Lithium-sulfur batteries(LSBs)represent a next-generation energy storage technology,but widespread applications are restricted by the shuttle of lithium polysulfides(LiPSs).The rational design of separators has been d...Lithium-sulfur batteries(LSBs)represent a next-generation energy storage technology,but widespread applications are restricted by the shuttle of lithium polysulfides(LiPSs).The rational design of separators has been demonstrated to be one of the most efficient and cost-effective strategies to curb the shuttle effect,and tremendous research progress has been achieved.The efficiency of a separator depends on its interaction with LiPSs,which is governed by the surface energy and binding strength.Despite several review works that have been reported to advance the separators,most of them primarily focus on active material innovation and construction.The most crucial issues of surface binding energy have not been systematically reviewed,limiting the precise design of efficient separators.In this review,fundamentals related to surface energy and binding interactions with LiPSs are comprehensively analyzed and discussed.With surface binding and energy main lines,the advancements in separator engineering strategies are elaborately summarized and discussed.Moreover,techniques for evaluating affinity to LiPSs are thoroughly analyzed to avoid any ambiguities in measurement.Based on the research context,valuable research directions are suggested to construct efficient separators.This work provides guidelines to regulate the surface binding and energy of separators for high-performance LSBs.展开更多
The rapid decay of the surface wettability of plasma-treated polymers remains a critical limitation for their practical application in advanced materials.This study introduces a continuous atmospheric pressure plasma(...The rapid decay of the surface wettability of plasma-treated polymers remains a critical limitation for their practical application in advanced materials.This study introduces a continuous atmospheric pressure plasma(APP)technique for fabricating polyethylene(PE)separators with durable wettability,and elucidates the underlying mechanism.A systematic comparison of APP treatments with non-deposition and deposition gases,including Ar,Ar/O_(2),Ar/tetramethylcyclotetrasiloxane(TMCTS),and Ar/O_(2)/TMCTS,revealed the key impact factors in achieving durable wettability.Owing to the synergistic interactions of SiO_(x)C_(y)H_(z)nanoparticulate deposition,physical etching,and oxidative functionalization,the PE separator treated by Ar/O_(2)/TMCTS exhibited a 17.5-fold electrolyte wetting area compared to the original one.The improved surface energy and roughness of the SiO_(x)C_(y)H_(z)nanoparticle coating enhanced its electrochemical performance.The ionic conductivity increased by 1.9 times,while the charge transfer resistance decreased by 73.7%.Remarkably,owing to further oxidation of the SiO_(x)C_(y)H_(z)nanoparticle coating and the increase in its silica-like structure,the wetting area of the Ar/O_(2)/TMCTS-treated separator was still over 14-fold larger than that of the original separator after aging for 90 days.This study demonstrates an eco-friendly and scalable approach for fabricating high-performance battery separators and provides mechanistic insights into durable wettability by APP.展开更多
The structural design and performance characteristics of the diaphragm have a decisive impact on the safety and electrochemical performance of lithium-ion batteries(LIBs).However,traditional polyolefin diaphragms stil...The structural design and performance characteristics of the diaphragm have a decisive impact on the safety and electrochemical performance of lithium-ion batteries(LIBs).However,traditional polyolefin diaphragms still face challenges in simultaneously improving the ion transport efficiency and thermal stability.Here,we report an in situ dynamic lithium compensation strategy for manufacturing a biobased furan aramid/ceramic diaphragm(BAS)with higher thermal stability and ion transport efficiency.Specifically,exchangeable carboxyl groups(–COOH)are introduced into the bio-based furan aramid(BA)framework,which are in situ converted into–COOLi groups to form lithium ions(Li^(+))transport channels,achieving dynamic compensation of active Li^(+).The dual transmission system of ion exchange and physical pore channels synergistically enhances the ionic conductivity of BAS to 1.536 mS cm^(-1).The high polarity structure of the furan ring and the electrolyte have excellent compatibility,significantly reducing the solid–liquid interfacial energy,making BAS have extremely high electrolyte wettability(contact angle of 0°).The BA amide group forms a multi-scale bonding network with the nano-ceramics.The BAS prepared by the water-coating process exhibits excellent thermal stability(with a thermal shrinkage rate of less than 1%after 1 h at 150℃).The LiFePO_(4)|Li half-cell assembled with BAS shows a capacity retention rate of up to 91.7%after 280 cycles at 1C,with a Coulomb efficiency of 99%,demonstrating excellent cycling stability.This design and development based on bio-materials provides a new approach for high safety and high energy density battery systems.展开更多
Aqueous zinc-based batteries have emerged as promising candidates for large-scale energy storage owing to their inherent safety and cost-effectiveness.However,their widespread application is impeded by dendritic forma...Aqueous zinc-based batteries have emerged as promising candidates for large-scale energy storage owing to their inherent safety and cost-effectiveness.However,their widespread application is impeded by dendritic formation and parasitic reactions at zinc anodes.To address these issues,this study employs polyethyleneimine grafting and macropore filling to synergistically modify the cellulose separator.The zincophilic–NH_(2) and–NH–groups introduced by polyethyleneimine promote Zn^(2+)ion desolvation and nucleation processes.Concurrently,the nanocellulose incorporated into macropores not only significantly enhances mechanical properties but also compensates for macroporous defects within the cellulose separator.The optimized separator exhibits ultralow thickness(18μm),ultrahigh modulus(3.2 GPa),large ionic conductivity(19.0 mS cm^(-1)),high Zn^(2+)ion transfer number(0.63),and good biodegradability.Comprehensive experimental measurements and theoretical analysis reveal that the utilization of this separator contributes to significantly suppressed zinc dendrites and improved electrochemical kinetics.The assembled Zn//Zn cell demonstrates exceptional cycling stability(over 1000 h lifespan at10 m A cm^(-2)and 2 mAh cm^(-2)),and the Zn//MnO_(2) and Zn//I_(2) full batteries maintain excellent longterm cyclability under high cathode mass loadings.This work advances our understanding of multifunctional separator design for next-generation electrochemical energy storage systems.展开更多
Aqueous zinc ion batteries(AZIBs)are considered promising candidates owing to their inherent safety and low cost.However,the conventional glass fiber(GF)separator used in AZIBs suffers from poor physicochemical proper...Aqueous zinc ion batteries(AZIBs)are considered promising candidates owing to their inherent safety and low cost.However,the conventional glass fiber(GF)separator used in AZIBs suffers from poor physicochemical properties,leading to uncontrolled zinc(Zn)dendrite formation and undesirable side reactions.To address these limitations and enhance the electrochemical performance of AZIBs,a precisely designed functional separator is developed by incorporating UiO-66-(COOH)_(2)into a poly(vinylidene fluoride)(PVDF)framework(U-PVDF)via a direct in situ growth method.This approach enables uniform distribution of UiO-66-(COOH)_(2)both on the surface and within the PVDF backbone,without increasing separator thickness.Owing to the strong interaction between Zn^(2+)and the abundant carboxyl groups in UiO-66-(COOH)_(2),the U-PVDF separator regulates the Zn^(2+)solvation structure toward a contact ion pair-dominated structure by reducing coordinated water molecules,which effectively mitigates water-induced parasitic reactions and promotes compact Zn deposition.Consequently,a Zn/Zn symmetric cell employing the U-PVDF separator demonstrates superior cycling stability over 1500 cycles without internal short-circuiting at a current density of 6 mA cm^(−2)and an areal capacity of 2 mAh cm^(−2).Moreover,Zn/NaV_(3)O_(8)·xH_(2)O(NVO)cell with the U-PVDF separator exhibits markedly improved cyclability and rate performance compared with those using conventional GF separator.展开更多
Lithium(Li)dendrites,resulting from poor ion desolvation and transport behavior at the anode/electrolyte interface during electrodeposition,severely impede the practicality of Li metal anodes.Inspired by the transmemb...Lithium(Li)dendrites,resulting from poor ion desolvation and transport behavior at the anode/electrolyte interface during electrodeposition,severely impede the practicality of Li metal anodes.Inspired by the transmembrane cascade transport mechanism of biological ion pumps,we design a biomimetic dual-cascade separator(BDS)based on gradient pore core–shell Gd_(2)O_(3)@ZIF-7 nanoparticles to stabilize Li metal anodes.The mesoporous Gd_(2)O_(3)core,via Lewis acidic surface,weakens Li^(+) -solvent interactions,thereby reconstructing the solvation structure and achieving pre-desolvation.The microporous ZIF-7 shell then promotes final desolvation through strong confinement effect and N-rich site coordination,while its nanochannels homogenize Li^(+) transport.This synergistic meso/microporous gradient creates a unique dual-cascade effect for ion desolvation and transport.Consequently,BDS achieves a low desolvation energy barrier,a high Li^(+) transference number(0.71),and dendrite-free Li deposition.The average Coulombic efficiency rises from 72.7%to 98.4%,the cycling performance of the Li||Li symmetrical cell improves by 3.2 times,and the capacity retention of LiFePO_4(LFP)||Li full cell increases from 38.3%to73.4%after 500 cycles.This work offers a novel separator design concept,deepens Li deposition understanding,and guides separators from passive protection to active regulation.展开更多
Traditional fluorination strategies have attracted significant attention due to their ability to construct a fluorine-rich solid-electrolyte interphase(SEI)at the anode-electrolyte interface.However,the inhomogeneous ...Traditional fluorination strategies have attracted significant attention due to their ability to construct a fluorine-rich solid-electrolyte interphase(SEI)at the anode-electrolyte interface.However,the inhomogeneous distribution of LiF within the SEI layer remains a critical challenge that hinders the effective suppression of lithium dendrite growth.This work explores the synergy between HDBDPE(degradation products of decabromodiphenyl ethane)and MgF_(2),developing a fluorinated,flame-retardant separator with optimized ion channels,HDBDPE acts as both a low-toxicity flame retardant and an"F-element guide"through hydrogen bonding with MgF_(2),forming a uniform LiF SEI layer on the Li anode for rapid reaction kinetics.Moreover,under thermal runaway conditions,the MgF_(2)@HDBDPE/PP separator constructs a"high-efficiency flame-retardant barrier",effectively quenching free radicals and promoting the formation of MgBr_(2),thereby suppressing electrolyte combustion.As a result,both symmetric and full cells assembled with the MgF_(2)@HDBDPE/PP separator demonstrate superior cyclic stability and rate performance due to improved interfacial reactions.The MgF_(2)@HDBDPE/PP separator exhibits rapid flame retardancy under thermal runaway conditions.展开更多
Zn-I_(2) batteries have emerged as promising next-generation energy storage systems owing to their inherent safety,environmental compatibility,rapid reaction kinetics,and small voltage hysteresis.Nevertheless,two crit...Zn-I_(2) batteries have emerged as promising next-generation energy storage systems owing to their inherent safety,environmental compatibility,rapid reaction kinetics,and small voltage hysteresis.Nevertheless,two critical challenges,i.e.,zinc dendrite growth and polyiodide shuttle effect,severely impede their commercial viability.To conquer these limitations,this study develops a multifunctional separator fabricated from straw-derived carboxylated nanocellulose,with its negative charge density further reinforced by anionic polyacrylamide incorporation.This modification simultaneously improves the separator’s mechanical properties,ionic conductivity,and Zn^(2+)ion transfer number.Remarkably,despite its ultrathin 20μm profile,the engineered separator demonstrates exceptional dendrite suppression and parasitic reaction inhibition,enabling Zn//Zn symmetric cells to achieve impressive cycle life(>1800 h at 2 m A cm^(-2)/2 m Ah cm^(-2))while maintaining robust performance even at ultrahigh areal capacities(25 m Ah cm^(-2)).Additionally,the separator’s anionic characteristic effectively blocks polyiodide migration through electrostatic repulsion,yielding Zn-I_(2) batteries with outstanding rate capability(120.7 m Ah g^(-1)at 5 A g^(-1))and excellent cyclability(94.2%capacity retention after 10,000 cycles).And superior cycling stability can still be achieved under zinc-deficient condition and pouch cell configuration.This work establishes a new paradigm for designing high-performance zinc-based energy storage systems through rational separator engineering.展开更多
All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional l...All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.展开更多
The growing demands for energy storage systems,electric vehicles,and portable electronics have significantly pushed forward the need for safe and reliable lithium batteries.It is essential to design functional separat...The growing demands for energy storage systems,electric vehicles,and portable electronics have significantly pushed forward the need for safe and reliable lithium batteries.It is essential to design functional separators with improved mechanical and electrochemical characteristics.This review covers the improved mechanical and electrochemical performances as well as the advancements made in the design of separators utilizing a variety of techniques.In terms of electrolyte wettability and adhesion of the coating materials,we provide an overview of the current status of research on coated separators,in situ modified separators,and grafting modified separators,and elaborate additional performance parameters of interest.The characteristics of inorganics coated separators,organic framework coated separators and inorganic-organic coated separators from different fabrication methods are compared.Future directions regarding new modified materials,manufacturing process,quantitative analysis of adhesion and so on are proposed toward next-generation advanced lithium batteries.展开更多
Shuttle effect of polysulfides overshadows the superiorities of lithium-sulfur batteries.Size-sieving effect could address this thorny trouble rely on size differ in polysulfides and lithium ions.However,clogged polys...Shuttle effect of polysulfides overshadows the superiorities of lithium-sulfur batteries.Size-sieving effect could address this thorny trouble rely on size differ in polysulfides and lithium ions.However,clogged polysulfides pose some challenges for cathode and are rarely recycled during charging/discharging.Herein,an amino functionalized titanium-organic framework is designed for modifying lithium-sulfur batteries separator to address the aforementioned challenges.Wherein,the introduction of amino narrows titanium-organic framework pore size,enabling functional separator to selectively modulate lithium ions and polysulfides migration using size-sieving effect,thereby completely suppressing polysulfides shuttle.Furthermore,the blocked polysulfides will be adsorbed on the separator surface by positively charged amino leveraging electrostatic adsorption,ensuring polysulfides to redistribute and reuse,and boosting active materials utilization.Significantly,the migration of lithium ions is not hindered since there are lithium ions transfer channels formed via Lewis acid-base interaction with the help of amino.Combined with these virtues,the lithium-sulfur batteries with amino functionalized titanium-organic framework modified separator enjoy an ultralow attenuation rate of 0.045%per cycle over 1000 cycles at 1.0C.Electrostatic adsorption and Lewis acid-base interaction cover deficiencies existing in the inhibition of polysulfides shuttle by size-sieving effect,providing fresh insight into the advancement of lithium-sulfur batteries.展开更多
The thermal stability of lithium-ion battery separators is a critical determinant of battery safety and performance,especially in the context of rapidly expanding applications in electric vehicles and energy storage s...The thermal stability of lithium-ion battery separators is a critical determinant of battery safety and performance,especially in the context of rapidly expanding applications in electric vehicles and energy storage systems.While traditional polyolefin separators(PP/PE)dominate the market due to their cost-effectiveness and mechanical robustness,their inherent poor thermal stability poses significant safety risks under high-temperature conditions.This review provides a comprehensive analysis of recent advancements in enhancing separator thermal stability through coating materials(metal,ceramic,inorganic)and novel high-temperature-resistant polymers(e.g.,PVDF copolymers,PI,PAN).Notably,we critically evaluate the trade-offs between thermal resilience and electrochemical performance,such as the unintended increase in electronic conductivity from metal coatings(e.g.,Cu,MOFs)and reduced electrolyte wettability in ceramic coatings(e.g.,Al_(2)O_(3)).Innovations in hybrid coatings(e.g.,BN/PAN composites,gradient-structured MOFs)and scalable manufacturing techniques(e.g.,roll-to-roll electrospinning)are highlighted as promising strategies to balance these competing demands.Furthermore,a comparative analysis of next-generation high-temperature-resistant separators underscores their ionic conductivity,mechanical strength,and scalability,offering actionable insights for material selection.The review concludes with forward-looking perspectives on integrating machine learning for material discovery,optimizing interfacial adhesion in ceramic coatings,and advancing semi-/all-solid-state batteries to address both thermal and electrochemical challenges.This work aims to bridge the gap between laboratory innovations and industrial applications,fostering safer and more efficient lithium battery technologies.展开更多
Separator modification is an effective approach to suppress dendrite growth to realize high-energy sodium metal batteries(SMBs)in practical applications,however,its success is mainly subject to surface modification.He...Separator modification is an effective approach to suppress dendrite growth to realize high-energy sodium metal batteries(SMBs)in practical applications,however,its success is mainly subject to surface modification.Herein,a separator with multifunctional layers composed of N-doped mesoporous hollow carbon spheres(HCS)as the inner layer and sodium fluoride(NaF)as the outer layer on commercial polypropylene separator(PP)is proposed(PP@HCS-NaF)to achieve stable cycling in SMB.At the molecular level,the inner HCS layer with a high content of pyrrolic-N induces the uniform Na^(+)flux as a potential Na^(+)redistributor for homogenous deposition,whereas its hollow mesoporous structure offers nanoporous buffers and ion channels to regulate Na^(+)ion distribution and uniform deposition.The outer layer(NaF)constructs the NaF-enriched robust solid electrolyte interphase layer,significantly lowering the Na^(+)ions diffusion barrier.Benefiting from these merits,higher electrochemical performances are achieved with multifunctional double-layered PP@HCS-NaF separators compared with single-layered separators(i.e.PP@HCS or PP@NaF)in SMBs.The Na‖Cu half-cell with PP@HCS-NaF offers stable cycling(280 cycles)with a high CE(99.6%),and Na‖Na symmetric cells demonstrate extended lifespans for over 6000 h at 1 mA cm^(-2)with a progressively stable overpotential of 9 mV.Remarkably,in Na‖NVP full-cells,the PP@HCS-NaF separator grants a stable capacity of~81 mA h g^(-1)after 3500 cycles at 1 C and an impressive rate capability performance(~70 mA h g^(-1)at 15 C).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
The safety and performance of lithium-ion batteries(LIBs)largely depend on the structural design and performance characteristics of the separator.Commercial polyolefin separators suffer from problems such as poor ther...The safety and performance of lithium-ion batteries(LIBs)largely depend on the structural design and performance characteristics of the separator.Commercial polyolefin separators suffer from problems such as poor thermal stability,insufficient porosity,and inferior electrolyte wettability,which not only easily lead to battery safety issues but also significantly affect the ionic conductivity and energy density of the batteries.Herein,we have designed a facile,efficient and controllable methodology to develop a high-porosity poly(m-phenylene isophthalamide)(PMIA)separator with both excellent wettability and superior thermal resistance by a vapor-induced phase separation technique.Specifically,the PMIA separator undergoes a thermal shrinkage of less than 1%even after being treated at 200℃ for one hour,which greatly enhances the thermal safety of the battery.In addition,a continuous and interconnected high-porosity structure(porosity of 69%)is formed by utilizing a stable and controllable solvent exchange rate,thereby constructing abundant channels for the transportation of ions within the battery.Moreover,the amide groups in the PMIA molecular structure further confer the separator with excellent wettability,enabling it to possess outstanding electrolyte absorption capacity(electrolyte absorption rate of 270%).As a result,the Li||LFP full cell with PMIA separator exhibits excellent capacity and cycling stability,maintaining a reversible specific capacity of 105.6 mAh g^(-1)after 600 cycles at 5 C.And Li||NCM811 full cell with PMIA separator show no significant degradation(168.1 mAh g^(-1)at 0.5 C)after long-cycle at high temperature.These results indicate the potential of the PMIA separator for high thermal stability and high energy battery,and the scalability of this technology also provides new ideas and directions for the preparation of separators with superior comprehensive performance.展开更多
Developing electrocatalysts to inhibit polysulfide shuttling and expedite sulfur species conversion is vital for the evolution of Lithium-sulfur(Li-S)batteries.This work provides a facile strategy to design an intimat...Developing electrocatalysts to inhibit polysulfide shuttling and expedite sulfur species conversion is vital for the evolution of Lithium-sulfur(Li-S)batteries.This work provides a facile strategy to design an intimate heterostructure of MIL-88A@CdS as a sulfur electrocatalyst combining high sulfur adsorption and accelerated polysulfide conversion.The MIL-88A can give a region of high-ordered polysulfide adsorption,whereas the CdS is an effective nanoreactor for the sulfur reduction reaction(SRR).Notedly,the significant size difference between MIL-88A and CdS enables the unique heterostructure interactions.The largesize MIL-88A ensures a uniform distribution of CdS nanoparticles as a substrate.This configuration facilitates control of the initial polysulfide adsorption position relative to its final deposition site as lithium sulfide.The heterostructure also demonstrates rapid transport and efficient conversion of lithium polysulfides.Consequently,the Li-S battery with MIL-88A@CdS heterostructure modified separator delivers exceptional performance,achieving an areal capacity exceeding 6 mAh cm^(−2),an excellent rate capability of 980 mAh g^(−1) at 5 C,and notable cycling stability in a 2 Ah pouch cell over 100 cycles.This work is significant for elucidating the relationship between heterostructure and electrocatalytic performance,providing great insights for material design aimed at highly efficient future electrocatalysts in practical applications.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
Lithium-sulfur(Li-S)batteries with high energy density and capacity have garnered significant research attention among various energy storage devices.However,the shuttle effect of polysulfides(LiPSs)remains a major ch...Lithium-sulfur(Li-S)batteries with high energy density and capacity have garnered significant research attention among various energy storage devices.However,the shuttle effect of polysulfides(LiPSs)remains a major challenge for their practical application.The design of battery separators has become a key aspect in addressing the challenge.MXenes,a promising two-dimensional(2D)material,offer exceptional conductivity,large surface area,high mechanical strength,and active sites for surface reactions.When assembled into layered films,MXenes form highly tunable two-dimensional channels ranging from a few angstroms to over 1 nm.These nanoconfined channels are instrumental in facilitating lithium-ion transport while effectively impeding the shuttle effect of LiPSs,which are essential for improving the specific capacity and cyclic stability of Li-S batteries.Substantial progress has been made in developing MXenes-based separators for Li-S batteries,yet there remains a research gap in summarizing advancements from the perspective of interlayer engineering.This entails maintaining the 2D nanochannels of layered MXenes-based separators while modulating the physicochemical environment within the MXenes interlayers through targeted modifications.This review highlights advancements in in situ modification of MXenes and their integration with 0D,1D,and 2D materials to construct laminated nanocomposite separators for Li-S batteries.The future development directions of MXenes-based materials in Li-S energy storage devices are also outlined,to drive further advancements in MXenes for Li-S battery separators.展开更多
Severe lithium dendrite growth and elevated thermal runaway risks pose significant hurdles for fast-charging lithium metal batteries(LMBs)This study reports a polydopamine-functionalized hydroxyapatite/aramid(PDA@HA)h...Severe lithium dendrite growth and elevated thermal runaway risks pose significant hurdles for fast-charging lithium metal batteries(LMBs)This study reports a polydopamine-functionalized hydroxyapatite/aramid(PDA@HA)hybrid nanofibers separator to synchronously improve th fast-charging LMB's stability and safety.(1)The separator's surface,enriched with lithiophilic carbonyl and hydroxyl groups,accelerates Li~+ion desolvation,while electrophilic imine groups impede anion movement.This dual mechanism optimizes the Li^(+)-ion flux distribution on th anode,mitigating dendrite formation.(2)The polar PDA modification layer fosters the development of a Li_(3)N/LiF-rich solid electrolyt interface,further enhancing Li anode stability.Consequently,Li//Li symmetric cells with PDA@HA separators exhibit extended cycle life in L plating/stripping tests:5000 h at 1 mA cm^(-2)and 700 h at 20 mA cm^(-2),respectively,outperforming PP separators(80 h and 8 h).In LiFePO_(4)(LFP,^(2.1)mg cm^(-2))//Li full cell evaluation,the PDA@HA separator enables stable operation for 11,000 cycles at 18.2C with 87%capacity retention,significantly outperforming existing fast-charging LMB counterparts in literature.At a high LFP loading of 15.5 mg cm^(-2),the cel maintains 137.6 mAh g^(-1)(2.13 mAh cm^(-2))over 250 cycles at 3C,achieving 98%capacity retention.Moreover,the PDA@HA separato increases threshold temperature for thermal runaway and reduces the exothermic rate,intensifying the battery's thermal safety.This research underscores the importance of functional separator design in improving Li metal anode reversibility,fast-charging performance,and therma safety of LMBs.展开更多
In aqueous zinc-ion batteries(ZIBs),the separator plays a critical role beyond merely acting as an ionicconductive medium-it directly influences Zn^(2+) flux uniformity,desolvation characteristics,and overall electroc...In aqueous zinc-ion batteries(ZIBs),the separator plays a critical role beyond merely acting as an ionicconductive medium-it directly influences Zn^(2+) flux uniformity,desolvation characteristics,and overall electrochemical reversibility.Therefore,addressing the inherent limitations of conventional separator materials-such as non-uniform ion transport and structural deformation-and introducing surface functionalities are critical for enhancing electrochemical performance.In this study,a polyvinylidene fluoride(PVDF) layer was coated onto the surface of a glass fiber(GF) separator to suppress structural deformation caused by prolonged electrolyte exposure.Furthermore,plasma treatment introduced hydrophilic functional groups onto the PVDF surface,enabling hydrogen bonding with water molecules and suppressing H_(2)O-induced side reactions.An MnO_(2)‖Zn full cell using the FP@GF separator retained ~98 % of its initial capacity after 350 cycles.Even after extensive charge/discharge cycling,the interface between the separator and Zn anode remained clean.Moreover,the MnO_(2)‖Zn full cell maintained a capacity exceeding 101 mAh g^(-1) at 2.0 C after 30 days of storage,approximately twice that of its bare-GF-based counterpart.Thus,this study demonstrates a strategy to overcome the mechanical shortcomings of GF separators and suppress water-induced parasitic reactions in aqueous electrolytes,substantially enhancing the longterm stability of GF-based ZIBs.展开更多
基金supported by the National Natural Science Foundation of China (52172228)the Natural Science Foundation of Fujian Province (2024J01475 and 2023J05127)
文摘Lithium-sulfur batteries(LSBs)represent a next-generation energy storage technology,but widespread applications are restricted by the shuttle of lithium polysulfides(LiPSs).The rational design of separators has been demonstrated to be one of the most efficient and cost-effective strategies to curb the shuttle effect,and tremendous research progress has been achieved.The efficiency of a separator depends on its interaction with LiPSs,which is governed by the surface energy and binding strength.Despite several review works that have been reported to advance the separators,most of them primarily focus on active material innovation and construction.The most crucial issues of surface binding energy have not been systematically reviewed,limiting the precise design of efficient separators.In this review,fundamentals related to surface energy and binding interactions with LiPSs are comprehensively analyzed and discussed.With surface binding and energy main lines,the advancements in separator engineering strategies are elaborately summarized and discussed.Moreover,techniques for evaluating affinity to LiPSs are thoroughly analyzed to avoid any ambiguities in measurement.Based on the research context,valuable research directions are suggested to construct efficient separators.This work provides guidelines to regulate the surface binding and energy of separators for high-performance LSBs.
基金supported by the National Natural Science Foundation of China(No.12075054)the Fundamental Research Funds for the Central Universities(No.CUSF-DH-T-2024069)。
文摘The rapid decay of the surface wettability of plasma-treated polymers remains a critical limitation for their practical application in advanced materials.This study introduces a continuous atmospheric pressure plasma(APP)technique for fabricating polyethylene(PE)separators with durable wettability,and elucidates the underlying mechanism.A systematic comparison of APP treatments with non-deposition and deposition gases,including Ar,Ar/O_(2),Ar/tetramethylcyclotetrasiloxane(TMCTS),and Ar/O_(2)/TMCTS,revealed the key impact factors in achieving durable wettability.Owing to the synergistic interactions of SiO_(x)C_(y)H_(z)nanoparticulate deposition,physical etching,and oxidative functionalization,the PE separator treated by Ar/O_(2)/TMCTS exhibited a 17.5-fold electrolyte wetting area compared to the original one.The improved surface energy and roughness of the SiO_(x)C_(y)H_(z)nanoparticle coating enhanced its electrochemical performance.The ionic conductivity increased by 1.9 times,while the charge transfer resistance decreased by 73.7%.Remarkably,owing to further oxidation of the SiO_(x)C_(y)H_(z)nanoparticle coating and the increase in its silica-like structure,the wetting area of the Ar/O_(2)/TMCTS-treated separator was still over 14-fold larger than that of the original separator after aging for 90 days.This study demonstrates an eco-friendly and scalable approach for fabricating high-performance battery separators and provides mechanistic insights into durable wettability by APP.
基金the financial support from the National Natural Science Foundation of China(22293011,T2341001)the Major Science and Technology Project of Anhui Province(202203a06020010)+1 种基金the Horizontal Project Provided by Jiangsu Zhuogao New Materials Technology Co.,Ltd.(Td00923003H)Joint Laboratory by China Power Investment Ronghe New Energy Technology Co.,Ltd.and the Central Government Guiding Special Fund Project for Local Science and Technology Development(202407a12020008)。
文摘The structural design and performance characteristics of the diaphragm have a decisive impact on the safety and electrochemical performance of lithium-ion batteries(LIBs).However,traditional polyolefin diaphragms still face challenges in simultaneously improving the ion transport efficiency and thermal stability.Here,we report an in situ dynamic lithium compensation strategy for manufacturing a biobased furan aramid/ceramic diaphragm(BAS)with higher thermal stability and ion transport efficiency.Specifically,exchangeable carboxyl groups(–COOH)are introduced into the bio-based furan aramid(BA)framework,which are in situ converted into–COOLi groups to form lithium ions(Li^(+))transport channels,achieving dynamic compensation of active Li^(+).The dual transmission system of ion exchange and physical pore channels synergistically enhances the ionic conductivity of BAS to 1.536 mS cm^(-1).The high polarity structure of the furan ring and the electrolyte have excellent compatibility,significantly reducing the solid–liquid interfacial energy,making BAS have extremely high electrolyte wettability(contact angle of 0°).The BA amide group forms a multi-scale bonding network with the nano-ceramics.The BAS prepared by the water-coating process exhibits excellent thermal stability(with a thermal shrinkage rate of less than 1%after 1 h at 150℃).The LiFePO_(4)|Li half-cell assembled with BAS shows a capacity retention rate of up to 91.7%after 280 cycles at 1C,with a Coulomb efficiency of 99%,demonstrating excellent cycling stability.This design and development based on bio-materials provides a new approach for high safety and high energy density battery systems.
基金the financial support from the Natural Science Foundation of Jiangsu Province(BK20231292)the Jiangsu Agricultural Science and Technology Innovation Fund(CX(24)3091)+7 种基金the National Key R&D Program of China(2024YFE0109200)the Fundamental Research Funds for the Central Universities(No.2024300440)the Guangdong Basic and Applied Basic Research Foundation(2025A1515011098)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX24_1299)the National Natural Science Foundation of China(12464032)the Natural Science Foundation of Jiangxi Province(20232BAB201032)the Ji’an Science and Technology Plan Project(2024H-100301)supported by the high-performance computing campus level public platform of Jinggangshan University。
文摘Aqueous zinc-based batteries have emerged as promising candidates for large-scale energy storage owing to their inherent safety and cost-effectiveness.However,their widespread application is impeded by dendritic formation and parasitic reactions at zinc anodes.To address these issues,this study employs polyethyleneimine grafting and macropore filling to synergistically modify the cellulose separator.The zincophilic–NH_(2) and–NH–groups introduced by polyethyleneimine promote Zn^(2+)ion desolvation and nucleation processes.Concurrently,the nanocellulose incorporated into macropores not only significantly enhances mechanical properties but also compensates for macroporous defects within the cellulose separator.The optimized separator exhibits ultralow thickness(18μm),ultrahigh modulus(3.2 GPa),large ionic conductivity(19.0 mS cm^(-1)),high Zn^(2+)ion transfer number(0.63),and good biodegradability.Comprehensive experimental measurements and theoretical analysis reveal that the utilization of this separator contributes to significantly suppressed zinc dendrites and improved electrochemical kinetics.The assembled Zn//Zn cell demonstrates exceptional cycling stability(over 1000 h lifespan at10 m A cm^(-2)and 2 mAh cm^(-2)),and the Zn//MnO_(2) and Zn//I_(2) full batteries maintain excellent longterm cyclability under high cathode mass loadings.This work advances our understanding of multifunctional separator design for next-generation electrochemical energy storage systems.
基金supported by the Basic Science Research Program(RS-2024-00455177)through the National Research Foundation of Korea(NRF)funded by the Ministry of Science,ICT.
文摘Aqueous zinc ion batteries(AZIBs)are considered promising candidates owing to their inherent safety and low cost.However,the conventional glass fiber(GF)separator used in AZIBs suffers from poor physicochemical properties,leading to uncontrolled zinc(Zn)dendrite formation and undesirable side reactions.To address these limitations and enhance the electrochemical performance of AZIBs,a precisely designed functional separator is developed by incorporating UiO-66-(COOH)_(2)into a poly(vinylidene fluoride)(PVDF)framework(U-PVDF)via a direct in situ growth method.This approach enables uniform distribution of UiO-66-(COOH)_(2)both on the surface and within the PVDF backbone,without increasing separator thickness.Owing to the strong interaction between Zn^(2+)and the abundant carboxyl groups in UiO-66-(COOH)_(2),the U-PVDF separator regulates the Zn^(2+)solvation structure toward a contact ion pair-dominated structure by reducing coordinated water molecules,which effectively mitigates water-induced parasitic reactions and promotes compact Zn deposition.Consequently,a Zn/Zn symmetric cell employing the U-PVDF separator demonstrates superior cycling stability over 1500 cycles without internal short-circuiting at a current density of 6 mA cm^(−2)and an areal capacity of 2 mAh cm^(−2).Moreover,Zn/NaV_(3)O_(8)·xH_(2)O(NVO)cell with the U-PVDF separator exhibits markedly improved cyclability and rate performance compared with those using conventional GF separator.
基金the financial support from the National Natural Science Foundation of China(22408182)the Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region(NJYT24024)the Natural Science Foundation of Inner Mongolia Autonomous Region(2023QN02007 and 2025QN02009)。
文摘Lithium(Li)dendrites,resulting from poor ion desolvation and transport behavior at the anode/electrolyte interface during electrodeposition,severely impede the practicality of Li metal anodes.Inspired by the transmembrane cascade transport mechanism of biological ion pumps,we design a biomimetic dual-cascade separator(BDS)based on gradient pore core–shell Gd_(2)O_(3)@ZIF-7 nanoparticles to stabilize Li metal anodes.The mesoporous Gd_(2)O_(3)core,via Lewis acidic surface,weakens Li^(+) -solvent interactions,thereby reconstructing the solvation structure and achieving pre-desolvation.The microporous ZIF-7 shell then promotes final desolvation through strong confinement effect and N-rich site coordination,while its nanochannels homogenize Li^(+) transport.This synergistic meso/microporous gradient creates a unique dual-cascade effect for ion desolvation and transport.Consequently,BDS achieves a low desolvation energy barrier,a high Li^(+) transference number(0.71),and dendrite-free Li deposition.The average Coulombic efficiency rises from 72.7%to 98.4%,the cycling performance of the Li||Li symmetrical cell improves by 3.2 times,and the capacity retention of LiFePO_4(LFP)||Li full cell increases from 38.3%to73.4%after 500 cycles.This work offers a novel separator design concept,deepens Li deposition understanding,and guides separators from passive protection to active regulation.
基金financially supported by the National Natural Science Foundation of China(52401283)National Natural Science Foundation of Jiangsu Province(BK20230933)+1 种基金Fundamental Research Funds for the Central Universities(No.30925010524)Young Faculty Development Fund of Nanjing University of Science and Technology。
文摘Traditional fluorination strategies have attracted significant attention due to their ability to construct a fluorine-rich solid-electrolyte interphase(SEI)at the anode-electrolyte interface.However,the inhomogeneous distribution of LiF within the SEI layer remains a critical challenge that hinders the effective suppression of lithium dendrite growth.This work explores the synergy between HDBDPE(degradation products of decabromodiphenyl ethane)and MgF_(2),developing a fluorinated,flame-retardant separator with optimized ion channels,HDBDPE acts as both a low-toxicity flame retardant and an"F-element guide"through hydrogen bonding with MgF_(2),forming a uniform LiF SEI layer on the Li anode for rapid reaction kinetics.Moreover,under thermal runaway conditions,the MgF_(2)@HDBDPE/PP separator constructs a"high-efficiency flame-retardant barrier",effectively quenching free radicals and promoting the formation of MgBr_(2),thereby suppressing electrolyte combustion.As a result,both symmetric and full cells assembled with the MgF_(2)@HDBDPE/PP separator demonstrate superior cyclic stability and rate performance due to improved interfacial reactions.The MgF_(2)@HDBDPE/PP separator exhibits rapid flame retardancy under thermal runaway conditions.
基金the financial support from the Natural Science Foundation of Jiangsu Province(BK20231292)the Jiangsu Agricultural Science and Technology Innovation Fund(CX(24)3091)+6 种基金the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX25_1429)the National Key R&D Program of China(2024YFE0109200)the Fundamental Research Funds for the Central Universities(No.2024300440)Guangdong Basic and Applied Basic Research Foundation(2025A1515011098)the National Natural Science Foundation of China(12464032)the Natural Science Foundation of Jiangxi Province(20232BAB201032)Ji'an Science and Technology Plan Project(2024H-100301)。
文摘Zn-I_(2) batteries have emerged as promising next-generation energy storage systems owing to their inherent safety,environmental compatibility,rapid reaction kinetics,and small voltage hysteresis.Nevertheless,two critical challenges,i.e.,zinc dendrite growth and polyiodide shuttle effect,severely impede their commercial viability.To conquer these limitations,this study develops a multifunctional separator fabricated from straw-derived carboxylated nanocellulose,with its negative charge density further reinforced by anionic polyacrylamide incorporation.This modification simultaneously improves the separator’s mechanical properties,ionic conductivity,and Zn^(2+)ion transfer number.Remarkably,despite its ultrathin 20μm profile,the engineered separator demonstrates exceptional dendrite suppression and parasitic reaction inhibition,enabling Zn//Zn symmetric cells to achieve impressive cycle life(>1800 h at 2 m A cm^(-2)/2 m Ah cm^(-2))while maintaining robust performance even at ultrahigh areal capacities(25 m Ah cm^(-2)).Additionally,the separator’s anionic characteristic effectively blocks polyiodide migration through electrostatic repulsion,yielding Zn-I_(2) batteries with outstanding rate capability(120.7 m Ah g^(-1)at 5 A g^(-1))and excellent cyclability(94.2%capacity retention after 10,000 cycles).And superior cycling stability can still be achieved under zinc-deficient condition and pouch cell configuration.This work establishes a new paradigm for designing high-performance zinc-based energy storage systems through rational separator engineering.
基金National Natural Science Foundation of China (52203123)Sichuan Science and Technology Program (2023NSFSC0991)+2 种基金State Key Laboratory of Polymer Materials Engineering (sklpme-2023-1-05 and sklpme-2024-2-04)Fundamental Research Funds for the Central UniversitiesThis research was also partially sponsored by the Double First-Class Construction Funds of Sichuan University。
文摘All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.
基金the Center of Lithium Battery Membrane Materials jointly established by School of Chemistry and Chemical Engineering of Huazhong University of Science and Technology and Shenzhen Senior Technology Material Co.Ltd.,the National Natural Science Foundation of China(52020105012,52303084)the Young Scientists Fund of Natural Science Foundation of Hubei Province(2023AFB220)for the support of this work.
文摘The growing demands for energy storage systems,electric vehicles,and portable electronics have significantly pushed forward the need for safe and reliable lithium batteries.It is essential to design functional separators with improved mechanical and electrochemical characteristics.This review covers the improved mechanical and electrochemical performances as well as the advancements made in the design of separators utilizing a variety of techniques.In terms of electrolyte wettability and adhesion of the coating materials,we provide an overview of the current status of research on coated separators,in situ modified separators,and grafting modified separators,and elaborate additional performance parameters of interest.The characteristics of inorganics coated separators,organic framework coated separators and inorganic-organic coated separators from different fabrication methods are compared.Future directions regarding new modified materials,manufacturing process,quantitative analysis of adhesion and so on are proposed toward next-generation advanced lithium batteries.
基金supported by the National Natural Science Foundation of China(52463013 and 52073133)Key Talent Project Foundation of Gansu Province+3 种基金Joint fund between Shenyang National Laboratory for Materials ScienceState Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals(18LHPY002)the Program for Hongliu Distinguished Young Scholars in Lanzhou University of Technologythe Incubation Program of Excellent Doctoral Dissertation–Lanzhou University of Technology
文摘Shuttle effect of polysulfides overshadows the superiorities of lithium-sulfur batteries.Size-sieving effect could address this thorny trouble rely on size differ in polysulfides and lithium ions.However,clogged polysulfides pose some challenges for cathode and are rarely recycled during charging/discharging.Herein,an amino functionalized titanium-organic framework is designed for modifying lithium-sulfur batteries separator to address the aforementioned challenges.Wherein,the introduction of amino narrows titanium-organic framework pore size,enabling functional separator to selectively modulate lithium ions and polysulfides migration using size-sieving effect,thereby completely suppressing polysulfides shuttle.Furthermore,the blocked polysulfides will be adsorbed on the separator surface by positively charged amino leveraging electrostatic adsorption,ensuring polysulfides to redistribute and reuse,and boosting active materials utilization.Significantly,the migration of lithium ions is not hindered since there are lithium ions transfer channels formed via Lewis acid-base interaction with the help of amino.Combined with these virtues,the lithium-sulfur batteries with amino functionalized titanium-organic framework modified separator enjoy an ultralow attenuation rate of 0.045%per cycle over 1000 cycles at 1.0C.Electrostatic adsorption and Lewis acid-base interaction cover deficiencies existing in the inhibition of polysulfides shuttle by size-sieving effect,providing fresh insight into the advancement of lithium-sulfur batteries.
基金supported by Beijing Institute of Technology Student Innovation Training Program(BIT2024LH013).
文摘The thermal stability of lithium-ion battery separators is a critical determinant of battery safety and performance,especially in the context of rapidly expanding applications in electric vehicles and energy storage systems.While traditional polyolefin separators(PP/PE)dominate the market due to their cost-effectiveness and mechanical robustness,their inherent poor thermal stability poses significant safety risks under high-temperature conditions.This review provides a comprehensive analysis of recent advancements in enhancing separator thermal stability through coating materials(metal,ceramic,inorganic)and novel high-temperature-resistant polymers(e.g.,PVDF copolymers,PI,PAN).Notably,we critically evaluate the trade-offs between thermal resilience and electrochemical performance,such as the unintended increase in electronic conductivity from metal coatings(e.g.,Cu,MOFs)and reduced electrolyte wettability in ceramic coatings(e.g.,Al_(2)O_(3)).Innovations in hybrid coatings(e.g.,BN/PAN composites,gradient-structured MOFs)and scalable manufacturing techniques(e.g.,roll-to-roll electrospinning)are highlighted as promising strategies to balance these competing demands.Furthermore,a comparative analysis of next-generation high-temperature-resistant separators underscores their ionic conductivity,mechanical strength,and scalability,offering actionable insights for material selection.The review concludes with forward-looking perspectives on integrating machine learning for material discovery,optimizing interfacial adhesion in ceramic coatings,and advancing semi-/all-solid-state batteries to address both thermal and electrochemical challenges.This work aims to bridge the gap between laboratory innovations and industrial applications,fostering safer and more efficient lithium battery technologies.
基金supported by the National Natural Science Foundation of China(Grant Number 22350410379)Zhejiang Provincial Natural Science Foundation of China(LZ23B030003)+1 种基金the Fundamental Research Funds for the Central Universities(226-202400075)Ten Thousand Talent Program of Zhejiang Province.
文摘Separator modification is an effective approach to suppress dendrite growth to realize high-energy sodium metal batteries(SMBs)in practical applications,however,its success is mainly subject to surface modification.Herein,a separator with multifunctional layers composed of N-doped mesoporous hollow carbon spheres(HCS)as the inner layer and sodium fluoride(NaF)as the outer layer on commercial polypropylene separator(PP)is proposed(PP@HCS-NaF)to achieve stable cycling in SMB.At the molecular level,the inner HCS layer with a high content of pyrrolic-N induces the uniform Na^(+)flux as a potential Na^(+)redistributor for homogenous deposition,whereas its hollow mesoporous structure offers nanoporous buffers and ion channels to regulate Na^(+)ion distribution and uniform deposition.The outer layer(NaF)constructs the NaF-enriched robust solid electrolyte interphase layer,significantly lowering the Na^(+)ions diffusion barrier.Benefiting from these merits,higher electrochemical performances are achieved with multifunctional double-layered PP@HCS-NaF separators compared with single-layered separators(i.e.PP@HCS or PP@NaF)in SMBs.The Na‖Cu half-cell with PP@HCS-NaF offers stable cycling(280 cycles)with a high CE(99.6%),and Na‖Na symmetric cells demonstrate extended lifespans for over 6000 h at 1 mA cm^(-2)with a progressively stable overpotential of 9 mV.Remarkably,in Na‖NVP full-cells,the PP@HCS-NaF separator grants a stable capacity of~81 mA h g^(-1)after 3500 cycles at 1 C and an impressive rate capability performance(~70 mA h g^(-1)at 15 C).
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supported by the National Natural Science Foundation of China(52273059,52403046)the Science and Technology Plans of Tianjin(22JCYBJC01030)+1 种基金the Tianjin Research Innovation Project for Postgraduate Students(2022BKY145)partially supported by financial contributions from Yantai Tayho Advanced Materials Co.,Ltd。
文摘The safety and performance of lithium-ion batteries(LIBs)largely depend on the structural design and performance characteristics of the separator.Commercial polyolefin separators suffer from problems such as poor thermal stability,insufficient porosity,and inferior electrolyte wettability,which not only easily lead to battery safety issues but also significantly affect the ionic conductivity and energy density of the batteries.Herein,we have designed a facile,efficient and controllable methodology to develop a high-porosity poly(m-phenylene isophthalamide)(PMIA)separator with both excellent wettability and superior thermal resistance by a vapor-induced phase separation technique.Specifically,the PMIA separator undergoes a thermal shrinkage of less than 1%even after being treated at 200℃ for one hour,which greatly enhances the thermal safety of the battery.In addition,a continuous and interconnected high-porosity structure(porosity of 69%)is formed by utilizing a stable and controllable solvent exchange rate,thereby constructing abundant channels for the transportation of ions within the battery.Moreover,the amide groups in the PMIA molecular structure further confer the separator with excellent wettability,enabling it to possess outstanding electrolyte absorption capacity(electrolyte absorption rate of 270%).As a result,the Li||LFP full cell with PMIA separator exhibits excellent capacity and cycling stability,maintaining a reversible specific capacity of 105.6 mAh g^(-1)after 600 cycles at 5 C.And Li||NCM811 full cell with PMIA separator show no significant degradation(168.1 mAh g^(-1)at 0.5 C)after long-cycle at high temperature.These results indicate the potential of the PMIA separator for high thermal stability and high energy battery,and the scalability of this technology also provides new ideas and directions for the preparation of separators with superior comprehensive performance.
基金supported by the Natural Science Foundation of China(22309179)the Natural Science Foundation of China(12404049)+4 种基金Natural Science Foundation of Ningxia(2023AAC01003)Guangdong Basic and Applied Basic Research Foundation(2021A1515110156,2022A1515010724,2023A1515110521,2023B1515120095,2024A1515011260)Science and Technology Program of Guangzhou(No.2019050001)the Outstanding Youth Project of Guangdong Natural Science Foundation(2021B1515020051)Dalian Revitalization Talents Program(No.2022RG01).
文摘Developing electrocatalysts to inhibit polysulfide shuttling and expedite sulfur species conversion is vital for the evolution of Lithium-sulfur(Li-S)batteries.This work provides a facile strategy to design an intimate heterostructure of MIL-88A@CdS as a sulfur electrocatalyst combining high sulfur adsorption and accelerated polysulfide conversion.The MIL-88A can give a region of high-ordered polysulfide adsorption,whereas the CdS is an effective nanoreactor for the sulfur reduction reaction(SRR).Notedly,the significant size difference between MIL-88A and CdS enables the unique heterostructure interactions.The largesize MIL-88A ensures a uniform distribution of CdS nanoparticles as a substrate.This configuration facilitates control of the initial polysulfide adsorption position relative to its final deposition site as lithium sulfide.The heterostructure also demonstrates rapid transport and efficient conversion of lithium polysulfides.Consequently,the Li-S battery with MIL-88A@CdS heterostructure modified separator delivers exceptional performance,achieving an areal capacity exceeding 6 mAh cm^(−2),an excellent rate capability of 980 mAh g^(−1) at 5 C,and notable cycling stability in a 2 Ah pouch cell over 100 cycles.This work is significant for elucidating the relationship between heterostructure and electrocatalytic performance,providing great insights for material design aimed at highly efficient future electrocatalysts in practical applications.
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 Beijing Natural Science Foundation(Nos.2232037 and 2242035)the National Natural Science Foundation of China(Nos.22005012,22105012 and 51803183)+1 种基金Chunhui Plan Cooperative Project of Ministry of Education(No.202201298)the China Postdoctoral Science Foundation Funded Project(No.2023M733520).
文摘Lithium-sulfur(Li-S)batteries with high energy density and capacity have garnered significant research attention among various energy storage devices.However,the shuttle effect of polysulfides(LiPSs)remains a major challenge for their practical application.The design of battery separators has become a key aspect in addressing the challenge.MXenes,a promising two-dimensional(2D)material,offer exceptional conductivity,large surface area,high mechanical strength,and active sites for surface reactions.When assembled into layered films,MXenes form highly tunable two-dimensional channels ranging from a few angstroms to over 1 nm.These nanoconfined channels are instrumental in facilitating lithium-ion transport while effectively impeding the shuttle effect of LiPSs,which are essential for improving the specific capacity and cyclic stability of Li-S batteries.Substantial progress has been made in developing MXenes-based separators for Li-S batteries,yet there remains a research gap in summarizing advancements from the perspective of interlayer engineering.This entails maintaining the 2D nanochannels of layered MXenes-based separators while modulating the physicochemical environment within the MXenes interlayers through targeted modifications.This review highlights advancements in in situ modification of MXenes and their integration with 0D,1D,and 2D materials to construct laminated nanocomposite separators for Li-S batteries.The future development directions of MXenes-based materials in Li-S energy storage devices are also outlined,to drive further advancements in MXenes for Li-S battery separators.
基金supported by the National Natural Science Foundation of China(Grant No.52202328,52372099,52271222)the Shanghai Sailing Program(22YF1455500)。
文摘Severe lithium dendrite growth and elevated thermal runaway risks pose significant hurdles for fast-charging lithium metal batteries(LMBs)This study reports a polydopamine-functionalized hydroxyapatite/aramid(PDA@HA)hybrid nanofibers separator to synchronously improve th fast-charging LMB's stability and safety.(1)The separator's surface,enriched with lithiophilic carbonyl and hydroxyl groups,accelerates Li~+ion desolvation,while electrophilic imine groups impede anion movement.This dual mechanism optimizes the Li^(+)-ion flux distribution on th anode,mitigating dendrite formation.(2)The polar PDA modification layer fosters the development of a Li_(3)N/LiF-rich solid electrolyt interface,further enhancing Li anode stability.Consequently,Li//Li symmetric cells with PDA@HA separators exhibit extended cycle life in L plating/stripping tests:5000 h at 1 mA cm^(-2)and 700 h at 20 mA cm^(-2),respectively,outperforming PP separators(80 h and 8 h).In LiFePO_(4)(LFP,^(2.1)mg cm^(-2))//Li full cell evaluation,the PDA@HA separator enables stable operation for 11,000 cycles at 18.2C with 87%capacity retention,significantly outperforming existing fast-charging LMB counterparts in literature.At a high LFP loading of 15.5 mg cm^(-2),the cel maintains 137.6 mAh g^(-1)(2.13 mAh cm^(-2))over 250 cycles at 3C,achieving 98%capacity retention.Moreover,the PDA@HA separato increases threshold temperature for thermal runaway and reduces the exothermic rate,intensifying the battery's thermal safety.This research underscores the importance of functional separator design in improving Li metal anode reversibility,fast-charging performance,and therma safety of LMBs.
基金supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government(MSIT)(RS2024-00342112)the Korea Institute of Energy Technology Evaluation and Planning(KETEP) grant funded by the Korea government (MOTIE) (RS-2023-00303581, Multiscale Simulation-Driven Development of Cost-Effective and Stable Aqueous Zn Ion Battery with Energy Density of 110 Wh/L for Energy Storage Systems: A Korea-USA Collaboration)+1 种基金the Technology Innovation Program (RS-2024-00429384) funded by the Ministry of Trade, Industry & Energy(MOTIE, Korea)the Technology Innovation Program (RS-2024-00470022) funded by the Ministry of Trade, Industry & Energy(MOTIE, Korea)。
文摘In aqueous zinc-ion batteries(ZIBs),the separator plays a critical role beyond merely acting as an ionicconductive medium-it directly influences Zn^(2+) flux uniformity,desolvation characteristics,and overall electrochemical reversibility.Therefore,addressing the inherent limitations of conventional separator materials-such as non-uniform ion transport and structural deformation-and introducing surface functionalities are critical for enhancing electrochemical performance.In this study,a polyvinylidene fluoride(PVDF) layer was coated onto the surface of a glass fiber(GF) separator to suppress structural deformation caused by prolonged electrolyte exposure.Furthermore,plasma treatment introduced hydrophilic functional groups onto the PVDF surface,enabling hydrogen bonding with water molecules and suppressing H_(2)O-induced side reactions.An MnO_(2)‖Zn full cell using the FP@GF separator retained ~98 % of its initial capacity after 350 cycles.Even after extensive charge/discharge cycling,the interface between the separator and Zn anode remained clean.Moreover,the MnO_(2)‖Zn full cell maintained a capacity exceeding 101 mAh g^(-1) at 2.0 C after 30 days of storage,approximately twice that of its bare-GF-based counterpart.Thus,this study demonstrates a strategy to overcome the mechanical shortcomings of GF separators and suppress water-induced parasitic reactions in aqueous electrolytes,substantially enhancing the longterm stability of GF-based ZIBs.
