on these aspects.Here,this review provides a comprehensive overview of the electrochemical behaviors of iodide in the aqueous ZBs.The effect of iodine ions on the Zn^(2+)desolvation behaviors and the interfacial behaviors of Zn anode was summarized.Iodine redox pairs boosting other redox pairs,such as MnO_(2)/Mn^(2+)redox pair and vanadium redox pair to obtain high reversibility and capacity was also discussed.Moreover,the catalytic behaviors related to iodine reactions in aqueous ZBs,synergistic reaction with other halogen ions and suppression of shuttle behaviors for high performance zinc-iodine batteries were systematically analyzed.Finally,future prospects for designing effective iodine electrochemical behaviors with practicability are proposed,which will provide scientific guidance for the practical application of iodine-related aqueous ZBs.展开更多
Aqueous Zn-iodine batteries(ZIBs)face the formidable challenges towards practical implementation,including metal corrosion and rampant dendrite growth on the Zn anode side,and shuttle effect of polyiodide species from...Aqueous Zn-iodine batteries(ZIBs)face the formidable challenges towards practical implementation,including metal corrosion and rampant dendrite growth on the Zn anode side,and shuttle effect of polyiodide species from the cathode side.These challenges lead to poor cycle stability and severe self-discharge.From the fabrication and cost point of view,it is technologically more viable to deploy electrolyte engineering than electrode protection strategies.More importantly,a synchronous method for modulation of both cathode and anode is pivotal,which has been often neglected in prior studies.In this work,cationic poly(allylamine hydrochloride)(Pah^(+))is adopted as a low-cost dual-function electrolyte additive for ZIBs.We elaborate the synchronous effect by Pah^(+)in stabilizing Zn anode and immobilizing polyiodide anions.The fabricated Zn-iodine coin cell with Pah^(+)(ZnI_(2) loading:25 mg cm^(−2))stably cycles 1000 times at 1 C,and a single-layered 3.4 cm^(2) pouch cell(N/P ratio~1.5)with the same mass loading cycles over 300 times with insignificant capacity decay.展开更多
Metal-sulfur electrochemistry represents a promising energy storage technology due to the natural abundance and unparalleled theoretical specific capacity of 1675 mAh g^(-1)of sulfur based on two-electron redox reacti...Metal-sulfur electrochemistry represents a promising energy storage technology due to the natural abundance and unparalleled theoretical specific capacity of 1675 mAh g^(-1)of sulfur based on two-electron redox reaction(S^(0)■S^(2-)).Commercially viable metal-sulfur batteries(MSBs)are hindered by sluggish sulfur conversion kinetics,which reduce the utilization efficiency of sulfur and lead to polysulfide shuttling.Single-atom catalysts(SACs)exhibit specific catalytic activity,a high atomic utilization ratio,and flexible selectivity,and are considered exceptional electrocatalysts for addressing the intractable challenges encountered by the MSBs.This review summarizes the recent progress in SACs for boosting the sulfur electrochemistry in MSBs,focusing on sulfur host materials,modified separators and functional interlayers,and analyzes the in-depth mechanisms of SACs.Moreover,the correlation between the coordination environments and the intrinsic activity of SACs is discussed.Finally,the main challenges and potential research directions of SACs for high-energy-density and long-life MSBs are outlined.This study provides significant guidance for constructing novel SACs that can accelerate the sulfur conversion kinetics in MSBs.展开更多
The practical application of lithium-sulfur(Li-S)batteries is still impeded by the severe shuttle effect of lithium polysulfides(LiPSs)and sluggish reaction kinetics of active sulfur.Designing catalytic carriers with ...The practical application of lithium-sulfur(Li-S)batteries is still impeded by the severe shuttle effect of lithium polysulfides(LiPSs)and sluggish reaction kinetics of active sulfur.Designing catalytic carriers with abundant active sites and strong chemisorption capability for LiPSs,is regarded as effective strategy to address these issues.Herein,Se-doping is introduced into the nitrogen-doped carbon coated CoP composite(Se-CoP@NC)to generate structural defects,which effectively enlarges the lattice spacing of CoP and reduces the conversion reaction energy barriers of LiPSs.Meanwhile,Se-doping sites bridges the interface of CoP and nitrogen-doped carbon,accelerating the charge transfer behavior and conversion reaction kinetics of LiPSs.Benefiting from the structural advantages,the assembled Li-S batteries with S/Se-CoP@NC as cathode exhibit high reversible capacity of 779.6 mAh/g at 0.5 C after 500 cycles,and high specific capacity of 805.9 mAh/g at 2 C.Even under extreme conditions(high sulfur-loading content of 6.9 mg/cm^(2);lean electrolyte dosage of 7μL/mg),the corresponding Li-S batteries also keep high reversible areal capacity of 4.5 mAh/cm^(2) after 100 cycles at 0.1 C.This work will inspire the design of metal compounds-based catalysts from atomic level to facilitate the practicability of Li-S batteries.展开更多
The intrinsic clustering behavior and kinetically sluggish conversion process of lithium polysulfides seriously limit the electrochemical reversibility of sulfur redox reactions in lithium-sulfur(Li-S)batteries.Here,w...The intrinsic clustering behavior and kinetically sluggish conversion process of lithium polysulfides seriously limit the electrochemical reversibility of sulfur redox reactions in lithium-sulfur(Li-S)batteries.Here,we introduce molybdenum pentachloride(MoCl_(5))into the electrolyte which could coordinate with lithium polysulfides and inhibit their intrinsic clustering behavior,subsequently serving as an improved mediator with the bi-functional catalytic effect for Li_(2)S deposition and activation.Moreover,the coordination bonding and accelerated conversion reaction can also greatly suppress the dissolution and shuttling of polysulfides.Consequently,such polysulfide complexes enable the Li-S coin cell to exhibit good longterm cycling stability with a capacity decay of 0.078%per cycle after 400 cycles at 2 C,and excellent rate performance with a discharge capacity of 589 mAh/g at 4 C.An area capacity of 3.94 mAh/cm^(2)is also achieved with a high sulfur loading of 4.5mg/cm^(2)at 0.2 C.Even at-20℃,the modified cell maintains standard discharge plateaus with low overpotential,delivering a high capacity of 741 mAh/g at 0.2 C after 80 cycles.The low-cost and convenient MoCl_(5)additive opens a new avenue for the effective regulation of polysulfides and significant enhancement in sulfur redox conversion.展开更多
The unavoidable dendrite growth and shuttle effect have long been stranglehold challenges limiting the safety and practicality of lithium-sulfur batteries.Herein,we propose a dual-action strategy to address the lithiu...The unavoidable dendrite growth and shuttle effect have long been stranglehold challenges limiting the safety and practicality of lithium-sulfur batteries.Herein,we propose a dual-action strategy to address the lithium dendrite issue in stages by constructing a multifunctional surface-negatively-charged nanodiamond layer with high ductility and robust puncture resistance on polypropylene (PP) separator.The uniformly loaded compact negative layer can not only significantly enhance electron transmission efficiency and promote uniform lithium deposition,but also reduce the formation of dendrite during early deposition stage.Most importantly,under the strong puncture stress encountered during the deterioration of lithium dendrite growth under limiting current,the high ductility and robust puncture resistance(145.88 MPa) of as-obtained nanodiamond layer can effectively prevent short circuits caused by unavoidable lithium dendrite.The Li||Li symmetrical cells assembled with nanodiamond layer modified PP demonstrated a stable cycle of over 1000 h at 2 mA cm^(-2)with a polarization voltage of only 29.3 mV.Additionally,the negative charged layer serves as a physical barrier blocking lithium polysulfide ions,effectively mitigating capacity attenuation.The improved cells achieved a capacity decay of only 0.042%per cycle after 700 cycles at 3 C,demonstrating effective suppression of dendrite growth and capacity attenuation,showing promising prospect.展开更多
Lithium-sulfur batteries(LSBs)have become a favorable contender for next-generation electrochemical energy storage systems due to their outstanding features such as high energy density,low cost,and environmental frien...Lithium-sulfur batteries(LSBs)have become a favorable contender for next-generation electrochemical energy storage systems due to their outstanding features such as high energy density,low cost,and environmental friendliness.However,the commercialization of LSBs is still characterized by critical issues such as low sulfur utilization,short cycle life,and poor rate performance,which need to be resolved.Single-atom catalysts,with their outstanding features such as ultra-high atom utilization rate close to 100%and adjustable coordination configuration,have received extensive attention in the field of lithium-sulfur battery research.In this paper,the preparation and characterization of single-atom catalysts for Li-S batteries are briefly introduced,and the latest research progress of single-atom catalysts for Li-S batteries is reviewed from three aspects:cathode,separator and anode.Finally,the key technical problems and future research directions of single-atom catalysts for lithium-sulfur batteries are also prospected,with a view to promoting the further development of commercialized LSBs.展开更多
Active sulfur dissolution and shuttle effect of lithium polysulfides(LiPSs)are the main obstacles hindering the practical application of lithium-sulfur batteries(LSBs),which is primarily induced by the direct interact...Active sulfur dissolution and shuttle effect of lithium polysulfides(LiPSs)are the main obstacles hindering the practical application of lithium-sulfur batteries(LSBs),which is primarily induced by the direct interaction between sulfur-loading cathode and liquid electrolyte.The introduction of functional interlayer within the separator and cathode is an effective strategy to stabilize the electrode/electrolyte interface reaction and improve the utilization rate of active sulfur.Herein,conductive composite nanofabrics(CCN)with multifunctional groups are employed as the interlayer of sulfur-loading cathode,in which the PMIA/PAN supporting fibers offer robust mechanical strength and high thermostable performance,and gelatin/polypyrrole functional fibers ensure high electrical conductivity and strong chemical interaction for LiPSs.As demonstrated by the experimental data and material characterizations,the presence of CCN interlayer not only blocks the shuttle behavior of LiPSs,but also strengthens the interface stability of both Li anode and sulfur-loading cathode.Interestingly,the assembled LSBs with CCN interlayer can maintain stable capacity of 686 mAh/g after 200 cycles at 0.5 A/g.This work will provide new ideas for the elaborate design of functional in terlayers/se para tors for LSBs and lithium metal batteries.展开更多
Lithium-sulfur batteries(LSBs)are promising energy storage systems due to their low cost and high energy density.However,sluggish reaction kinetics and the“shuttle effect”of lithium polysulfides(LiPSs)from sulfur ca...Lithium-sulfur batteries(LSBs)are promising energy storage systems due to their low cost and high energy density.However,sluggish reaction kinetics and the“shuttle effect”of lithium polysulfides(LiPSs)from sulfur cathode hinder the practical application of LSBs.In this work,a separator loaded with the Eu_(2)O_(3-δ)nanoparticles/carbon nanotube interlayer is designed to immobilize Li PSs and catalyze their conversion reaction.The oxygen-deficient Eu_(2)O_(3-δ)nanoparticles,with abundant catalytic sites,promote Li PSs conversion kinetics even at high current densities.Moreover,the unique 4f electronic structure of Eu_(2)O_(3-δ)effectively mitigates undesired sulfur cathode crossover,significantly enhancing the cycling performance of LSBs.Specifically,a high capacity of 620.7 mAh/g at a rate of 5 C is achieved,maintaining at 545 mAh/g after 300 cycles at 1 C.This work demonstrates the potential application of rare earth catalysts in LSBs,offering new research avenues for promoting dynamic conversion design in electrocatalysts.展开更多
基金financially supported by Soft Science Research Project of Guangdong Province(No.2017B030301013)the Shenzhen Science and Technology Research(Grant No.JCYJ20170818085823773,ZDSYS201707281026184)+1 种基金China Postdoctoral Science Foundation(2019M660317)the National Science Foundation of China(No.U1864213)。
文摘Sodium-oxygen batteries(Na-O_(2))have attracted extensive attention as promising energy storage systems due to their high energy density and low cost.Redox mediators are often employed to improve Na-O_(2) battery performance,however,their effect on the formation mechanism of the oxygen reduction product(NaO_(2))is still unclear.Here,we have investigated the formation mechanism of NaO_(2) during the discharge process in the presence of a redox mediator with the help of atomic/nano-scale in-situ characterization tools used in concert(e.g.atomic force microscope,electrochemical quartz crystal microbalance(EQCM)and laser nano-particle analyzer).As a result,real-time observations on different time scales show that by shuttling electrons to the electrolyte,the redox mediator enables formation of NaO_(2) in the solution-phase instead of within a finite region near the electrode surface.These findings provide new fundamental insights on the understanding of Na-O_(2) batteries and new consequently perspectives on designing high performance metal-O_(2) batteries and other related functions.
文摘A functional interlayer based on two-dimensional(2D)porous modified vermiculite nanosheets(PVS)was obtained by acid-etching vermiculite nanosheets.The as-obtained 2D porous nanosheets exhibited a high specific surface area of 427 m^(2)·g^(-1)and rich surface active sites,which help restrain polysulfides(LiPSs)through good physi-cal and chemical adsorption,while simultaneously accelerating the nucleation and dissolution kinetics of Li_(2)S,effec-tively suppressing the shuttle effect.The assembled lithium-sulfur batteries(LSBs)employing the PVS-based inter-layer delivered a high initial discharge capacity of 1386 mAh·g^(-1)at 0.1C(167.5 mAh·g^(-1)),long-term cycling stabil-ity,and good rate property.
基金financially supported by Jilin province science and technology department(No.20230402059GH)Changchun Science and Technology Bureau(No.23YQ11)+4 种基金Jilin Province Science and Technology Department major science and technology project(Nos.20220301004GX and 20220301005GX)Key Subject Construction of Physical Chemistry of Northeast Normal University(No.2412022XK004)the National Natural Science Foundation of China(No.22102020)the Swedish Foundation for International Cooperation in Research and Higher Education(No.KO2017-7351)Swedish Energy Agency(No.P2020-90216)。
文摘Developing effective heterostructure strategies to mitigate the shuttling effect and accelerate lithium polysulfide(Li PS)conversion remains a critical challenge in lithium–sulfur(Li–S)batteries.Here,we report the first carbon–free VO_(2)–VS_(2)heterostructure material synthesized via in situ sulfurization,applied as a modifier on a commercial polypropylene(PP)separator(denoted as VO_(2)–VS_(2)@PP).The as–prepared VO_(2)–VS_(2)nanorods synergistically combine the high absorptivity of VO_(2)with the efficient catalytic properties of VS_(2),simultaneously enhancing Li PS anchoring and promoting its conversion.We systematically investigate the influence of material composition on battery performance,leveraging these functional attributes,Li–S cells incorporating VO_(2)–VS_(2)@PP exhibit exceptional cycle stability(over 500cycles at 1C),impressive rate performance(807 m Ah.g^(–1)at 5C),desirable reversibility(49.9%capacity retention after 300 cycles at 5C)and exceptional pouch cell performance(3.65 m Ah.cm^(–2)after 50 stable cycles at 0.1C).This study underscores the potential of tailored heterostructures in realizing high–performance Li–S batteries,offering new insights for next–generation energy storage solutions.
基金supported by National Natural Science Foundation of China(Nos.52472194,52101243)Natural Science Foundation of Guangdong Province,China(No.2023A1515012619)the Science and Technology Planning Project of Guangzhou(No.202201010565).
文摘Lithium-sulfur batteries(LSBs)are considered as the most promising energy storage technologies owing to their large theoretical energy density(2500Wh/kg)and specific capacity(1675 mAh/g).However,the heavy shuttle effect of polysulfides and the growth of lithium dendrites greatly hinder their further development and commercial application.In this paper,cobalt-molybdenum bimetallic carbides heterostructure(Co_(6)Mo_(6)C_(2)@Co@NC)was successfully prepared through chemical etching procedure of ZIF-67 precursor with sodium molybdate and the subsequent high temperature annealing process.The obtained dodecahedral Co_(6)Mo_(6)C_(2)@Co@NC with hollow and porous structure provides large specific surface area and plentiful active sites,which speeds up the chemisorption and catalytic conversion of polysulfides,thus mitigating the shuttle effect of polysulfides and the generation of lithium dendrites.When applied as the LSBs separator modifier layer,the cell with modified separator present excellent rate capability and durable cycling stability.In particular,the cell with Co_(6)Mo_(6)C_(2)@Co@NC/PP separator can maintain the high capacity of 738 mAh/g at the current density of 2 C and the specific capacity of 782.6 mAh/g after 300 cycles at 0.5 C,with the coulombic efficiency(CE)near to 100%.Moreover,the Co_(6)Mo_(6)C_(2)@Co@NC/PP battery exhibits the impressive capacity of 431 mAh/g in high sulfur loading(4.096 mg/cm^(2))at 0.5 C after 200 cycles.This work paves the way for the development of bimetallic carbides heterostructure multifunctional catalysts for durable Li-S battery applications and reveals the synergistic regulation of polysulfides and lithium dendrites through the optimization of the structure and composition.
基金supported by the Key Research and Development Projects of Anhui Province(No.202304a05020031).
文摘Lithium-sulfur batteries(LSBs)have attracted widespread attention due to their high theoretical energy density.However,the dissolution of long-chain polysulfides into the electrolyte(the“shuttle effect”)leads to rapid capacity decay.Therefore,finding suitable materials to mitigate the shuttle effect of polysulfides is crucial for enhancing the electrochemical performance of lithium-sulfur batteries.In this study,LSBs’separator is modified with Ni_(3)V_(2)O_(8)nanoparticles@carboxylated carbon nanotubes(Ni_(3)V_(2)O_(8)@CNTs)composite.There are abundant oxygen vacancies in Ni_(3)V_(2)O_(8)@CNTs composite which plays a synergistic effect on shuttle effect.The Ni_(3)V_(2)O_(8)can tightly anchor soluble polysulfides through oxygen vacancies,while the CNTs not only facilitate the transport of ions and electrons but also weaken the migration of polysulfides,limiting shuttle effect.As a result,the cycling stability of LSBs using Ni_(3)V_(2)O_(8)@CNTs-modified separator has been significantly improved(with a capacity decay rate of only 0.0334%after 1500 cycles at 4.0C).This study proposes a strategy to design modified separator for high-performance LSBs.
基金financially supported by the National Natural Science Foundation of China(No.52130101)the Project of Science and Technology Development Plan of Jilin Province in China(Nos.20210402058GH and 20220201114GX)。
文摘Lithium-sulfur batteries(LSBs)have attracted the attention of more and more researchers due to the advantages of high energy density,environmental friendliness,and low production cost.However,the low electronic conductivity of active material and shuttling effect of lithium polysulfides(LiPSs)limit the commercial development of LSBs.To solve these problems,we design a core-shell composite with nitrogen-doped carbon(NC)and two types of selenides(FeSe_(2)-NC@ZnSe-NC).The FeSe_(2)-NC@ZnSe-NC has a strong adsorption capacity,and can effectively adsorb LiPSs.At the same time,it also effectively alleviates the shuttling effect of LiPSs,and improves the utilization of the active substance during the charge/discharge reaction processes.The mechanism involved in FeSe_(2)-NC@ZnSe-NC is demonstrated by both experiments and density-functional theory(DFT)calculations.The electrochemical test results indicate that LSB with S/FeSe_(2)-NC@ZnSe-NC delivers an initial discharge capacity of 1260 mAh·g^(-1)at 0.2C.And after 500 cycles at 1C,the capacity decay rate per cycle is 0.031%,and the capacity retention rate is 85%.The FeSe_(2)-NC@ZnSe-NC core-shell structure verifies a rational strategy to construct an electrode material for high-performance LSBs.
基金support from the “Joint International Laboratory on Environmental and Energy Frontier Materials”“Innovation Research Team of High-Level Local Universities in Shanghai”support from the National Natural Science Foundation of China (22209103)
文摘Lithium–sulfur(Li–S)batteries are supposed to be one of the most potential next-generation batteries owing to their high theoretical capacity and low cost.Nevertheless,the shuttle effect of firm multi-step two-electron reaction between sulfur and lithium in liquid electrolyte makes the capacity much smaller than the theoretical value.Many methods were proposed for inhibiting the shuttle effect of polysulfide,improving corresponding redox kinetics and enhancing the integral performance of Li–S batteries.Here,we will comprehensively and systematically summarize the strategies for inhibiting the shuttle effect from all components of Li–S batteries.First,the electrochemical principles/mechanism and origin of the shuttle effect are described in detail.Moreover,the efficient strategies,including boosting the sulfur conversion rate of sulfur,confining sulfur or lithium polysulfides(LPS)within cathode host,confining LPS in the shield layer,and preventing LPS from contacting the anode,will be discussed to suppress the shuttle effect.Then,recent advances in inhibition of shuttle effect in cathode,electrolyte,separator,and anode with the aforementioned strategies have been summarized to direct the further design of efficient materials for Li–S batteries.Finally,we present prospects for inhibition of the LPS shuttle and potential development directions in Li–S batteries.
基金the financial support from the Australian Research Council (ARC) through Future Fellowship (FT210100298)DECRA Fellowship (DE230101068)+2 种基金Discovery Project (DP230100198 and DP210102215)Linkage Projects (LP220100088 and LP180100722)partially supported by AIIM FOR GOLD Grant (2017, 2018)
文摘Metal sulfides are a class of promising anode materials for sodium-ion batteries(SIBs)owing to their high theoretical specific capacity.Nevertheless,the reactant products(polysulfides)could dissolve into electrolyte,shuttle across separator,and react with sodium anode,leading to severe capacity loss and safety concerns.Herein,for the first time,gallium(Ga)-based liquid metal(LM)alloy is incorporated with MoS_(2)nanosheets to work as an anode in SIBs.The electron-rich,ultrahigh electrical conductivity,and self-healing properties of LM endow the heterostructured MoS_(2)-LM with highly improved conductivity and electrode integrity.Moreover,LM is demonstrated to have excellent capability for the adsorption of polysulfides(e.g.,Na_(2)S,Na_(2)S_(6),and S_(8))and subsequent catalytic conversion of Na_(2)S.Consequently,the MoS_(2)-LM electrode exhibits superior ion diffusion kinetics and long cycling performance in SIBs and even in lithium/potassium-ion battery(LIB/PIB)systems,far better than those electrodes with conventional binders(polyvinylidene difluoride(PVDF)and sodium carboxymethyl cellulose(CMC)).This work provides a unique material design concept based on Ga-based liquid metal alloy for metal sulfide anodes in rechargeable battery systems and beyond.
基金financially supported by the University Natural Science Research Key Project of Anhui Province(Nos.KJ2021A1091,2023AH051619)Innovation and Entrepreneurship Training Program for College Students(No.202310377030)Scientific Research Start Foundation Project of Chuzhou University(No.2022qd011)。
文摘Metal organic frameworks(MOFs)are crystalline materials with three-dimensional porous network structure.They are obtained by self-assembly of coordinate bond with metal ions as the nodes and organic ligands as the connecting chains.MOFs have attracted extensive attention from researchers over the years due to their clear pore and rich topological structure.As the typical powder materials,a specific separator manufacturing process must be possessed when incorporating MOFs into lithium sulfur batteries separator.This mini review summarized the manufacturing process of MOFs separator for LSBs in recent years,and summed up the effects and mechanisms of separators prepared by various separator-forming processes on the performance of LSBs,the potential for industrialization of different separator manufacturing processes is also mentioned briefly.
基金supported by the National Natural Science Foundation of China(No.52371240)the Natural Science Foundation of Jiangsu Province(No.BK20230556)+2 种基金China Postdoctoral Science Foundation(No.2022M722686)Jiangsu Funding Program for Excellent Postdoctoral Talent(No.2023ZB701)The Big Data Computing Center of Southeast University.
文摘Metal-iodine batteries have attracted widespread attention due to their long cycle life,high energy density,remarkable charging capability and low self-discharge rate.Nevertheless,this development is hampered by the challenges of the iodine cathode and metal anode,including the hydrogen evolution reaction(HER),sluggish kinetics,shuttle effect of polyiodine ion at the cathode and dendrite formation,corrosion and passivation at the anode.This review summarizes recent developments in metaliodine batteries,including zinc-iodine batteries,lithiumiodine batteries,sodium-iodine batteries,etc.The challenges in the cathode,anode,electrolyte and separator of metal-iodine batteries are discussed,along with the corresponding design and synthesis strategies and specific methods to improve the electrochemical performance.Selecting appropriate cathode hosts,constructing surface protective layers,adding anode additives,making threedimensional anode designs and employing better electrolytes and functional separators to obstruct the production and shuttling of polyiodine ions are highlighted.Finally,future guidelines and directions for the development of metal-iodine batteries are proposed.
基金supported by the China Scholarship Council(No.201809370046)a scholarship from the Laboratory of Inorganic Materials Chemistry,Universitéde Namur+5 种基金the National Key R&D Program of China(2016YFA0202602)the National Natural Science Foundation of China(No.U1663225,22293020,22293022 and 52103342)the Program of Introducing Talents of Discipline to Universities-Plan 111(Grant No.B20002)from the Ministry of Science and Technologythe Program for Changjiang Scholars and Innovative Research Team in University(IRT_15R52)of the Chinese Ministry of EducationBelgium-China Governmental Key Cooperation Program WBI-MOST(SUB/2021/IND493971/524448)the“Plan of relance”Wallonia Government(2310153-Bat Factory)。
文摘Lithium-selenium(Li-Se)batteries have attracted increasing attention as one of the next-generation battery systems due to much higher electronic conductivity and comparable volumetric capacity of Se compared to the popular sulfur cathode.However,its practical application still faces great challenges,especially the rapid capacity decay triggered by the loss of active Se species.A comprehensive review to uncover the in-depth failure mechanism and provide targeted solutions to promote the stable operation of Li-Se batteries is urgently needed.This review systematically summarizes the strategies in the new perspective,focusing on the optimization of Se utilization in Li-Se batteries by keeping a high Se maintenance in the cathode and accelerating the electrochemical kinetics of lithium polyselenides(LiPSe)conversion.On the basis of stru ctural design and Li_(2)Se active material introduction to accommodate volume expansion,blocking s huttle transport of LiPSe by physical/chemical adsorption,bonding Se with polymers or cathode electrolyte interphase(CEI)construction,and catalytic design to accelerate the conversion of LiPSe,different strategies for improving the utilization of Se have been evaluated and discussed.To address the inevitable loss of Se,prospects on inactive Se reactivation and Li protection are detailedly proposed and analyzed referring to the chemistry and corrosion science.Additionally,the perspectives on the future design and comprehensive parameter evaluations for the optimization of Li-Se batteries are recommended.This review comprehensively explains the causes and solutions of capacity fading and provides potential efforts for lifespan expansion of batteries,shedding light on the future development of Li-Se batteries.
基金supported by the Natural Science Foundation of Xinjiang Uygur Autonomous Region(Grant No.2023D01C168)Scientific Research Program of the Higher Education Institution of Xinjiang(Grant No.XJEDU2022P001)+1 种基金Autonomous Region"Tianchi Talent"Introduction Program Youth Doctoral Program(Grant No.51052401544)Tianshan Innovation Team Program of Xinjiang Uygur Autonomous Region(Grant No.2023D14001).
文摘Iodine is widely used in aqueous zinc batteries(ZBs)due to its abundant resources,low cost,and active redox reactions.In addition to the active material in zinc-iodine batteries,iodine also plays an important role in other ZBs,such as regulating the electrochemical behavior of zinc ions,promoting the reaction kinetic and reversibility of other redox pairs,catalytic behaviors related to iodine reactions,coupling with other halogen ions,shuttle behaviors of polyiodides,etc.However,there is currently a lack of comprehensive discussion on these aspects.Here,this review provides a comprehensive overview of the electrochemical behaviors of iodide in the aqueous ZBs.The effect of iodine ions on the Zn^(2+)desolvation behaviors and the interfacial behaviors of Zn anode was summarized.Iodine redox pairs boosting other redox pairs,such as MnO_(2)/Mn^(2+)redox pair and vanadium redox pair to obtain high reversibility and capacity was also discussed.Moreover,the catalytic behaviors related to iodine reactions in aqueous ZBs,synergistic reaction with other halogen ions and suppression of shuttle behaviors for high performance zinc-iodine batteries were systematically analyzed.Finally,future prospects for designing effective iodine electrochemical behaviors with practicability are proposed,which will provide scientific guidance for the practical application of iodine-related aqueous ZBs.
基金supported by the financial support from the National Research Foundation,Singapore,under its Singapore-China Joint Flagship Project(Clean Energy).
文摘Aqueous Zn-iodine batteries(ZIBs)face the formidable challenges towards practical implementation,including metal corrosion and rampant dendrite growth on the Zn anode side,and shuttle effect of polyiodide species from the cathode side.These challenges lead to poor cycle stability and severe self-discharge.From the fabrication and cost point of view,it is technologically more viable to deploy electrolyte engineering than electrode protection strategies.More importantly,a synchronous method for modulation of both cathode and anode is pivotal,which has been often neglected in prior studies.In this work,cationic poly(allylamine hydrochloride)(Pah^(+))is adopted as a low-cost dual-function electrolyte additive for ZIBs.We elaborate the synchronous effect by Pah^(+)in stabilizing Zn anode and immobilizing polyiodide anions.The fabricated Zn-iodine coin cell with Pah^(+)(ZnI_(2) loading:25 mg cm^(−2))stably cycles 1000 times at 1 C,and a single-layered 3.4 cm^(2) pouch cell(N/P ratio~1.5)with the same mass loading cycles over 300 times with insignificant capacity decay.
基金financial support from the National Natural Science Foundation of China(No.22379001 and 22309003)the Natural Science Research Project of Anhui Province Education department(No.2022AH030046)the Top Young Talents of Anhui University of Technology,the Young Scholars of the Introduction and Education of Talents in Anhui Province,and the Scientific Research Foundation of Anhui University of Technology for Talent Introduction。
文摘Metal-sulfur electrochemistry represents a promising energy storage technology due to the natural abundance and unparalleled theoretical specific capacity of 1675 mAh g^(-1)of sulfur based on two-electron redox reaction(S^(0)■S^(2-)).Commercially viable metal-sulfur batteries(MSBs)are hindered by sluggish sulfur conversion kinetics,which reduce the utilization efficiency of sulfur and lead to polysulfide shuttling.Single-atom catalysts(SACs)exhibit specific catalytic activity,a high atomic utilization ratio,and flexible selectivity,and are considered exceptional electrocatalysts for addressing the intractable challenges encountered by the MSBs.This review summarizes the recent progress in SACs for boosting the sulfur electrochemistry in MSBs,focusing on sulfur host materials,modified separators and functional interlayers,and analyzes the in-depth mechanisms of SACs.Moreover,the correlation between the coordination environments and the intrinsic activity of SACs is discussed.Finally,the main challenges and potential research directions of SACs for high-energy-density and long-life MSBs are outlined.This study provides significant guidance for constructing novel SACs that can accelerate the sulfur conversion kinetics in MSBs.
基金the financial support from the National Natural Science Foundation of China(No.52101250)the S&T program of Hebei(Nos.215A4401D and 225A4404D)+5 种基金the Collaborative Innovation Center of Marine Science and Technology of Hainan University(No.XTCX2022HYC14)the Fundamental Research Funds for the Hebei University(No.2021YWF11)the Science Research Project of Hebei Education Department(No.QN2024087)the Xingtai City Natural Science Foundation(No.2023ZZ027)the Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),College of Chemistry,Nankai Universitypartially supported by the Pico Election Microscopy Center of Hainan University。
文摘The practical application of lithium-sulfur(Li-S)batteries is still impeded by the severe shuttle effect of lithium polysulfides(LiPSs)and sluggish reaction kinetics of active sulfur.Designing catalytic carriers with abundant active sites and strong chemisorption capability for LiPSs,is regarded as effective strategy to address these issues.Herein,Se-doping is introduced into the nitrogen-doped carbon coated CoP composite(Se-CoP@NC)to generate structural defects,which effectively enlarges the lattice spacing of CoP and reduces the conversion reaction energy barriers of LiPSs.Meanwhile,Se-doping sites bridges the interface of CoP and nitrogen-doped carbon,accelerating the charge transfer behavior and conversion reaction kinetics of LiPSs.Benefiting from the structural advantages,the assembled Li-S batteries with S/Se-CoP@NC as cathode exhibit high reversible capacity of 779.6 mAh/g at 0.5 C after 500 cycles,and high specific capacity of 805.9 mAh/g at 2 C.Even under extreme conditions(high sulfur-loading content of 6.9 mg/cm^(2);lean electrolyte dosage of 7μL/mg),the corresponding Li-S batteries also keep high reversible areal capacity of 4.5 mAh/cm^(2) after 100 cycles at 0.1 C.This work will inspire the design of metal compounds-based catalysts from atomic level to facilitate the practicability of Li-S batteries.
基金the National Natural Science Foundation of China(Nos.51904344,52172264)the Natural Science Foundation of Hunan Province of China(Nos.2021JJ10060 and 2022GK2033).
文摘The intrinsic clustering behavior and kinetically sluggish conversion process of lithium polysulfides seriously limit the electrochemical reversibility of sulfur redox reactions in lithium-sulfur(Li-S)batteries.Here,we introduce molybdenum pentachloride(MoCl_(5))into the electrolyte which could coordinate with lithium polysulfides and inhibit their intrinsic clustering behavior,subsequently serving as an improved mediator with the bi-functional catalytic effect for Li_(2)S deposition and activation.Moreover,the coordination bonding and accelerated conversion reaction can also greatly suppress the dissolution and shuttling of polysulfides.Consequently,such polysulfide complexes enable the Li-S coin cell to exhibit good longterm cycling stability with a capacity decay of 0.078%per cycle after 400 cycles at 2 C,and excellent rate performance with a discharge capacity of 589 mAh/g at 4 C.An area capacity of 3.94 mAh/cm^(2)is also achieved with a high sulfur loading of 4.5mg/cm^(2)at 0.2 C.Even at-20℃,the modified cell maintains standard discharge plateaus with low overpotential,delivering a high capacity of 741 mAh/g at 0.2 C after 80 cycles.The low-cost and convenient MoCl_(5)additive opens a new avenue for the effective regulation of polysulfides and significant enhancement in sulfur redox conversion.
基金National Natural Science Foundation of China (Grant 52372083, 52173255)Opening Project of the Jiangsu Key Laboratory for Chemistry of Low-Dimensional Materials (JSKC24025)+1 种基金Special Funds for the Trans-formation of Scientific and Technological Achievements in Jiangsu Province(BA2023003)Collaborative Innovation Center for Advanced Micro/nanomaterials and Equipment (Co-constructed by Jiangsu Province and Ministry of Education)。
文摘The unavoidable dendrite growth and shuttle effect have long been stranglehold challenges limiting the safety and practicality of lithium-sulfur batteries.Herein,we propose a dual-action strategy to address the lithium dendrite issue in stages by constructing a multifunctional surface-negatively-charged nanodiamond layer with high ductility and robust puncture resistance on polypropylene (PP) separator.The uniformly loaded compact negative layer can not only significantly enhance electron transmission efficiency and promote uniform lithium deposition,but also reduce the formation of dendrite during early deposition stage.Most importantly,under the strong puncture stress encountered during the deterioration of lithium dendrite growth under limiting current,the high ductility and robust puncture resistance(145.88 MPa) of as-obtained nanodiamond layer can effectively prevent short circuits caused by unavoidable lithium dendrite.The Li||Li symmetrical cells assembled with nanodiamond layer modified PP demonstrated a stable cycle of over 1000 h at 2 mA cm^(-2)with a polarization voltage of only 29.3 mV.Additionally,the negative charged layer serves as a physical barrier blocking lithium polysulfide ions,effectively mitigating capacity attenuation.The improved cells achieved a capacity decay of only 0.042%per cycle after 700 cycles at 3 C,demonstrating effective suppression of dendrite growth and capacity attenuation,showing promising prospect.
基金supported by the Shenzhen Key Basic Research Project:Ionic Liquid-Assisted Synthesis of Single Catalyst and Its Applications in Lithium Sulfur Batteries(GXWD20220817125846003)Major Instrument Project of National Natural Science Foundation of China(62127807)Shenzhen Sustainable Development Special Project(KCXFZ20201221173000001).
文摘Lithium-sulfur batteries(LSBs)have become a favorable contender for next-generation electrochemical energy storage systems due to their outstanding features such as high energy density,low cost,and environmental friendliness.However,the commercialization of LSBs is still characterized by critical issues such as low sulfur utilization,short cycle life,and poor rate performance,which need to be resolved.Single-atom catalysts,with their outstanding features such as ultra-high atom utilization rate close to 100%and adjustable coordination configuration,have received extensive attention in the field of lithium-sulfur battery research.In this paper,the preparation and characterization of single-atom catalysts for Li-S batteries are briefly introduced,and the latest research progress of single-atom catalysts for Li-S batteries is reviewed from three aspects:cathode,separator and anode.Finally,the key technical problems and future research directions of single-atom catalysts for lithium-sulfur batteries are also prospected,with a view to promoting the further development of commercialized LSBs.
基金supported by National Natural Science Foundation of China(No.22309029)Guangdong Basic and Applied Basic Research Foundation(No.2021A1515110089)+2 种基金Dongguan Social Development Technology Foundation(No.20231800907933)Collaborative Innovation Center of Marine Science and Technology of Hainan University(No.XTCX2022HYC14)Start-up Research Foundation of Hainan University(No.KYQD(ZR)-23069)。
文摘Active sulfur dissolution and shuttle effect of lithium polysulfides(LiPSs)are the main obstacles hindering the practical application of lithium-sulfur batteries(LSBs),which is primarily induced by the direct interaction between sulfur-loading cathode and liquid electrolyte.The introduction of functional interlayer within the separator and cathode is an effective strategy to stabilize the electrode/electrolyte interface reaction and improve the utilization rate of active sulfur.Herein,conductive composite nanofabrics(CCN)with multifunctional groups are employed as the interlayer of sulfur-loading cathode,in which the PMIA/PAN supporting fibers offer robust mechanical strength and high thermostable performance,and gelatin/polypyrrole functional fibers ensure high electrical conductivity and strong chemical interaction for LiPSs.As demonstrated by the experimental data and material characterizations,the presence of CCN interlayer not only blocks the shuttle behavior of LiPSs,but also strengthens the interface stability of both Li anode and sulfur-loading cathode.Interestingly,the assembled LSBs with CCN interlayer can maintain stable capacity of 686 mAh/g after 200 cycles at 0.5 A/g.This work will provide new ideas for the elaborate design of functional in terlayers/se para tors for LSBs and lithium metal batteries.
基金the financial support from the National Natural Science Foundation of China(Nos.52104312,22278329,22271229,22105153)Qin Chuangyuan Talent Project of Shaanxi Province(Nos.2021QCYRC4-43,QCYRCXM-2022-308)the State Key Laboratory for Electrical Insulation and Power Equipment(No.EIPE23125)。
文摘Lithium-sulfur batteries(LSBs)are promising energy storage systems due to their low cost and high energy density.However,sluggish reaction kinetics and the“shuttle effect”of lithium polysulfides(LiPSs)from sulfur cathode hinder the practical application of LSBs.In this work,a separator loaded with the Eu_(2)O_(3-δ)nanoparticles/carbon nanotube interlayer is designed to immobilize Li PSs and catalyze their conversion reaction.The oxygen-deficient Eu_(2)O_(3-δ)nanoparticles,with abundant catalytic sites,promote Li PSs conversion kinetics even at high current densities.Moreover,the unique 4f electronic structure of Eu_(2)O_(3-δ)effectively mitigates undesired sulfur cathode crossover,significantly enhancing the cycling performance of LSBs.Specifically,a high capacity of 620.7 mAh/g at a rate of 5 C is achieved,maintaining at 545 mAh/g after 300 cycles at 1 C.This work demonstrates the potential application of rare earth catalysts in LSBs,offering new research avenues for promoting dynamic conversion design in electrocatalysts.
