Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because ...Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because it has a high specific surfacearea for sulfur loading.We have developed a pressurizedphysical activation(PPA)method that producedan activated carbon(PPAC)with a high specific surfacearea comparable to that of CAC.The pore structure of PPAC could be changed and its use as a cathode material for Li–Sbatteries was investigated.Battery tests at different capacity rates(C-rates)showed that it had a much improved high-rate performancewith a discharge capacity of 900 mAh/(g of sulfur)at 1 C,in contrast to only 600 mAh/(g of sulfur)for CAC.Porestructure analyses showed that PPAC prepared at a high activation temperature(1000℃)had unusual channel-like mesoporesbetween the microdomains that are the basic structural units of artificial carbon materials.These are connected to microporesdeveloped in each microdomain,and deliver ions from the surroundings to the internal pores and vice versa.The well-developedmicropores and mesopores of PPAC respectively ensured the high adsorption of lithium polysulfides and a high rate ofion diffusion.Compared to CAC,PPAC is a high-performance,low-cost cathode material that is promising for use in futureLi–S batteries.展开更多
Herein,3‑aminopropyltriethoxysilane(APTES)was used to modify F‑containing silica slag(SS)by simple grafting and served as a multifunctional barrier layer.The amino group(—NH2)in the amino‑modified SS(NH2‑SS)forms lig...Herein,3‑aminopropyltriethoxysilane(APTES)was used to modify F‑containing silica slag(SS)by simple grafting and served as a multifunctional barrier layer.The amino group(—NH2)in the amino‑modified SS(NH2‑SS)forms ligand bonds or hydrogen bonds with sulfur ions in lithium polysulfides(LiPSs),thus inhibiting the shuttle effect.Electrochemical analyses demonstrated that lithium‑sulfur(Li‑S)batteries employing the NH2‑SS interlayer exhibited discharge specific capacities of 1048 and 789 mAh·g^(-1) at 0.2C and 2C,respectively,and even at 4C,the initial discharge specific capacity remained at 590 mAh·g^(-1),outperforming the Li‑S battery with unmodified SS as the interlayer.展开更多
Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a no...Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a novel MoS_(2)-Mo_(2)C heterostructure anchored on a carbon sponge(CS)as a Li_(2)S host to solve these problems.A simple hydrothermal process following carbothermal reduction was used to construct the MoS_(2)-Mo_(2)C heterostructure,enabling control of the phases and integration of MoS_(2) and Mo_(2)C.Structural characterization confirmed the coherent interface of the heterostructure with a precise orientation relationship between the two phases and their uniform distribution.An evaluation of the adsorption and catalytic performance of the material showed that it has an exceptional LiPSs adsorption capacity with faster conversion from Li_(2)S_(4) to Li_(2)S_(2).Density functional theory calculations further confirmed these results.As a result,the cathode had a high initial discharge capacity of 693 mAh g^(−1) at 0.2 C and achieved stable cycling at 2 C for 500 cycles with a low decay rate of 0.107%per cycle.The heterostructure design,coupled with the macroporous CS framework,effectively prevented the shuttling and increased sulfur utilization,offering a promising way to produce practical high-energydensity Li–S batteries.展开更多
Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_...Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_(2)(PO_(4))_(3)(LVP@C)nanoparticles on carbon nanofibers(CNFs)has been achieved by an electrospinning technique followed by calcination.The protective carbon coating prevents the aggregation of the LVP nanoparticles and suppresses V dissolution by preventing direct contact with aqueous electrolytes.The CNFs derived from the electrospun nanofibers provide a 3D network to increase the electronic conductivity of the LVP electrode,and the LVP@C-CNF hybrid film can be directly used as a freestanding cathode for zinc-ion batteries without adding conductive additives and binders.A mechanism for the formation of a uniform and continuous carbon coating has been proposed.This nanostructure,combined with the uniform and intact carbon coverage,significantly increases the electronic conductivity.This LVP@C-CNF freestanding electrode has an excellent rate capability(47.3%retention at 2 C)and cycling stability(61.2%retention after 100 cycles)within the voltage range 0.6 V to 1.95 V and is highly suitable for zinc-ion battery applications.展开更多
Aqueous zinc-ion batteries(AZIBs) are regarded as one of the most promising energy conversion and storage devices.Nevertheless,side reactions and dendrite growth on the zinc metal anode hinder their widespread applica...Aqueous zinc-ion batteries(AZIBs) are regarded as one of the most promising energy conversion and storage devices.Nevertheless,side reactions and dendrite growth on the zinc metal anode hinder their widespread application.In this study,hemin was employed as a multi-functional artificial interface for the first time to inhibit the disordered growth of zinc dendrites and mitigate side reactions.Theoretical calculations indicate that hemin is preferentially adsorbed onto the zinc anode,thus blocking the interaction between the active zinc anode and electrolyte.Compared with zinc foil,the Hemin@Zn anode demonstrates enhanced corrosion resistance,a decrease in hydrogen evolution,and more orderly deposition of zinc.As expected,the symmetric cell with Hemin@Zn anode can sustain up to 4000 h at 0.2 mA/cm^(2),0.2 mAh/cm^(2).Asymmetric Zn//Cu cells exhibit an average coulombic efficiency exceeding 99.72 % during 500 cycles.Moreover,the full cell Hemin@Zn//NH_(4)V_(4)O_(10) delivers a superior capacity up to 367 m Ah/g and the discharge capacity retention reaches 124 mAh/g after 1200 cycles even at a current density of 5 A/g.This work provides a simple and effective method for constructing a robust artificial interface to promote the application of long-life AZIBs.展开更多
Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully syn...Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully synthesize nano-sized Wadsley-Roth FeNb_(11)O_(29)through Fe-driven phase transformation of Nb_(2)O_(5),which delivers a high specific capacity(280.5 mA h g^(−1)at 0.25 C)along with abundant redox-active sites.Moreover,the Wadsley-Roth shear structure of FeNb_(11)O_(29)facilitates rapid Li^(+)diffusion and guarantees exceptional structural stability.Theoretical calculations further confirm that FeNb_(11)O_(29)has a narrow band gap,which significantly enhances the conductivity.Owing to these merits,FeNb_(11)O_(29)achieves a full charge/discharge cycle within merely 25 s at 75 C rate and retains remarkable cycling stability over 2500 cycles.As a consequence,our assembled FeNb_(11)O_(29)||LiFePO_(4)full cell demonstrates ultra-long cyclability(>10000 cycles)and outstanding fast-charging capability(complete cycling within 2 min at 30 C).These findings highlight nano-sized FeNb_(11)O_(29)as a highly promising anode candidate for next-generation fast-charging LIBs.展开更多
Strategies for achieving high-energy-density lithium-ion batteries include using high-capacity materials such as high-nickel NCM,increasing the active material content in the electrode by utilizing high-conductivity c...Strategies for achieving high-energy-density lithium-ion batteries include using high-capacity materials such as high-nickel NCM,increasing the active material content in the electrode by utilizing high-conductivity carbon nanotubes(CNT)conductive materials,and electrode thickening.However,these methods are still limited due to the limitation in the capacity of high-nickel NCM,aggregation of CNT conductive materials,and nonuniform material distribution of thick-film electrodes,which ultimately damage the mechanical and electrical integrity of the electrode,leading to a decrease in electrochemical performance.Here,we present an integrated binder-CNT composite dispersion solution to realize a high-solids-content(>77 wt%)slurry for high-mass-loading electrodes and to mitigate the migration of binder and conductive additives.Indeed,the approach reduces solvent usage by approximately 30%and ensures uniform conductive additive-binder domain distribution during electrode manufacturing,resulting in improved coating quality and adhesive strength for high-mass-loading electrodes(>12 mAh cm^(−2)).In terms of various electrode properties,the presented electrode showed low resistance and excellent electrochemical properties despite the low CNT contents of 0.6 wt%compared to the pristine-applied electrode with 0.85 wt%CNT contents.Moreover,our strategy enables faster drying,which increases the coating speed,thereby offering potential energy savings and supporting carbon neutrality in wet-based electrode manufacturing processes.展开更多
The development of shape-customizable and bulk flexible electrochemical devices through processing technologies as versatile as those used for plastics promises to revolutionize the future of battery technology.Howeve...The development of shape-customizable and bulk flexible electrochemical devices through processing technologies as versatile as those used for plastics promises to revolutionize the future of battery technology.However,this pursuit has been fundamentally hindered by the absence of transformative battery materials capable of delivering the necessary electrochemical functions,robust interface adhesion,and,crucially,the suitable rheological properties required for on-demand shaping.In this work,we introduce a concept of a multifunctional plasticine electrode matrix(PEM)featuring nano-interpenetrating networks(nano-IPN)to address this challenge.Utilizing the nonflammable liquid-electrolyte hydration combined with conductive nanomaterials,we have realized a PEM in the form of a multifunctional nanocomposite that integrates ion and electron conduction,component binding,non-flammability,and plasticine-like moldability.With this PEM,we have successfully fabricated a variety of bulk-flexible electrodes with high mass loading of active material(AM)(>70 wt%)using industry-friendly extrusion and compression molding techniques.Moreover,these high AM-loading composite electrodes achieve an unparalleled bulk conformability and flexibility,remaining structurally intact even under severe mechanical stress.Ultimately,we have successfully produced shape-patternable and flexible batteries via extrusion molding.This study underscores the potential of the PEM to revolutionize battery microstructures,interfaces,manufacturing processes,and performance characteristics.展开更多
The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightfor...The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightforward reduction approach was employed to design three bimetallic alloy nanoparticles(FeNi,FeCo,and NiCo)supported on multistage porous carbon substrates.Experimental and theoretical calculations reveal that the charge transfer within the alloy catalyst influences the position of its d-band center and its degree of hybridization with sodium polysulfides(NaPSs).An increased charge transfer leads to a shift of the alloy’s d-band center closer to the Fermi energy level,thereby enhancing its adsorption and catalytic capabilities.Among the three alloy compositions,the FeNi alloy exhibits the highest charge transfer.Consequently,the FeNi alloy demonstrates the superior electrochemical performance,achieving a high reversible specific capacity of 848.2 mA h g^(−1),with an average capacity degradation rate of only 0.037%per cycle over 1000 cycles at 1.2 C.The S/FeNi/NC cathode exhibits a low electrolyte-to-sulfur(E/S)ratio of 6.6µL mg^(−1),while maintaining a high reversible specific capacity of 568.1 mA h g^(−1).This offers valuable insights for the application of alloy catalysts in the S/FeNi/NC cathode of RT Na-S batteries.展开更多
All-solid-state batteries(ASSBs)represent a next-generation energy storage technology,offering enhanced safety,higher energy density,and improved cycling stability compared to conventional liquid-electrolyte-based lit...All-solid-state batteries(ASSBs)represent a next-generation energy storage technology,offering enhanced safety,higher energy density,and improved cycling stability compared to conventional liquid-electrolyte-based lithium-ion batteries.Understanding and optimizing the complex chemistries and interfaces that underpin ASSB performance present significant challenges from both experimental and modeling perspectives.In particular,atomistic simulations face difficulties in capturing the complex structure,disorder,and dynamic evolution of materials and interfaces under practically relevant conditions.While established methods such as density functional theory and classical force fields have provided valuable insights,some questions remain difficult to address,particularly those involving large system sizes or long timescales.Recently,machine learning interatomic potentials(MLIPs)have emerged as a transformative tool,enabling atomistic simulations at length and time scales that were previously challenging to access with conventional approaches.By delivering near first-principles accuracy with much greater efficiency,MLIPs open new avenues for large-scale,long-timescale,and high-throughput simulations of solid-state battery materials.In this review,we present a comparative overview of density functional theory,classical force fields,and MLIPs,highlighting their respective strengths and limitations in ASSB research.We then discuss how MLIPs enable simulations that reach longer timescales,larger system sizes,and support high-throughput calculations,providing unique insights into ion transport and interfacial evolution in ASSBs.Finally,we conclude with a summary and outlook on current challenges and future opportunities for expanding MLIP capabilities and accelerating their impact in solid-state battery research.展开更多
Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and of...Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.展开更多
Achieving high-energy density remains a key objective for advanced energy storage systems.However,challenges,such as poor cathode conductivity,anode dendrite formation,polysulfide shuttling,and electrolyte degradation...Achieving high-energy density remains a key objective for advanced energy storage systems.However,challenges,such as poor cathode conductivity,anode dendrite formation,polysulfide shuttling,and electrolyte degradation,continue to limit performance and stability.Molecular and ionic dipole interactions have emerged as an effective strategy to address these issues by regulating ionic transport,modulating solvation structures,optimizing interfacial chemistry,and enhancing charge transfer kinetics.These interactions also stabilize electrode interfaces,suppress side reactions,and mitigate anode corrosion,collectively improving the durability of high-energy batteries.A deeper understanding of these mechanisms is essential to guide the design of next-generation battery materials.Herein,this review summarizes the development,classification,and advantages of dipole interactions in high-energy batteries.The roles of dipoles,including facilitating ion transport,controlling solvation dynamics,stabilizing the electric double layer,optimizing solid electrolyte interphase and cathode–electrolyte interface layers,and inhibiting parasitic reactions—are comprehensively discussed.Finally,perspectives on future research directions are proposed to advance dipole-enabled strategies for high-performance energy storage.This review aims to provide insights into the rational design of dipole-interactive systems and promote the progress of electrochemical energy storage technologies.展开更多
Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implem...Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implementation remains a significant challenge.Herein,we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs.Specifically,polypyrrole(PPy)is in situ vapor-phase polymerized on the surface of N-doped TiO_(2) nanorods supported on carbon cloth(N-TiO_(2)/CC),thereby forming a well-defined p–n heterojunction.This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field.Thus,the PPy@N-TiO_(2)/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur,enabling ultrafast sulfur redox dynamics,as convincingly validated by both theoretical simulations and experimental results.Consequently,the PPy@N-TiO_(2)/CC PALSB achieves a high discharge capacity of 1653 mAh g^(−1),reaching 98.7%of the theoretical value.Furthermore,5 h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333 mAh g^(−1),achieving dual-mode energy harvesting capabilities.This work successfully integrates solar energy conversion and storage within a rechargeable battery system,providing a promising strategy for sustainable energy storage technologies.展开更多
Zinc-air batteries(ZABs)are promising candidates for flexible electronics due to their high energy density and low cost.However,their development is hindered by the sluggish kinetics of the oxygen evolution reaction(O...Zinc-air batteries(ZABs)are promising candidates for flexible electronics due to their high energy density and low cost.However,their development is hindered by the sluggish kinetics of the oxygen evolution reaction(OER)and oxygen reduction reaction(ORR).Herein,we present a novel heterostructured electrocatalyst composed of vertically aligned N-doped graphene(NVG)arrays anchored on Ru-doped ceria(RCO)nanofibers,synthesized via a one-step plasma-enhanced chemical vapor deposition process.Notably,during the plasma-enhanced driven NVG growth,Ru nanoparticles are spontaneously in-situ exsolved from the RCO lattice,forming a unique Ru@RCO-NVG heterostructure.Density functional theory calculations reveal that the Ru@RCO-NVG heterojunction induces interfacial electronic redistribution,thereby significantly lowering the energy barriers for both OER and ORR.Benefiting from the synergistic effects,the Ru@RCO-NVG catalyst exhibits exceptional intrinsic activity towards OER/ORR(an overpotential of 370 mV for OER at 10 mA cm^(−2)and a half-wave potential of 0.86 V for ORR),and higher all-solid-state flexible ZAB performance(peak power density of 286.1 mW cm^(−2)),surpassing commercial Pt/C-IrO_(2)catalysts.This work not only advances the integration of synergistic graphene/ceria composites but also offers a promising strategy for designing efficient electrocatalysts for next-generation energy conversion technologies.展开更多
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
Lithium metal batteries(LMBs)have emerged as pivotal energy storage solutions for electric vehicles and portable electronics.However,their operation under extreme conditions(high-temperature and fast-charging conditio...Lithium metal batteries(LMBs)have emerged as pivotal energy storage solutions for electric vehicles and portable electronics.However,their operation under extreme conditions(high-temperature and fast-charging conditions)faces significant challenges,including accelerated electrolyte decomposition,interfacial instability,and potential thermal runaway risks.To address these challenges,we present a solvation-interphase synergistic regulation strategy using 2-fluorobenzenesulfonamide(2-FBS)as a multifunctional electrolyte additive.The 2-FBS molecule effectively modulates the Li^(+)solvation structure by reducing the coordination of ethylene carbonate(EC)solvent.This transformation suppresses EC-induced parasitic reactions while scavenging superoxide radicals,thereby mitigating gas evolution at electrode interfaces.Upon preferential decomposition,2-FBS further promotes the formation of a robust LiF-Li_(3)N-Li_(2)S-rich interphase with exceptional mechanical strength(Young’s modulus:39.4 GPa).This inorganic-rich hybrid interphase simultaneously enables dendrite-free lithium plating and enhances cathode thermal stability.Consequently,2-FBS-modified electrolyte empowers LiCoO_(2)//Li cells to deliver 82.8%capacity retention after 800 cycles at 55°C and sustain 81.2%capacity retention after 1500 cycles at 4 C.Moreover,practical validation through nail penetration tests confirms the effectiveness of the electrolyte in preventing thermal propagation in fully charged pouch cells.This work establishes a paradigm for enabling reliable battery operation under extreme conditions through synergistic solvation and interphase engineering.展开更多
Sn-based batteries have emerged as an optimal energy storage system owing to their abundant Sn resources,environmental compatibility,non-toxicity,corrosion resistance,and high hydrogen evolution overpotential.However,...Sn-based batteries have emerged as an optimal energy storage system owing to their abundant Sn resources,environmental compatibility,non-toxicity,corrosion resistance,and high hydrogen evolution overpotential.However,the practical application of these batteries is hindered by challenges such as“dead Sn”shedding and hydrogen evolution side reactions.Extensive research has focused on improving the performance of Sn-based batteries.This paper provides a comprehensive review of the recent advancements in Sn-based battery research,including the selection of current collectors,electrolyte optimization,and the development of new cathode materials.The energy storage mechanisms and challenges of Sn-based batteries are discussed.Overall,this paper presents future perspectives of high-performance rechargeable Sn-based batteries and provides valuable guidance for developing Sn-based energy storage technologies.展开更多
Lithium-sulfur(Li-S)batteries require efficient catalysts to accelerate polysulfide conversion and mitigate the shuttle effect.However,the rational design of catalysts remains challenging due to the lack of a systemat...Lithium-sulfur(Li-S)batteries require efficient catalysts to accelerate polysulfide conversion and mitigate the shuttle effect.However,the rational design of catalysts remains challenging due to the lack of a systematic strategy that rationally optimizes electronic structures and mesoscale transport properties.In this work,we propose an autogenously transformed CoWO_(4)/WO_(2) heterojunction catalyst,integrating a strong polysulfide-adsorbing intercalation catalyst with a metallic-phase promoter for enhanced activity.CoWO_(4) effectively captures polysulfides,while the CoWO_(4)/WO_(2) interface facilitates their S-S bond activation on heterogenous catalytic sites.Benefiting from its directional intercalation channels,CoWO_(4) not only serves as a dynamic Li-ion reservoir but also provides continuous and direct pathways for rapid Li-ion transport.Such synergistic interactions across the heterojunction interfaces enhance the catalytic activity of the composite.As a result,the CoWO_(4)/WO_(2) heterostructure demonstrates significantly enhanced catalytic performance,delivering a high capacity of 1262 mAh g^(−1) at 0.1 C.Furthermore,its rate capability and high sulfur loading performance are markedly improved,surpassing the limitations of its single-component counterparts.This study provides new insights into the catalytic mechanisms governing Li-S chemistry and offers a promising strategy for the rational design of high-performance Li-S battery catalysts.展开更多
Wide-temperature applications of sodium-ion batteries(SIBs)are severely limited by the sluggish ion insertion/diffusion kinetics of conversion-type anodes.Quantum-sized transition metal dichalcogenides possess unique ...Wide-temperature applications of sodium-ion batteries(SIBs)are severely limited by the sluggish ion insertion/diffusion kinetics of conversion-type anodes.Quantum-sized transition metal dichalcogenides possess unique advantages of charge delocalization and enrich uncoordinated electrons and short-range transfer kinetics,which are crucial to achieve rapid low-temperature charge transfer and high-temperature interface stability.Herein,a quantum-scale FeS_(2) loaded on three-dimensional Ti_(3)C_(2) MXene skeletons(FeS_(2) QD/MXene)fabricated as SIBs anode,demonstrating impressive performance under wide-temperature conditions(−35 to 65).The theoretical calculations combined with experimental characterization interprets that the unsaturated coordination edges of FeS_(2) QD can induce delocalized electronic regions,which reduces electrostatic potential and significantly facilitates efficient Na+diffusion across a broad temperature range.Moreover,the Ti_(3)C_(2) skeleton reinforces structural integrity via Fe-O-Ti bonding,while enabling excellent dispersion of FeS_(2) QD.As expected,FeS_(2) QD/MXene anode harvests capacities of 255.2 and 424.9 mAh g^(−1) at 0.1 A g^(−1) under−35 and 65,and the energy density of FeS_(2) QD/MXene//NVP full cell can reach to 162.4 Wh kg^(−1) at−35,highlighting its practical potential for wide-temperatures conditions.This work extends the uncoordinated regions induced by quantum-size effects for exceptional Na^(+)ion storage and diffusion performance at wide-temperatures environment.展开更多
Aqueous zinc-ion batteries(AZIBs)hold great promise for next-generation energy storage but face challenges such as Zn dendrite growth,side reactions,and limited performance at low temperatures.Here,we propose an elect...Aqueous zinc-ion batteries(AZIBs)hold great promise for next-generation energy storage but face challenges such as Zn dendrite growth,side reactions,and limited performance at low temperatures.Here,we propose an electrolyte design strategy that reconstructs the hydrogenbond network through the synergistic effect of glycerol(GL)and methylsulfonamide(MSA),enabling the formation of a(100)-oriented Zn anode.This design significantly broadens the operating current and temperature windows of AZIBs.As a result,Zn||Zn symmetric cells exhibit remarkable cycling stability,achieving 4,000 h at 1 mA cm^(-2)and 600 h at 40 mA cm^(-2)(both at 1 mAh cm^(-2)capacity);even at-20℃,Zn||Zn symmetric cells deliver ultra-stable cycling for over 5,400 h.Furthermore,Zn||VO_(2)full cells retain 77.3%of their capacity after 2,000 cycles at 30°C with a current density of 0.5 A g^(-1)and 85.4%capacity retention after 2,000 cycles at-20°C and 0.25 A g^(-1).These results demonstrate a robust pathway for enhancing the practicality and low-temperature adaptability of AZIBs.展开更多
文摘Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because it has a high specific surfacearea for sulfur loading.We have developed a pressurizedphysical activation(PPA)method that producedan activated carbon(PPAC)with a high specific surfacearea comparable to that of CAC.The pore structure of PPAC could be changed and its use as a cathode material for Li–Sbatteries was investigated.Battery tests at different capacity rates(C-rates)showed that it had a much improved high-rate performancewith a discharge capacity of 900 mAh/(g of sulfur)at 1 C,in contrast to only 600 mAh/(g of sulfur)for CAC.Porestructure analyses showed that PPAC prepared at a high activation temperature(1000℃)had unusual channel-like mesoporesbetween the microdomains that are the basic structural units of artificial carbon materials.These are connected to microporesdeveloped in each microdomain,and deliver ions from the surroundings to the internal pores and vice versa.The well-developedmicropores and mesopores of PPAC respectively ensured the high adsorption of lithium polysulfides and a high rate ofion diffusion.Compared to CAC,PPAC is a high-performance,low-cost cathode material that is promising for use in futureLi–S batteries.
文摘Herein,3‑aminopropyltriethoxysilane(APTES)was used to modify F‑containing silica slag(SS)by simple grafting and served as a multifunctional barrier layer.The amino group(—NH2)in the amino‑modified SS(NH2‑SS)forms ligand bonds or hydrogen bonds with sulfur ions in lithium polysulfides(LiPSs),thus inhibiting the shuttle effect.Electrochemical analyses demonstrated that lithium‑sulfur(Li‑S)batteries employing the NH2‑SS interlayer exhibited discharge specific capacities of 1048 and 789 mAh·g^(-1) at 0.2C and 2C,respectively,and even at 4C,the initial discharge specific capacity remained at 590 mAh·g^(-1),outperforming the Li‑S battery with unmodified SS as the interlayer.
文摘Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a novel MoS_(2)-Mo_(2)C heterostructure anchored on a carbon sponge(CS)as a Li_(2)S host to solve these problems.A simple hydrothermal process following carbothermal reduction was used to construct the MoS_(2)-Mo_(2)C heterostructure,enabling control of the phases and integration of MoS_(2) and Mo_(2)C.Structural characterization confirmed the coherent interface of the heterostructure with a precise orientation relationship between the two phases and their uniform distribution.An evaluation of the adsorption and catalytic performance of the material showed that it has an exceptional LiPSs adsorption capacity with faster conversion from Li_(2)S_(4) to Li_(2)S_(2).Density functional theory calculations further confirmed these results.As a result,the cathode had a high initial discharge capacity of 693 mAh g^(−1) at 0.2 C and achieved stable cycling at 2 C for 500 cycles with a low decay rate of 0.107%per cycle.The heterostructure design,coupled with the macroporous CS framework,effectively prevented the shuttling and increased sulfur utilization,offering a promising way to produce practical high-energydensity Li–S batteries.
文摘Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_(2)(PO_(4))_(3)(LVP@C)nanoparticles on carbon nanofibers(CNFs)has been achieved by an electrospinning technique followed by calcination.The protective carbon coating prevents the aggregation of the LVP nanoparticles and suppresses V dissolution by preventing direct contact with aqueous electrolytes.The CNFs derived from the electrospun nanofibers provide a 3D network to increase the electronic conductivity of the LVP electrode,and the LVP@C-CNF hybrid film can be directly used as a freestanding cathode for zinc-ion batteries without adding conductive additives and binders.A mechanism for the formation of a uniform and continuous carbon coating has been proposed.This nanostructure,combined with the uniform and intact carbon coverage,significantly increases the electronic conductivity.This LVP@C-CNF freestanding electrode has an excellent rate capability(47.3%retention at 2 C)and cycling stability(61.2%retention after 100 cycles)within the voltage range 0.6 V to 1.95 V and is highly suitable for zinc-ion battery applications.
基金financially supported by the National Natural Science Foundation of China (No.52372188)Natural Science Foundation of Henan (Nos.242300421625,252300421333)+4 种基金CAS Henan Industrial Technology Innovation & Incubation Center (No.2024121)Key Scientific Research Project of Education Department of Henan Province (Nos.22A150042,23A150038,and 24A150019)2023 Introduction of studying abroad talent programthe China Postdoctoral Science Foundation (No.2019 M652546)Key Project of Science and Technology of Henan Province (No.252102240007)。
文摘Aqueous zinc-ion batteries(AZIBs) are regarded as one of the most promising energy conversion and storage devices.Nevertheless,side reactions and dendrite growth on the zinc metal anode hinder their widespread application.In this study,hemin was employed as a multi-functional artificial interface for the first time to inhibit the disordered growth of zinc dendrites and mitigate side reactions.Theoretical calculations indicate that hemin is preferentially adsorbed onto the zinc anode,thus blocking the interaction between the active zinc anode and electrolyte.Compared with zinc foil,the Hemin@Zn anode demonstrates enhanced corrosion resistance,a decrease in hydrogen evolution,and more orderly deposition of zinc.As expected,the symmetric cell with Hemin@Zn anode can sustain up to 4000 h at 0.2 mA/cm^(2),0.2 mAh/cm^(2).Asymmetric Zn//Cu cells exhibit an average coulombic efficiency exceeding 99.72 % during 500 cycles.Moreover,the full cell Hemin@Zn//NH_(4)V_(4)O_(10) delivers a superior capacity up to 367 m Ah/g and the discharge capacity retention reaches 124 mAh/g after 1200 cycles even at a current density of 5 A/g.This work provides a simple and effective method for constructing a robust artificial interface to promote the application of long-life AZIBs.
基金financially supported by the National Natural Science Foundation of China(52272209).Dedicated to his Alma Mater,Tianjin University,on the occasion of her 130th anniversary by Wei Zhang,who earned his bachelor's degree there in 1997.
文摘Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully synthesize nano-sized Wadsley-Roth FeNb_(11)O_(29)through Fe-driven phase transformation of Nb_(2)O_(5),which delivers a high specific capacity(280.5 mA h g^(−1)at 0.25 C)along with abundant redox-active sites.Moreover,the Wadsley-Roth shear structure of FeNb_(11)O_(29)facilitates rapid Li^(+)diffusion and guarantees exceptional structural stability.Theoretical calculations further confirm that FeNb_(11)O_(29)has a narrow band gap,which significantly enhances the conductivity.Owing to these merits,FeNb_(11)O_(29)achieves a full charge/discharge cycle within merely 25 s at 75 C rate and retains remarkable cycling stability over 2500 cycles.As a consequence,our assembled FeNb_(11)O_(29)||LiFePO_(4)full cell demonstrates ultra-long cyclability(>10000 cycles)and outstanding fast-charging capability(complete cycling within 2 min at 30 C).These findings highlight nano-sized FeNb_(11)O_(29)as a highly promising anode candidate for next-generation fast-charging LIBs.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.2022M3H4A6A0103720142)the National Research Council of Science&Technology(NST)grant by the Korea government(MSIT)(No.GTL24011-000)+1 种基金the Technology Innovation Program(RS-2024-00404165)through the Korea Planning&Evaluation Institute of Industrial Technology(KEIT)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea)supported by the Samsung SDI Co.Ltd.and the Korea Institute of Science and Technology(KIST)institutional program(2E33942,2E3394B)。
文摘Strategies for achieving high-energy-density lithium-ion batteries include using high-capacity materials such as high-nickel NCM,increasing the active material content in the electrode by utilizing high-conductivity carbon nanotubes(CNT)conductive materials,and electrode thickening.However,these methods are still limited due to the limitation in the capacity of high-nickel NCM,aggregation of CNT conductive materials,and nonuniform material distribution of thick-film electrodes,which ultimately damage the mechanical and electrical integrity of the electrode,leading to a decrease in electrochemical performance.Here,we present an integrated binder-CNT composite dispersion solution to realize a high-solids-content(>77 wt%)slurry for high-mass-loading electrodes and to mitigate the migration of binder and conductive additives.Indeed,the approach reduces solvent usage by approximately 30%and ensures uniform conductive additive-binder domain distribution during electrode manufacturing,resulting in improved coating quality and adhesive strength for high-mass-loading electrodes(>12 mAh cm^(−2)).In terms of various electrode properties,the presented electrode showed low resistance and excellent electrochemical properties despite the low CNT contents of 0.6 wt%compared to the pristine-applied electrode with 0.85 wt%CNT contents.Moreover,our strategy enables faster drying,which increases the coating speed,thereby offering potential energy savings and supporting carbon neutrality in wet-based electrode manufacturing processes.
基金financial support from the National Natural Science Foundation of China(52473248,52203123,52125301,22279070 and U21A20170)the State Key Laboratory of Polymer Materials Engineering(Grant No:sklpme 2023-1-05 and sklpme 2024-2-04)+2 种基金the Ministry of Science and Technology of China(No.2019YFA0705703)the Sichuan Science and Technology Program(2023NSFSC0991 and 2025ZNSFSC1411)the Fundamental Research Funds for the Central Universities.This research was partially sponsored by the Double First-Class Construction Funds of Sichuan University.
文摘The development of shape-customizable and bulk flexible electrochemical devices through processing technologies as versatile as those used for plastics promises to revolutionize the future of battery technology.However,this pursuit has been fundamentally hindered by the absence of transformative battery materials capable of delivering the necessary electrochemical functions,robust interface adhesion,and,crucially,the suitable rheological properties required for on-demand shaping.In this work,we introduce a concept of a multifunctional plasticine electrode matrix(PEM)featuring nano-interpenetrating networks(nano-IPN)to address this challenge.Utilizing the nonflammable liquid-electrolyte hydration combined with conductive nanomaterials,we have realized a PEM in the form of a multifunctional nanocomposite that integrates ion and electron conduction,component binding,non-flammability,and plasticine-like moldability.With this PEM,we have successfully fabricated a variety of bulk-flexible electrodes with high mass loading of active material(AM)(>70 wt%)using industry-friendly extrusion and compression molding techniques.Moreover,these high AM-loading composite electrodes achieve an unparalleled bulk conformability and flexibility,remaining structurally intact even under severe mechanical stress.Ultimately,we have successfully produced shape-patternable and flexible batteries via extrusion molding.This study underscores the potential of the PEM to revolutionize battery microstructures,interfaces,manufacturing processes,and performance characteristics.
基金supported by Shaanxi Fundamental Science Research Project for Chemistry and Biology(23JHQ011)Natural Science Foundation of Shaanxi(2024JC-YBMS-115)Natural Science Basic Research Plan in Shaanxi Province of China(2025JC-YBMS-141)。
文摘The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightforward reduction approach was employed to design three bimetallic alloy nanoparticles(FeNi,FeCo,and NiCo)supported on multistage porous carbon substrates.Experimental and theoretical calculations reveal that the charge transfer within the alloy catalyst influences the position of its d-band center and its degree of hybridization with sodium polysulfides(NaPSs).An increased charge transfer leads to a shift of the alloy’s d-band center closer to the Fermi energy level,thereby enhancing its adsorption and catalytic capabilities.Among the three alloy compositions,the FeNi alloy exhibits the highest charge transfer.Consequently,the FeNi alloy demonstrates the superior electrochemical performance,achieving a high reversible specific capacity of 848.2 mA h g^(−1),with an average capacity degradation rate of only 0.037%per cycle over 1000 cycles at 1.2 C.The S/FeNi/NC cathode exhibits a low electrolyte-to-sulfur(E/S)ratio of 6.6µL mg^(−1),while maintaining a high reversible specific capacity of 568.1 mA h g^(−1).This offers valuable insights for the application of alloy catalysts in the S/FeNi/NC cathode of RT Na-S batteries.
文摘All-solid-state batteries(ASSBs)represent a next-generation energy storage technology,offering enhanced safety,higher energy density,and improved cycling stability compared to conventional liquid-electrolyte-based lithium-ion batteries.Understanding and optimizing the complex chemistries and interfaces that underpin ASSB performance present significant challenges from both experimental and modeling perspectives.In particular,atomistic simulations face difficulties in capturing the complex structure,disorder,and dynamic evolution of materials and interfaces under practically relevant conditions.While established methods such as density functional theory and classical force fields have provided valuable insights,some questions remain difficult to address,particularly those involving large system sizes or long timescales.Recently,machine learning interatomic potentials(MLIPs)have emerged as a transformative tool,enabling atomistic simulations at length and time scales that were previously challenging to access with conventional approaches.By delivering near first-principles accuracy with much greater efficiency,MLIPs open new avenues for large-scale,long-timescale,and high-throughput simulations of solid-state battery materials.In this review,we present a comparative overview of density functional theory,classical force fields,and MLIPs,highlighting their respective strengths and limitations in ASSB research.We then discuss how MLIPs enable simulations that reach longer timescales,larger system sizes,and support high-throughput calculations,providing unique insights into ion transport and interfacial evolution in ASSBs.Finally,we conclude with a summary and outlook on current challenges and future opportunities for expanding MLIP capabilities and accelerating their impact in solid-state battery research.
基金supported by Basic Science Research Program(Priority Research Institute)through the NRF of Korea funded by the Ministry of Education(2021R1A6A1A10039823)by the Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Ministry of Education(2020R1A6C101B194)。
文摘Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.
基金supported by the introduction of Talent Research Fund in Nanjing Institute of Technology(YKJ202204)the National Natural Science Foundation of China(52401282 and 52300206)the Natural Science Foundation of Jiangsu Province(BK20230701 and BK20230705).
文摘Achieving high-energy density remains a key objective for advanced energy storage systems.However,challenges,such as poor cathode conductivity,anode dendrite formation,polysulfide shuttling,and electrolyte degradation,continue to limit performance and stability.Molecular and ionic dipole interactions have emerged as an effective strategy to address these issues by regulating ionic transport,modulating solvation structures,optimizing interfacial chemistry,and enhancing charge transfer kinetics.These interactions also stabilize electrode interfaces,suppress side reactions,and mitigate anode corrosion,collectively improving the durability of high-energy batteries.A deeper understanding of these mechanisms is essential to guide the design of next-generation battery materials.Herein,this review summarizes the development,classification,and advantages of dipole interactions in high-energy batteries.The roles of dipoles,including facilitating ion transport,controlling solvation dynamics,stabilizing the electric double layer,optimizing solid electrolyte interphase and cathode–electrolyte interface layers,and inhibiting parasitic reactions—are comprehensively discussed.Finally,perspectives on future research directions are proposed to advance dipole-enabled strategies for high-performance energy storage.This review aims to provide insights into the rational design of dipole-interactive systems and promote the progress of electrochemical energy storage technologies.
基金the financial support from the National Natural Science Foundation of China (22109127)the Chinese Postdoctoral Science Foundation (2021M702666)+2 种基金the Research Fund of the State Key Laboratory of Solidification Processing (NPU),China (Grant No.2023-TS-02)The financial support from the Youth Project of"Shaanxi High-level Talents Introduction Plan"the Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) are also sincerely appreciated
文摘Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implementation remains a significant challenge.Herein,we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs.Specifically,polypyrrole(PPy)is in situ vapor-phase polymerized on the surface of N-doped TiO_(2) nanorods supported on carbon cloth(N-TiO_(2)/CC),thereby forming a well-defined p–n heterojunction.This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field.Thus,the PPy@N-TiO_(2)/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur,enabling ultrafast sulfur redox dynamics,as convincingly validated by both theoretical simulations and experimental results.Consequently,the PPy@N-TiO_(2)/CC PALSB achieves a high discharge capacity of 1653 mAh g^(−1),reaching 98.7%of the theoretical value.Furthermore,5 h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333 mAh g^(−1),achieving dual-mode energy harvesting capabilities.This work successfully integrates solar energy conversion and storage within a rechargeable battery system,providing a promising strategy for sustainable energy storage technologies.
基金supported by the National Natural Science Foundation of China(Grant No.22479133,and No.22469008)the Natural Science Foundation of Guangdong Province(Grant No.2024A1515012235).
文摘Zinc-air batteries(ZABs)are promising candidates for flexible electronics due to their high energy density and low cost.However,their development is hindered by the sluggish kinetics of the oxygen evolution reaction(OER)and oxygen reduction reaction(ORR).Herein,we present a novel heterostructured electrocatalyst composed of vertically aligned N-doped graphene(NVG)arrays anchored on Ru-doped ceria(RCO)nanofibers,synthesized via a one-step plasma-enhanced chemical vapor deposition process.Notably,during the plasma-enhanced driven NVG growth,Ru nanoparticles are spontaneously in-situ exsolved from the RCO lattice,forming a unique Ru@RCO-NVG heterostructure.Density functional theory calculations reveal that the Ru@RCO-NVG heterojunction induces interfacial electronic redistribution,thereby significantly lowering the energy barriers for both OER and ORR.Benefiting from the synergistic effects,the Ru@RCO-NVG catalyst exhibits exceptional intrinsic activity towards OER/ORR(an overpotential of 370 mV for OER at 10 mA cm^(−2)and a half-wave potential of 0.86 V for ORR),and higher all-solid-state flexible ZAB performance(peak power density of 286.1 mW cm^(−2)),surpassing commercial Pt/C-IrO_(2)catalysts.This work not only advances the integration of synergistic graphene/ceria composites but also offers a promising strategy for designing efficient electrocatalysts for next-generation energy conversion technologies.
基金supported by the National Natural Science Foundation of China(52172228)the Natural Science Foundation of Fujian Province(2024J01475 and 2023J05127)This report was proposed and supervised by Liangxu Lin.All other co-authors provided assistance and suggestions on the writing and presentation.
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 Key Laboratory of Sichuan Province for Lithium Resources Comprehensive Utilization and New Lithium Based Materials for Advanced Battery Technology(LRMKF202405)the National Natural Science Foundation of China(52402226)+1 种基金the Sichuan Provincial Natural Science Foundation(2024NSFSC1016)The authors extend their gratitude Scientific Compass(www.shiyanjia.com)for providing invaluable assistance with the HRTEM analysis.The authors also thank Yi Tang from SCI-GO(www.sci-go.com)for the AFM analysis and Hua Guo from Phadcalc(www.phadcalc.com)for molecular dynamics simulations.
文摘Lithium metal batteries(LMBs)have emerged as pivotal energy storage solutions for electric vehicles and portable electronics.However,their operation under extreme conditions(high-temperature and fast-charging conditions)faces significant challenges,including accelerated electrolyte decomposition,interfacial instability,and potential thermal runaway risks.To address these challenges,we present a solvation-interphase synergistic regulation strategy using 2-fluorobenzenesulfonamide(2-FBS)as a multifunctional electrolyte additive.The 2-FBS molecule effectively modulates the Li^(+)solvation structure by reducing the coordination of ethylene carbonate(EC)solvent.This transformation suppresses EC-induced parasitic reactions while scavenging superoxide radicals,thereby mitigating gas evolution at electrode interfaces.Upon preferential decomposition,2-FBS further promotes the formation of a robust LiF-Li_(3)N-Li_(2)S-rich interphase with exceptional mechanical strength(Young’s modulus:39.4 GPa).This inorganic-rich hybrid interphase simultaneously enables dendrite-free lithium plating and enhances cathode thermal stability.Consequently,2-FBS-modified electrolyte empowers LiCoO_(2)//Li cells to deliver 82.8%capacity retention after 800 cycles at 55°C and sustain 81.2%capacity retention after 1500 cycles at 4 C.Moreover,practical validation through nail penetration tests confirms the effectiveness of the electrolyte in preventing thermal propagation in fully charged pouch cells.This work establishes a paradigm for enabling reliable battery operation under extreme conditions through synergistic solvation and interphase engineering.
基金supported by the National Natural Science Foundation of China(No.62464010)the Spring City Plan-Special Program for Young Talents(K202005007)+2 种基金the Yunnan Talents Support Plan for Young Talents(XDYC-QNRC-2022-0482)the Yunnan Local Colleges Applied Basic Research Projects(202101BA070001-138)the Key Laboratory of Artificial Microstructures in Yunnan Higher Education,and the Frontier Research Team of Kunming University 2023.
文摘Sn-based batteries have emerged as an optimal energy storage system owing to their abundant Sn resources,environmental compatibility,non-toxicity,corrosion resistance,and high hydrogen evolution overpotential.However,the practical application of these batteries is hindered by challenges such as“dead Sn”shedding and hydrogen evolution side reactions.Extensive research has focused on improving the performance of Sn-based batteries.This paper provides a comprehensive review of the recent advancements in Sn-based battery research,including the selection of current collectors,electrolyte optimization,and the development of new cathode materials.The energy storage mechanisms and challenges of Sn-based batteries are discussed.Overall,this paper presents future perspectives of high-performance rechargeable Sn-based batteries and provides valuable guidance for developing Sn-based energy storage technologies.
基金support of the National Natural Science Foundation of China(22075131 and 22078265)the Shaanxi Fundamental Science Research Project for Mathematics and Physics under Grants(No.22JSZ005)the State-Key Laboratory of Multiphase Complex Systems(No.MPCS-2021-A).
文摘Lithium-sulfur(Li-S)batteries require efficient catalysts to accelerate polysulfide conversion and mitigate the shuttle effect.However,the rational design of catalysts remains challenging due to the lack of a systematic strategy that rationally optimizes electronic structures and mesoscale transport properties.In this work,we propose an autogenously transformed CoWO_(4)/WO_(2) heterojunction catalyst,integrating a strong polysulfide-adsorbing intercalation catalyst with a metallic-phase promoter for enhanced activity.CoWO_(4) effectively captures polysulfides,while the CoWO_(4)/WO_(2) interface facilitates their S-S bond activation on heterogenous catalytic sites.Benefiting from its directional intercalation channels,CoWO_(4) not only serves as a dynamic Li-ion reservoir but also provides continuous and direct pathways for rapid Li-ion transport.Such synergistic interactions across the heterojunction interfaces enhance the catalytic activity of the composite.As a result,the CoWO_(4)/WO_(2) heterostructure demonstrates significantly enhanced catalytic performance,delivering a high capacity of 1262 mAh g^(−1) at 0.1 C.Furthermore,its rate capability and high sulfur loading performance are markedly improved,surpassing the limitations of its single-component counterparts.This study provides new insights into the catalytic mechanisms governing Li-S chemistry and offers a promising strategy for the rational design of high-performance Li-S battery catalysts.
基金supported by the National Nature Science Foundation of China(Nos.52202335 and 52171227)Natural Science Foundation of Jiangsu Province(No.BK20221137)National Key R&D Program of China(2024YFE0108500).
文摘Wide-temperature applications of sodium-ion batteries(SIBs)are severely limited by the sluggish ion insertion/diffusion kinetics of conversion-type anodes.Quantum-sized transition metal dichalcogenides possess unique advantages of charge delocalization and enrich uncoordinated electrons and short-range transfer kinetics,which are crucial to achieve rapid low-temperature charge transfer and high-temperature interface stability.Herein,a quantum-scale FeS_(2) loaded on three-dimensional Ti_(3)C_(2) MXene skeletons(FeS_(2) QD/MXene)fabricated as SIBs anode,demonstrating impressive performance under wide-temperature conditions(−35 to 65).The theoretical calculations combined with experimental characterization interprets that the unsaturated coordination edges of FeS_(2) QD can induce delocalized electronic regions,which reduces electrostatic potential and significantly facilitates efficient Na+diffusion across a broad temperature range.Moreover,the Ti_(3)C_(2) skeleton reinforces structural integrity via Fe-O-Ti bonding,while enabling excellent dispersion of FeS_(2) QD.As expected,FeS_(2) QD/MXene anode harvests capacities of 255.2 and 424.9 mAh g^(−1) at 0.1 A g^(−1) under−35 and 65,and the energy density of FeS_(2) QD/MXene//NVP full cell can reach to 162.4 Wh kg^(−1) at−35,highlighting its practical potential for wide-temperatures conditions.This work extends the uncoordinated regions induced by quantum-size effects for exceptional Na^(+)ion storage and diffusion performance at wide-temperatures environment.
基金financially supported by Guangdong Major Project of Basic Research(No.2023B0303000002)Shenzhen Fundamental Research Programs(No.JCYJ20241202125404007)+1 种基金Shenzhen Key Laboratory of Advanced Energy Storage(No.ZDSYS20220401141000001)National Natural Science Foundation of China(No.52263016,22265007)。
文摘Aqueous zinc-ion batteries(AZIBs)hold great promise for next-generation energy storage but face challenges such as Zn dendrite growth,side reactions,and limited performance at low temperatures.Here,we propose an electrolyte design strategy that reconstructs the hydrogenbond network through the synergistic effect of glycerol(GL)and methylsulfonamide(MSA),enabling the formation of a(100)-oriented Zn anode.This design significantly broadens the operating current and temperature windows of AZIBs.As a result,Zn||Zn symmetric cells exhibit remarkable cycling stability,achieving 4,000 h at 1 mA cm^(-2)and 600 h at 40 mA cm^(-2)(both at 1 mAh cm^(-2)capacity);even at-20℃,Zn||Zn symmetric cells deliver ultra-stable cycling for over 5,400 h.Furthermore,Zn||VO_(2)full cells retain 77.3%of their capacity after 2,000 cycles at 30°C with a current density of 0.5 A g^(-1)and 85.4%capacity retention after 2,000 cycles at-20°C and 0.25 A g^(-1).These results demonstrate a robust pathway for enhancing the practicality and low-temperature adaptability of AZIBs.
