The octahedral tunnel-like three-dimensional(3D)structure of V_(2)O_(3)enables fast metal ion(de)intercalation and high capacity in aqueous zinc-ion batteries(ZIBs),but suffers from phase transition-induced structural...The octahedral tunnel-like three-dimensional(3D)structure of V_(2)O_(3)enables fast metal ion(de)intercalation and high capacity in aqueous zinc-ion batteries(ZIBs),but suffers from phase transition-induced structural degradation and capacity fading.Herein,we demonstrate that the undesirable phase transition of V_(2)O_(3)can be effectively suppressed through a new La^(3+)doping strategy and its implementation as a robust ZIBs cathode.The introduced La^(3+)ions not only can increase cell volume and expand ion channels of V_(2)O_(3)but also offer plentiful Zn^(2+)storage sites and promote the transport of Zn^(2+)ions and electrons.In particular,the doping of La^(3+)maintains the octahedral tunnel structure of V_(2)O_(3)and prevents its phase transition during(dis)charge,which improves the cycle stability of the V_(2)O_(3)cathode in ZIBs.By virtue of the above favorable factors,La-doped V_(2)O_(3)electrode presents an impressive discharge capacity of632.1 m Ah g^(-1)at 0.1 A g^(-1)after 100 cycles with a capacity retention up to 93.1%.Even at 10 A g^(-1),its discharge capacity remains at 342.7 mAh g^(-1)after 1000 cycles with a capacity attenuation of solely0.0069%per cycle.This work establishes rare-earth cation doping as a universal paradigm to reconcile structural stability and multi-electron redox activity in high-capacity battery electrodes.展开更多
Aqueous sodium-ion batteries(ASIBs)have attracted great attention in aqueous batteries due to their merit of high safety.However,the constrained work potential and insufficient chemical stability of anode materials in...Aqueous sodium-ion batteries(ASIBs)have attracted great attention in aqueous batteries due to their merit of high safety.However,the constrained work potential and insufficient chemical stability of anode materials in aqueous electro-lytes hinder the large-scale application of ASIBs.Sodium titanium phosphate,NaTi_(2)(PO_(4))_(3)(NTP),is considered one of the most promising anode materials for ASIBs due to its excellent electrochemical performance and tunable structure.Recently,great achievements have been made in the development of NTP,however,a comprehensive review of existing studies is still lacking.This article firstly introduces the basic properties of NTP and analyzes the existing challenges.Subsequently,it will provide a comprehensive overview of the key strategies related to the design and modification of NTP materials with optimized electrochemical performance.Finally,based on the current research status and practical needs,suggestions,and future perspectives for advancing NTP in practical applications of ASIBs are presented.This review aims to guide the future research trajectory from basic material innovation to industrial applications,thus promoting the large-scale commercializa-tion of ASIBs.展开更多
Aqueous zinc-ion batteries have emerged as highly promising energy storage devices due to their high theoretical capacity,low cost,and high safety.However,they still suffer from dendrite growth and parasitic side reac...Aqueous zinc-ion batteries have emerged as highly promising energy storage devices due to their high theoretical capacity,low cost,and high safety.However,they still suffer from dendrite growth and parasitic side reactions caused by reactive aqueous electrolytes,which not only compromise reversibility but may also lead to internal short circuits,severely limiting practical applications.Herein,inulin(INU),a hydroxyl-rich polysaccharide,is proposed as a multifunctional electrolyte additive.Experimental and density functional theory calculations reveal that INU molecules effectively disrupt the original hydrogen-bond network,facilitating Zn^(2+)desolvation and rapid migration,thereby effectively resisting hydrogen evolution reaction,Zn corrosion,and by-products formation.Additionally,INU preferentially adsorbs on the Zn(002)crystal plane,forming a hydrophobic protective layer and guiding uniform Zn^(2+)deposition,thus inhibiting random dendritic growth.The presence of INU also effectively retards the dissolution process of V_(2)O_(5).As a result,the Zn‖Zn symmetric cell assembled with INU-3 electrolyte achieves an extended cycling life of 2400 h at a current density of 0.5 mA cm^(-2) and an areal capacity of0.5 mAh m^(-2).Furthermore,the Zn‖V_(2)O_(5) full cell exhibits a high capacity of 386.0 mAh g^(-1) at0.5 A g^(-1) and a high capacity retention of 55.26%at 8 A g^(-1).The full cell maintains remarkable capacity retention of 73%after 500 cycles at 1 A g^(-1) and 91%after 1000 cycles at 3 A g^(-1).This work inspires the study of electrolyte additives for aqueous zinc-ion batteries.展开更多
The formation of Zn dendrites and the occurrence of the hydrogen evolution reaction(HER)at Zn anodes represent two major obstacles that significantly impede the widespread commercialization of aqueous Zn-ion batteries...The formation of Zn dendrites and the occurrence of the hydrogen evolution reaction(HER)at Zn anodes represent two major obstacles that significantly impede the widespread commercialization of aqueous Zn-ion batteries.In this work,we propose sorbitan oleate(Span 80)as a novel amphiphilic electrolyte additive for 2 mol/L ZnSO_(4),demonstrating multifunctional performance.The unique ultra-long hydrophobic carbon chains of Span 80 effectively reduce free water molecules at the Zn anode-electrolyte interface,forming a robust hydrophobic interfacial layer that significantly suppresses HER and corrosion reactions.Simultaneously,carbon chains can enhance the desolvation effect of[Zn(H_(2)O)_(6)]^(2+),leading to improve rate performance.Additionally,the hydrophilic sorbitan groups in Span 80 selectively adsorb onto active sites of the Zn anode,promoting uniform Zn^(2+)deposition and suppressing dendrite growth.The optimized Zn||Zn symmetric cell exhibits outstanding cycling stability,sustaining reversible plating/stripping for 570 h at 50 mA/cm^(2) and the Zn||V_(2)O_(5) full cell retains exceptional stability over 2000 cycles at 1 A/g.Our work presents a promising strategy for suppressing interfacial side reactions by constructing a hydrophobic protective layer through the use of ultra-long carbon chain surfactants.This approach offers new insights into enhancing the performance of aqueous Zn-ion batteries.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
MnO_(2) stands out among cathode materials for aqueous zinc-ion batteries(AZIBs)high capacity and voltage,it has poor stability and slow Zn^(2+) kinetics.Herein,we propose a dual-regulation strategy integrating copper...MnO_(2) stands out among cathode materials for aqueous zinc-ion batteries(AZIBs)high capacity and voltage,it has poor stability and slow Zn^(2+) kinetics.Herein,we propose a dual-regulation strategy integrating copper doping and carbon-based confinement.Residual carbon(RC),derived from acid-washed coal gasification fine slag(CGFS),serves as a conductive and porous framework for the directional growth of Cu-doped MnO_(2) nanowires(CMO@RC).The synergistic modulation of Cu-induced electronic structure tuning and carbon confinement induced mechanical/electrical stabilization significantly enhances Zn^(2+) transport and electrochemical performance.CMO@RC achieves a high capacity of 563 mA·h·g^(−1) at 0.1 A·g^(−1) and maintains 106%after 1000 cycles at 1 A·g^(−1).Kinetic analyses confirm the dual-path Zn^(2+) diffusion and accelerated reaction kinetics,while DFT calculations reveal that Cu doping enhances Mn 3d orbital hybridization and electron interaction with carbon,elevating the density of states near the Fermi level and reducing charge transfer barriers.Furthermore,pouch cell testing demonstrates outstanding flexibility and mechanical resilience.This study provides a cost-effective and scalable strategy for high-performance AZIBs,leveraging both experimental and theoretical validations.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 metal batteries(AZMBs)are promising candidates for next-generation energy storage,but their commercialization is hindered by zinc anode challenges,notably parasitic reactions and dendrite growth.Herein,we...Aqueous zinc metal batteries(AZMBs)are promising candidates for next-generation energy storage,but their commercialization is hindered by zinc anode challenges,notably parasitic reactions and dendrite growth.Herein,we present a biodegradable biomass-derived protective layer,primarily composed of curcumin,as a zincophilic interface for AZMBs.The curcumin-based layer,fabricated via a homogeneous solution process,exhibits strong adhesion,uniform coverage,and robust mechanical integrity.Rich polar functional groups in curcumin facilitate homogeneous Zn~(2+)flux and suppress side reactions.The curcumin-based layer shows a favorable affinity for zinc trifluoromethanesulfonate(Zn(OTf)_(2))electrolyte,which is the representative of organic zinc salts,enabling optimal thickness for both protection and ion transport.The protected Zn anodes demonstrate an extended lifespan of 2500 h in symmetrical cells and a high Coulombic efficiency of 99.15%.Furthermore,Zn(OTf)_(2)-based system typically exhibits poor stability at high current densities.Fortunately,the lifespan of symmetrical cells was extended by 40-fold at the high current density.When paired with an Na V_(3)O_(8)·1.5H_(2)O(NVO)cathode,the system achieves 86.5%capacity retention after 3000 cycles at a large specific current density of 10 A g^(-1).These results underscore the efficacy of the curcumin-based protective layer in enhancing the reversibility and stability of metal electrodes,specifically relieving the instability of Zn(OTf)_(2)-based systems at high current densities,advancing its commercial viability.展开更多
Driven by the burgeoning demand for wearable electronics,the development of inherently safe,mechanically compliant,and high-energy–density power sources has become imperative.Flexible aqueous Zn ions batteries(FAZIBs...Driven by the burgeoning demand for wearable electronics,the development of inherently safe,mechanically compliant,and high-energy–density power sources has become imperative.Flexible aqueous Zn ions batteries(FAZIBs)are hampered by Zn dendrite formation and hydrogen evolution,underscoring the urgent need for highly stable and novel flexible energy-storage devices.Although flexible aqueous cobalt-ion batteries(FACIBs)employing cobalt-salt aqueous electrolytes exhibit high theoretical capacity,they suffer from two limitations:the rapid dissolution of cathode active substances in the aqueous electrolyte and the risk of liquid electrolyte leakage under mechanical deformation.Here,we report the first realization of an ultra-stable,quasi-solid-state and mechanically FACIBs.Polyacrylamide(PAM)containing CoSO_(4) serves as the quasi-solid electrolyte,while cobalt hexacyanoferrate(CoHCF)functions as the cathode active material,and metallic cobalt foil as the flexible anode.This configuration simultaneously eliminates electrolyte leakage and suppresses the dissolution of CoHCF due to the common-ion effect of Co^(2+).Consequently,the fabricated FACIBs exhibit extraordinary cycling durability and remarkable mechanical robustness(95.9%retention after 500 bending cycles).Thus,this work provides a new way for designing ultra-stable energy storage devices for wearable electronics.展开更多
Aqueous zinc-ion batteries(AZIBs)suffer from poor electrolyte/anode interfacial stability and severe performance degradation under low-temperature conditions.To address these issues,this study proposes natural okra po...Aqueous zinc-ion batteries(AZIBs)suffer from poor electrolyte/anode interfacial stability and severe performance degradation under low-temperature conditions.To address these issues,this study proposes natural okra polysaccharides(OPs)as an electrolyte additive for interfacial engineering,OPs,rich in polar functional groups,preferentially adsorb onto the Zn/electrolyte interface via strong dipole interactions,forming a robust protective layer.This layer promotes uniform Zn deposition,suppresses side reactions and corrosion,and enhances the hydrogen-bond network of the electrolyte,thereby reducing interfacial water activity and lowering the freezing point.As a result,the low-temperature stability and electrochemical reversibility of AZIBs are significantly improved.Zn‖Zn symmetric cells incorporating OPs exhibit exceptional cycling stability,maintaining reversible zinc plating/stripping for over 5000 h at 2 mA cm^(-2) and 1 mAh cm^(-2) and sustaining stable operation at-10℃for 1600 h under 1 mA cm^(-2)and 0.5 mAh cm^(-2),as well as for 300 h under 10 mA cm^(-2) and 10 mAh cm^(-2).Furthermore,full cells employing V_(2)O_(5) cathodes retain 83%of their capacity after 1000 cycles,confirming the practical applicability of OPs as a functio nal electrolyte additive.This work demonstrates the significant potential of OPs to overcome key limitations of AZIBs,particularly for low-temperature operation,offering a sustainable and cost-effective strategy for next-generation energy storage.展开更多
Aqueous alkali metal-ion batteries(AAMIBs)have been recognized as emerging electrochemical energy storage technologies for grid-scale applications owning to their intrinsic safety,cost-effectiveness,and environmental ...Aqueous alkali metal-ion batteries(AAMIBs)have been recognized as emerging electrochemical energy storage technologies for grid-scale applications owning to their intrinsic safety,cost-effectiveness,and environmental sustainability.However,the practical application of AAMIBs is still severely constrained by the tendency of aqueous electrolytes to freeze at low temperatures and decompose at high temperatures,limiting their operational temperature range.Considering the urgent need for energy systems with higher adaptability and resilience at various application scenarios,designing novel electrolytes via structure modulation has increasingly emerged as a feasible and economical strategy for the performance optimization of wide-temperature AAMIBs.In this review,the latest advancement of wide-temperature electrolytes for AAMIBs is systematically and comprehensively summarized.Specifically,the key challenges,failure mechanisms,correlations between hydrogen bond behaviors and physicochemical properties,and thermodynamic and kinetic interpretations in aqueous electrolytes are discussed firstly.Additionally,we offer forward-looking insights and innovative design principles for developing aqueous electrolytes capable of operating across a broad temperature range.This review is expected to provide some guidance and reference for the rational design and regulation of widetemperature electrolytes for AAMIBs and promote their future development.展开更多
Aqueous zinc-ion batteries(AZIBs)are currently confronted with the challenge of achieving long-term cyclic stability under high current densities.This issue is primarily attributed to the excessive growth of dendrites...Aqueous zinc-ion batteries(AZIBs)are currently confronted with the challenge of achieving long-term cyclic stability under high current densities.This issue is primarily attributed to the excessive growth of dendrites and the occurrence of significant side reactions.Herein,sucralose(SCL),as an electrolyte additive,has been used to promote the exposure of the Zn(002)texture.The introduction of SCL can adjust the Zn~(2+)nucleation and diffusion along different crystal facets,promoting the exposure of the Zn(002)texture.By substituting water molecules in the[Zn(H_(2)O)_(6)]~(2+),SCL reconfigures the hydrogen bond network in the electrolyte,reconstructing the solvation structure and suppressing the hydrogen evolution reaction.Consequently,the Zn//Zn symmetric battery exhibits long-term cycling stability of over 4900 h at 1 mA cm^(-2)-1 mAh cm^(-2).Even at a harsh condition of 30 mA cm^(-2)-30 mAh cm^(-2)(DOD=73.3%),it can stably cycle for 171 h.The CE of the Zn//Cu half battery reaches 99.61% at 0.2 mA cm^(-2)with 0.2 mAh cm^(-2).Employing the optimized electrolyte,after 500 cycles,a high specific capacity of 420 mAh g^(-1)can be retained for the NH_4V_4O_(10)//Zn full battery at 500 mA g^(-1),corresponding to a capacity retention of 90.7%.展开更多
Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density...Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density.However,their practical commercialization is hindered by critical challenges on the anode side,including dendrite growth and parasitic reactions at the anode/electrolyte interface.Recent studies highlight that rational electrolyte structure engineering offers an effective route to mitigate these issues and strengthen the electrochemical performance of the zinc metal anode.In this review,we systematically summarize state-of-the-art strategies for electrolyte optimization,with a particular focus on the zinc salts regulation,electrolyte additives,and the construction of novel electrolytes,while elucidating the underlying design principles.We further discuss the key structure–property relationships governing electrolyte behavior to provide guidance for the development of next-generation electrolytes.Finally,future perspectives on advanced electrolyte design are proposed.This review aims to serve as a comprehensive reference for researchers exploring high-performance electrolyte engineering in AZIBs.展开更多
Aqueous zinc metal batteries(AZMBs)face significant challenges in achieving reversibility and cycling stability,primarily due to hydrogen evolution reactions(HER)and zinc dendrite growth.In this study,by employing car...Aqueous zinc metal batteries(AZMBs)face significant challenges in achieving reversibility and cycling stability,primarily due to hydrogen evolution reactions(HER)and zinc dendrite growth.In this study,by employing carefully designed cells that approximate the structural characteristics of practical batteries,we revisit this widely held view through in-operando X-ray radiography to examine zinc dendrite formation and HER under nearpractical operating conditions.While conventional understanding emphasizes the severity of these processes,our findings suggest that zinc dendrites and HER are noticeably less pronounced in dense,real-operation configurations compared to modified cells,possibly due to a more uniform electric field and the suppression of triple-phase boundaries.This study indicates that other components,such as degradation at the cathode current collector interface and configuration mismatches within the full cell,may also represent important barriers to the practical application of AZMBs,particularly during the early stages of electrodeposition.展开更多
Vanadium-based materials have emerged as promising cathode candidates for aqueous zinc-ion batteries(AZIBs)due to their multivalent redox characteristics and diverse crystal structures,which enable high energy storage...Vanadium-based materials have emerged as promising cathode candidates for aqueous zinc-ion batteries(AZIBs)due to their multivalent redox characteristics and diverse crystal structures,which enable high energy storage capacity.Nevertheless,practical applications are hindered by several critical challenges,including vanadium species dissolution,side-product formation,sluggish Zn^(2+)diffusion kinetics,and low electrical conductivity.Organic functionalization,benefiting from its structural tunability and abundant functional groups,has been proven to be an effective strategy for enhancing the electrochemical performance of vanadium-based cathodes.This review systematically summarizes recent advances in organic-functionalized vanadium-based cathodes.First,the energy storage mechanism of vanadiumbased cathodes and the fundamental properties of organic compounds relevant to cathode optimization are outlined.Then,the functions of organic compounds are comprehensively analyzed from four key perspectives:capacity improvement,conductivity enhancement,Zn^(2+)diffusion kinetics optimization,and cycling stability promotion.Furthermore,the specific electrochemical performance modulation effects and practical application examples of this strategy are discussed in detail.Finally,current limitations and challenges in this field are highlighted,and corresponding solutions and future research directions are proposed,offering theoretical guidance and insights for the development of high-performance vanadium-based cathodes for AZIBs.展开更多
Layered double hydroxides(LDHs)hold great promise as cathode materials for aqueous zinc-ion batteries(AZIBs).Nevertheless,they also face challenges of sluggish kinetics and rapid capacity loss.Herein,a conformational ...Layered double hydroxides(LDHs)hold great promise as cathode materials for aqueous zinc-ion batteries(AZIBs).Nevertheless,they also face challenges of sluggish kinetics and rapid capacity loss.Herein,a conformational entropy regulation strategy has been applied to surmount the shortcomings.A medium-entropy iron-based metal organic framework(MIL-88)derived NiCoFeInZnV-based layered double hydroxide with carbon loaded(ME-NiCoFeInZnV-LDH/C)has been first proposed and prepared with a designed method.The increased entropy optimizes electron conductivity and alleviates structure alteration and diffusion barrier during interactions with charge carriers,due to electron-induced effect and“cocktail”effect.Moreover,the nanosheet assembled hollow prismatic structures could homogenize flux distribution and electric field distribution.Therefore,the electrochemical kinetics,crystal structure stability,and activity could be dramatically improved.Leveraging the advantages of structure and composition regulation,Zn||ME-NiCoFeInZnV-LDH/C zinc battery delivers high specific capacities,rate performance,and cycling stability.This work proposes a novel and feasible medium-entropy strategy to prepare a high-performance cathode for advanced AZIBs,which is of prominent significance for the development of charge storage devices.展开更多
Hydrogel microcapsules are powerful microreactor vessels that have attracted widespread attention and research.Among the various methods for their generation,the aqueous two-phase system(ATPS)is by far the most straig...Hydrogel microcapsules are powerful microreactor vessels that have attracted widespread attention and research.Among the various methods for their generation,the aqueous two-phase system(ATPS)is by far the most straightforward approach.However,the high viscosity of ATPS solutions significantly limits the generation throughput of hydrogel microcapsule.In this study,we developed a novel high-throughput approach for generating hydrogel microcapsules using a microfluidic bubble-triggering strategy.By integrating constant-pressure air flow with droplet microfluidics devices,we efficiently manipulated the formation of ATPS droplet through bubble-induced Rayleigh-Plateau instability,enabling the production of uniform,monodisperse microcapsules.Additionally,the droplet generation frequency in the bubble-triggering method exceeded 36 kHz.We further demonstrated the encapsulation of genetically engineered Escherichia coli strains,which acted as biosensors for arsenic ions and caprolactam,highlighting the potential of these microcapsules for biosensing applications.This advancement in hydrogel microcapsule generation offers promising implications for scalable applications in biosensing,organoid culture,and high-throughput screening.展开更多
Aqueous zinc-ion batteries(AZIBs) have advantages including low economic cost and high safety.Nevertheless,the serious hydrogen evolution reactions(HER) and rampant growth of Zn dendrite hinder their further developme...Aqueous zinc-ion batteries(AZIBs) have advantages including low economic cost and high safety.Nevertheless,the serious hydrogen evolution reactions(HER) and rampant growth of Zn dendrite hinder their further development.Herein,potassium acetate(KAc) additive with cation/anion synergy effect is added into the ZnSO_(4) electrolyte to effectively promote the oriented uniform Zn deposition and suppress side reactions.According to density functional theory calculation and experimental results,CH_(3)COO^(-)(Ac^(-))anions are capable of forming stronger hydrogen bonds with H_(2)O molecules,leading to an expanded electrochemical stability window,reduced the reactivity of H_(2)O,and hence suppressing HER.Meanwhile,Ac-anions can also preferentially adsorb onto the Zn anode,promoting dense deposition towards the(100) crystal plane.Besides,dissociated K^(+) ions serve as electrostatic shielding cations,which significantly promote uniform Zn deposition and prevent dendrite formation.Thus,the Zn||Zn symmetric cell demonstrates an impressive cycle lifespan of 3000 h at 1.0 m A/cm^(2).Furthermore,the Zn||MnO_(2) full battery exhibits superior stability with a capacity retention of 86.95 % at 2.0 A/g after 4000 cycles.Therefore,the cation/anion synergy effect in KAc additive offers a viable solution to address HER and hinder dendrite growth at the interface of Zn anodes.展开更多
Aqueous ammonium-ion batteries(AAIBs)have emerged as a promising candidate for grid-scale energy stor-age owing to their intrinsic safety(e.g.,dendrite-free and nonflammable),environmental friendliness,and potential f...Aqueous ammonium-ion batteries(AAIBs)have emerged as a promising candidate for grid-scale energy stor-age owing to their intrinsic safety(e.g.,dendrite-free and nonflammable),environmental friendliness,and potential for fast charge/discharge capability.Extensive research has been conducted in recent years to explore high-performance ammonium-ion storage materials and the associated electrochemistry to advance the commercialization of AAIBs.Therefore,it is necessary to review the progress in ammonium-ion storage materials and related electrochemical theories to guide further research on AAIBs.Herein,we systematically summarize the advanced electrode materials for AAIBs by introducing the physicochemical characteristics and ammonium-ion storage behaviors of various electrode materials,such as Prussian blue analogs,organic polymers,and metal oxides,discussing feasible material-design strategies to enhance their ammonium-ion storage performance,and outlining the future development prospects of AAIBs.This review aims to provide valuable insights into the design of advanced electrode materials for high-performance AAIBs.展开更多
The development of aqueous zinc-ion batteries is crucial for advancing sustainable energy storage technologies.However,their widespread application is hindered by Zn corrosion and uncontrolled Zn dendrite growth.One p...The development of aqueous zinc-ion batteries is crucial for advancing sustainable energy storage technologies.However,their widespread application is hindered by Zn corrosion and uncontrolled Zn dendrite growth.One promising approach involves creating a functional organic-inorganic interface on the Zn surface.Traditional binders,such as polyvinylidene fluoride(PVDF),fail to regulate water activity and ion migration,limiting the effectiveness of the interface.Herein,we introduce an aqueous dual ionic/electronic conducting binder,poly(3,4-ethylenedioxythiophene):polystyrene sulfonate(PEDOT:PSS),to build a water-scarce,Zn^(2+)-enriched interface.Our findings demonstrate that PEDOT:PSS not only facilitates uniform distribution of inorganic fillers,forming a cohesive and compact interface,but also significantly enhances mechanical integrity.Additionally,the sulfonate groups within the binder matrix disrupt the hydrogen bond network of water molecules,reducing water activity and lowering the desolvation energy barrier of Zn(H_(2)O)_(6)^(2+)clusters.Therefore,the transference number of Zn^(2+)is elevated to 0.81(compared to 0.61 with PVDF),mitigating undesirable side reactions and enabling dendrite-less Zn deposition.Consequently,symmetrical Zn||Zn cells with PEDOT:PSS binder demonstrate a lifetime with 4.2 times longer than those with PVDF.This work underscores the critical role of binder chemistry in stabilizing metal anodes for aqueous batteries.展开更多
基金financially supported by the National Natural Science Foundation of China(No.51962027,and 52262039)the Fundamental Research Funds for Inner Mongolia University of Science&Technology(No.2024QNJS071,2023QNJS052 and 2024QNJS064)+2 种基金the Program for Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region(No.NJYT24002)the Central Guidance Fund for Local Scientific and Technological Development(2024ZY0012)the Ordos Higher Education Institutions Scientific Research Innovation Project(KYLJ25Z004)。
文摘The octahedral tunnel-like three-dimensional(3D)structure of V_(2)O_(3)enables fast metal ion(de)intercalation and high capacity in aqueous zinc-ion batteries(ZIBs),but suffers from phase transition-induced structural degradation and capacity fading.Herein,we demonstrate that the undesirable phase transition of V_(2)O_(3)can be effectively suppressed through a new La^(3+)doping strategy and its implementation as a robust ZIBs cathode.The introduced La^(3+)ions not only can increase cell volume and expand ion channels of V_(2)O_(3)but also offer plentiful Zn^(2+)storage sites and promote the transport of Zn^(2+)ions and electrons.In particular,the doping of La^(3+)maintains the octahedral tunnel structure of V_(2)O_(3)and prevents its phase transition during(dis)charge,which improves the cycle stability of the V_(2)O_(3)cathode in ZIBs.By virtue of the above favorable factors,La-doped V_(2)O_(3)electrode presents an impressive discharge capacity of632.1 m Ah g^(-1)at 0.1 A g^(-1)after 100 cycles with a capacity retention up to 93.1%.Even at 10 A g^(-1),its discharge capacity remains at 342.7 mAh g^(-1)after 1000 cycles with a capacity attenuation of solely0.0069%per cycle.This work establishes rare-earth cation doping as a universal paradigm to reconcile structural stability and multi-electron redox activity in high-capacity battery electrodes.
基金supported by the Natural Sci-ence Foundation of Fujian Province (No.2024J011210)the High-Level Talent Start-Up Foundation of Xiamen Institute of Technology (No.YKJ23017R)。
文摘Aqueous sodium-ion batteries(ASIBs)have attracted great attention in aqueous batteries due to their merit of high safety.However,the constrained work potential and insufficient chemical stability of anode materials in aqueous electro-lytes hinder the large-scale application of ASIBs.Sodium titanium phosphate,NaTi_(2)(PO_(4))_(3)(NTP),is considered one of the most promising anode materials for ASIBs due to its excellent electrochemical performance and tunable structure.Recently,great achievements have been made in the development of NTP,however,a comprehensive review of existing studies is still lacking.This article firstly introduces the basic properties of NTP and analyzes the existing challenges.Subsequently,it will provide a comprehensive overview of the key strategies related to the design and modification of NTP materials with optimized electrochemical performance.Finally,based on the current research status and practical needs,suggestions,and future perspectives for advancing NTP in practical applications of ASIBs are presented.This review aims to guide the future research trajectory from basic material innovation to industrial applications,thus promoting the large-scale commercializa-tion of ASIBs.
基金the financial support by the National Natural Science Foundation of China(No.52573221,U2330124,U20A2072,52072352,21875226)the Foundation for the Youth S&T Innovation Team of Sichuan Province(2020JDTD0035)+1 种基金the Scientific Research Funds for Central Universities(ZYGX2025XJ016)the Sichuan Science and Technology Program(2023ZYD0026)。
文摘Aqueous zinc-ion batteries have emerged as highly promising energy storage devices due to their high theoretical capacity,low cost,and high safety.However,they still suffer from dendrite growth and parasitic side reactions caused by reactive aqueous electrolytes,which not only compromise reversibility but may also lead to internal short circuits,severely limiting practical applications.Herein,inulin(INU),a hydroxyl-rich polysaccharide,is proposed as a multifunctional electrolyte additive.Experimental and density functional theory calculations reveal that INU molecules effectively disrupt the original hydrogen-bond network,facilitating Zn^(2+)desolvation and rapid migration,thereby effectively resisting hydrogen evolution reaction,Zn corrosion,and by-products formation.Additionally,INU preferentially adsorbs on the Zn(002)crystal plane,forming a hydrophobic protective layer and guiding uniform Zn^(2+)deposition,thus inhibiting random dendritic growth.The presence of INU also effectively retards the dissolution process of V_(2)O_(5).As a result,the Zn‖Zn symmetric cell assembled with INU-3 electrolyte achieves an extended cycling life of 2400 h at a current density of 0.5 mA cm^(-2) and an areal capacity of0.5 mAh m^(-2).Furthermore,the Zn‖V_(2)O_(5) full cell exhibits a high capacity of 386.0 mAh g^(-1) at0.5 A g^(-1) and a high capacity retention of 55.26%at 8 A g^(-1).The full cell maintains remarkable capacity retention of 73%after 500 cycles at 1 A g^(-1) and 91%after 1000 cycles at 3 A g^(-1).This work inspires the study of electrolyte additives for aqueous zinc-ion batteries.
基金supported by the financial support from the Guangdong Basic and Applied Basic Research Foundation(No.2023B1515120095)the National Natural Science Foundation of China(Nos.52471229 and 52171210)the Jilin Province Science and Technology Department Program(No.20240101004JJ).
文摘The formation of Zn dendrites and the occurrence of the hydrogen evolution reaction(HER)at Zn anodes represent two major obstacles that significantly impede the widespread commercialization of aqueous Zn-ion batteries.In this work,we propose sorbitan oleate(Span 80)as a novel amphiphilic electrolyte additive for 2 mol/L ZnSO_(4),demonstrating multifunctional performance.The unique ultra-long hydrophobic carbon chains of Span 80 effectively reduce free water molecules at the Zn anode-electrolyte interface,forming a robust hydrophobic interfacial layer that significantly suppresses HER and corrosion reactions.Simultaneously,carbon chains can enhance the desolvation effect of[Zn(H_(2)O)_(6)]^(2+),leading to improve rate performance.Additionally,the hydrophilic sorbitan groups in Span 80 selectively adsorb onto active sites of the Zn anode,promoting uniform Zn^(2+)deposition and suppressing dendrite growth.The optimized Zn||Zn symmetric cell exhibits outstanding cycling stability,sustaining reversible plating/stripping for 570 h at 50 mA/cm^(2) and the Zn||V_(2)O_(5) full cell retains exceptional stability over 2000 cycles at 1 A/g.Our work presents a promising strategy for suppressing interfacial side reactions by constructing a hydrophobic protective layer through the use of ultra-long carbon chain surfactants.This approach offers new insights into enhancing the performance of aqueous Zn-ion batteries.
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.
基金support from the Key projects of scientific research projects of universities in Anhui Province(2024AH050360).
文摘MnO_(2) stands out among cathode materials for aqueous zinc-ion batteries(AZIBs)high capacity and voltage,it has poor stability and slow Zn^(2+) kinetics.Herein,we propose a dual-regulation strategy integrating copper doping and carbon-based confinement.Residual carbon(RC),derived from acid-washed coal gasification fine slag(CGFS),serves as a conductive and porous framework for the directional growth of Cu-doped MnO_(2) nanowires(CMO@RC).The synergistic modulation of Cu-induced electronic structure tuning and carbon confinement induced mechanical/electrical stabilization significantly enhances Zn^(2+) transport and electrochemical performance.CMO@RC achieves a high capacity of 563 mA·h·g^(−1) at 0.1 A·g^(−1) and maintains 106%after 1000 cycles at 1 A·g^(−1).Kinetic analyses confirm the dual-path Zn^(2+) diffusion and accelerated reaction kinetics,while DFT calculations reveal that Cu doping enhances Mn 3d orbital hybridization and electron interaction with carbon,elevating the density of states near the Fermi level and reducing charge transfer barriers.Furthermore,pouch cell testing demonstrates outstanding flexibility and mechanical resilience.This study provides a cost-effective and scalable strategy for high-performance AZIBs,leveraging both experimental and theoretical validations.
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the financial support from Research Institute for Smart Energy at the Hong Kong Polytechnic University(Grant No.CDB2)the support of the Hong Kong PhD Fellowship Scheme(Grant No.PF21-65328)。
文摘Aqueous zinc metal batteries(AZMBs)are promising candidates for next-generation energy storage,but their commercialization is hindered by zinc anode challenges,notably parasitic reactions and dendrite growth.Herein,we present a biodegradable biomass-derived protective layer,primarily composed of curcumin,as a zincophilic interface for AZMBs.The curcumin-based layer,fabricated via a homogeneous solution process,exhibits strong adhesion,uniform coverage,and robust mechanical integrity.Rich polar functional groups in curcumin facilitate homogeneous Zn~(2+)flux and suppress side reactions.The curcumin-based layer shows a favorable affinity for zinc trifluoromethanesulfonate(Zn(OTf)_(2))electrolyte,which is the representative of organic zinc salts,enabling optimal thickness for both protection and ion transport.The protected Zn anodes demonstrate an extended lifespan of 2500 h in symmetrical cells and a high Coulombic efficiency of 99.15%.Furthermore,Zn(OTf)_(2)-based system typically exhibits poor stability at high current densities.Fortunately,the lifespan of symmetrical cells was extended by 40-fold at the high current density.When paired with an Na V_(3)O_(8)·1.5H_(2)O(NVO)cathode,the system achieves 86.5%capacity retention after 3000 cycles at a large specific current density of 10 A g^(-1).These results underscore the efficacy of the curcumin-based protective layer in enhancing the reversibility and stability of metal electrodes,specifically relieving the instability of Zn(OTf)_(2)-based systems at high current densities,advancing its commercial viability.
基金supported by the National Natural Science Foundation of China(52402040 and 52561160149)National Key R&D Program of China(2024YFE0109200)+7 种基金Fundamental Research Funds for the Central Universities(2024300440)Open Project(M37033)of National Laboratory of Solid State Microstructures,Nanjing UniversityGuangdong Basic and Applied Basic Research Foundation(2025A1515011098)Shenzhen Science and Technology Program(JCYJ20250604190115021)Key Research Project of Universities in Henan Province(25A430006)Henan Province University Students Innovation Training Project(202510479001)Funded by the Training Program for Young Backbone Teachers in Higher Education Institutions of Henan Province(Prof.Chaowei Li)Science and Technology Research Project of Henan Province(242102240076)。
文摘Driven by the burgeoning demand for wearable electronics,the development of inherently safe,mechanically compliant,and high-energy–density power sources has become imperative.Flexible aqueous Zn ions batteries(FAZIBs)are hampered by Zn dendrite formation and hydrogen evolution,underscoring the urgent need for highly stable and novel flexible energy-storage devices.Although flexible aqueous cobalt-ion batteries(FACIBs)employing cobalt-salt aqueous electrolytes exhibit high theoretical capacity,they suffer from two limitations:the rapid dissolution of cathode active substances in the aqueous electrolyte and the risk of liquid electrolyte leakage under mechanical deformation.Here,we report the first realization of an ultra-stable,quasi-solid-state and mechanically FACIBs.Polyacrylamide(PAM)containing CoSO_(4) serves as the quasi-solid electrolyte,while cobalt hexacyanoferrate(CoHCF)functions as the cathode active material,and metallic cobalt foil as the flexible anode.This configuration simultaneously eliminates electrolyte leakage and suppresses the dissolution of CoHCF due to the common-ion effect of Co^(2+).Consequently,the fabricated FACIBs exhibit extraordinary cycling durability and remarkable mechanical robustness(95.9%retention after 500 bending cycles).Thus,this work provides a new way for designing ultra-stable energy storage devices for wearable electronics.
基金supported by the National Natural Science Foundation of China(22265007)the Guangxi Science and Technology Plan Project(GuikeAD25069100)+1 种基金the Guangdong Major Project of Basic Research(No.2023B0303000002)the High Level of Special Funds(No.G03034K00)。
文摘Aqueous zinc-ion batteries(AZIBs)suffer from poor electrolyte/anode interfacial stability and severe performance degradation under low-temperature conditions.To address these issues,this study proposes natural okra polysaccharides(OPs)as an electrolyte additive for interfacial engineering,OPs,rich in polar functional groups,preferentially adsorb onto the Zn/electrolyte interface via strong dipole interactions,forming a robust protective layer.This layer promotes uniform Zn deposition,suppresses side reactions and corrosion,and enhances the hydrogen-bond network of the electrolyte,thereby reducing interfacial water activity and lowering the freezing point.As a result,the low-temperature stability and electrochemical reversibility of AZIBs are significantly improved.Zn‖Zn symmetric cells incorporating OPs exhibit exceptional cycling stability,maintaining reversible zinc plating/stripping for over 5000 h at 2 mA cm^(-2) and 1 mAh cm^(-2) and sustaining stable operation at-10℃for 1600 h under 1 mA cm^(-2)and 0.5 mAh cm^(-2),as well as for 300 h under 10 mA cm^(-2) and 10 mAh cm^(-2).Furthermore,full cells employing V_(2)O_(5) cathodes retain 83%of their capacity after 1000 cycles,confirming the practical applicability of OPs as a functio nal electrolyte additive.This work demonstrates the significant potential of OPs to overcome key limitations of AZIBs,particularly for low-temperature operation,offering a sustainable and cost-effective strategy for next-generation energy storage.
基金supported by the National Natural Science Foundation of China(52002297)National Key R&D Program of China(2022VFB2404800)+1 种基金Wuhan Yellow Crane Talents Program,China Postdoctoral Science Foundation(No.2024M752495)the Postdoctoral Fellowship Program of CPSF(No.GZB20230552).
文摘Aqueous alkali metal-ion batteries(AAMIBs)have been recognized as emerging electrochemical energy storage technologies for grid-scale applications owning to their intrinsic safety,cost-effectiveness,and environmental sustainability.However,the practical application of AAMIBs is still severely constrained by the tendency of aqueous electrolytes to freeze at low temperatures and decompose at high temperatures,limiting their operational temperature range.Considering the urgent need for energy systems with higher adaptability and resilience at various application scenarios,designing novel electrolytes via structure modulation has increasingly emerged as a feasible and economical strategy for the performance optimization of wide-temperature AAMIBs.In this review,the latest advancement of wide-temperature electrolytes for AAMIBs is systematically and comprehensively summarized.Specifically,the key challenges,failure mechanisms,correlations between hydrogen bond behaviors and physicochemical properties,and thermodynamic and kinetic interpretations in aqueous electrolytes are discussed firstly.Additionally,we offer forward-looking insights and innovative design principles for developing aqueous electrolytes capable of operating across a broad temperature range.This review is expected to provide some guidance and reference for the rational design and regulation of widetemperature electrolytes for AAMIBs and promote their future development.
基金supported by the Anhui Provincial Science and Technology Innovation Initiative(202423i08050051)the Anhui Provincial Natural Science Foundation(2408085MB029)+1 种基金the HFIPS Director’s Fund(YZJJGGZX202201)the Natural Science Foundation of Hebei Province of China(B2024402018)。
文摘Aqueous zinc-ion batteries(AZIBs)are currently confronted with the challenge of achieving long-term cyclic stability under high current densities.This issue is primarily attributed to the excessive growth of dendrites and the occurrence of significant side reactions.Herein,sucralose(SCL),as an electrolyte additive,has been used to promote the exposure of the Zn(002)texture.The introduction of SCL can adjust the Zn~(2+)nucleation and diffusion along different crystal facets,promoting the exposure of the Zn(002)texture.By substituting water molecules in the[Zn(H_(2)O)_(6)]~(2+),SCL reconfigures the hydrogen bond network in the electrolyte,reconstructing the solvation structure and suppressing the hydrogen evolution reaction.Consequently,the Zn//Zn symmetric battery exhibits long-term cycling stability of over 4900 h at 1 mA cm^(-2)-1 mAh cm^(-2).Even at a harsh condition of 30 mA cm^(-2)-30 mAh cm^(-2)(DOD=73.3%),it can stably cycle for 171 h.The CE of the Zn//Cu half battery reaches 99.61% at 0.2 mA cm^(-2)with 0.2 mAh cm^(-2).Employing the optimized electrolyte,after 500 cycles,a high specific capacity of 420 mAh g^(-1)can be retained for the NH_4V_4O_(10)//Zn full battery at 500 mA g^(-1),corresponding to a capacity retention of 90.7%.
基金supported by the Natural Science Foundation of China(Nos.52125202,52202100,and U24A2065)the Natural Science Foundation of Jiangsu Province(BK20243016)Fundamental Research Funds for the Central Universities,China Postdoctoral Science Foundation(No.2024T171166).
文摘Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density.However,their practical commercialization is hindered by critical challenges on the anode side,including dendrite growth and parasitic reactions at the anode/electrolyte interface.Recent studies highlight that rational electrolyte structure engineering offers an effective route to mitigate these issues and strengthen the electrochemical performance of the zinc metal anode.In this review,we systematically summarize state-of-the-art strategies for electrolyte optimization,with a particular focus on the zinc salts regulation,electrolyte additives,and the construction of novel electrolytes,while elucidating the underlying design principles.We further discuss the key structure–property relationships governing electrolyte behavior to provide guidance for the development of next-generation electrolytes.Finally,future perspectives on advanced electrolyte design are proposed.This review aims to serve as a comprehensive reference for researchers exploring high-performance electrolyte engineering in AZIBs.
基金the fundamental Research Funds for the central Universities(x2wjD2240360)for the funding supportMeanwhile,Engineering and Physical Sciences Research Council(EPSRC,EP/V027433/3)+2 种基金UK Research and Innovation(UKRI)under the UK government’s Horizon Europe funding(101077226,EP/Y008707/1)Faraday Institution(EP/S003053/1)Degradation project(FIRG001),Royal Society(IEC\NSFC\233361),QUB Agility Fund and Wright Technology and Research Centre(W-Tech,R5240MEE)Funding from UK aid from the UK Government through the Faraday Institution and the Transforming Energy Access Programme(Grant number FIRG050-Device engineering of Zn-based hybrid micro-flow batteries and by-product H2 collection for Emerging Economies)。
文摘Aqueous zinc metal batteries(AZMBs)face significant challenges in achieving reversibility and cycling stability,primarily due to hydrogen evolution reactions(HER)and zinc dendrite growth.In this study,by employing carefully designed cells that approximate the structural characteristics of practical batteries,we revisit this widely held view through in-operando X-ray radiography to examine zinc dendrite formation and HER under nearpractical operating conditions.While conventional understanding emphasizes the severity of these processes,our findings suggest that zinc dendrites and HER are noticeably less pronounced in dense,real-operation configurations compared to modified cells,possibly due to a more uniform electric field and the suppression of triple-phase boundaries.This study indicates that other components,such as degradation at the cathode current collector interface and configuration mismatches within the full cell,may also represent important barriers to the practical application of AZMBs,particularly during the early stages of electrodeposition.
基金financial support from the National Natural Science Foundation of China(No.21676036)the Natural Science Foundation of Chongqing(No.CSTB2023NSCQMSX0580)the Large-scale Equipment Sharing Fund of Chongqing University(No.202403150240 and 202503150091)。
文摘Vanadium-based materials have emerged as promising cathode candidates for aqueous zinc-ion batteries(AZIBs)due to their multivalent redox characteristics and diverse crystal structures,which enable high energy storage capacity.Nevertheless,practical applications are hindered by several critical challenges,including vanadium species dissolution,side-product formation,sluggish Zn^(2+)diffusion kinetics,and low electrical conductivity.Organic functionalization,benefiting from its structural tunability and abundant functional groups,has been proven to be an effective strategy for enhancing the electrochemical performance of vanadium-based cathodes.This review systematically summarizes recent advances in organic-functionalized vanadium-based cathodes.First,the energy storage mechanism of vanadiumbased cathodes and the fundamental properties of organic compounds relevant to cathode optimization are outlined.Then,the functions of organic compounds are comprehensively analyzed from four key perspectives:capacity improvement,conductivity enhancement,Zn^(2+)diffusion kinetics optimization,and cycling stability promotion.Furthermore,the specific electrochemical performance modulation effects and practical application examples of this strategy are discussed in detail.Finally,current limitations and challenges in this field are highlighted,and corresponding solutions and future research directions are proposed,offering theoretical guidance and insights for the development of high-performance vanadium-based cathodes for AZIBs.
基金the funding support from the National Natural Science Foundation of China(Grant No.52202217,52471222)the Natural Science Foundation of Jilin Province(Grant No.YDZJ202201ZYTS375).
文摘Layered double hydroxides(LDHs)hold great promise as cathode materials for aqueous zinc-ion batteries(AZIBs).Nevertheless,they also face challenges of sluggish kinetics and rapid capacity loss.Herein,a conformational entropy regulation strategy has been applied to surmount the shortcomings.A medium-entropy iron-based metal organic framework(MIL-88)derived NiCoFeInZnV-based layered double hydroxide with carbon loaded(ME-NiCoFeInZnV-LDH/C)has been first proposed and prepared with a designed method.The increased entropy optimizes electron conductivity and alleviates structure alteration and diffusion barrier during interactions with charge carriers,due to electron-induced effect and“cocktail”effect.Moreover,the nanosheet assembled hollow prismatic structures could homogenize flux distribution and electric field distribution.Therefore,the electrochemical kinetics,crystal structure stability,and activity could be dramatically improved.Leveraging the advantages of structure and composition regulation,Zn||ME-NiCoFeInZnV-LDH/C zinc battery delivers high specific capacities,rate performance,and cycling stability.This work proposes a novel and feasible medium-entropy strategy to prepare a high-performance cathode for advanced AZIBs,which is of prominent significance for the development of charge storage devices.
基金sponsored by the National Key R&D Program of China(no.2023YFB3208203)the National Natural Science Foundation of China(no.62374170)the Science and Technology Commission of Shanghai Municipality(no.23J21900200).
文摘Hydrogel microcapsules are powerful microreactor vessels that have attracted widespread attention and research.Among the various methods for their generation,the aqueous two-phase system(ATPS)is by far the most straightforward approach.However,the high viscosity of ATPS solutions significantly limits the generation throughput of hydrogel microcapsule.In this study,we developed a novel high-throughput approach for generating hydrogel microcapsules using a microfluidic bubble-triggering strategy.By integrating constant-pressure air flow with droplet microfluidics devices,we efficiently manipulated the formation of ATPS droplet through bubble-induced Rayleigh-Plateau instability,enabling the production of uniform,monodisperse microcapsules.Additionally,the droplet generation frequency in the bubble-triggering method exceeded 36 kHz.We further demonstrated the encapsulation of genetically engineered Escherichia coli strains,which acted as biosensors for arsenic ions and caprolactam,highlighting the potential of these microcapsules for biosensing applications.This advancement in hydrogel microcapsule generation offers promising implications for scalable applications in biosensing,organoid culture,and high-throughput screening.
基金financially supported by the National Natural Science Foundation of China (No.52372188)the 111 Project (No.D17007)2023 Introduction of studying abroad talent program。
文摘Aqueous zinc-ion batteries(AZIBs) have advantages including low economic cost and high safety.Nevertheless,the serious hydrogen evolution reactions(HER) and rampant growth of Zn dendrite hinder their further development.Herein,potassium acetate(KAc) additive with cation/anion synergy effect is added into the ZnSO_(4) electrolyte to effectively promote the oriented uniform Zn deposition and suppress side reactions.According to density functional theory calculation and experimental results,CH_(3)COO^(-)(Ac^(-))anions are capable of forming stronger hydrogen bonds with H_(2)O molecules,leading to an expanded electrochemical stability window,reduced the reactivity of H_(2)O,and hence suppressing HER.Meanwhile,Ac-anions can also preferentially adsorb onto the Zn anode,promoting dense deposition towards the(100) crystal plane.Besides,dissociated K^(+) ions serve as electrostatic shielding cations,which significantly promote uniform Zn deposition and prevent dendrite formation.Thus,the Zn||Zn symmetric cell demonstrates an impressive cycle lifespan of 3000 h at 1.0 m A/cm^(2).Furthermore,the Zn||MnO_(2) full battery exhibits superior stability with a capacity retention of 86.95 % at 2.0 A/g after 4000 cycles.Therefore,the cation/anion synergy effect in KAc additive offers a viable solution to address HER and hinder dendrite growth at the interface of Zn anodes.
基金Guangdong Basic and Applied Basic Research Foundation(Grant No.2023A1515012087)funded by Science and Technology Projects in Guangzhou(Grant No.2024A04J3267)the Fundamental Research Funds for the Central Universities(Grant No.21624411).
文摘Aqueous ammonium-ion batteries(AAIBs)have emerged as a promising candidate for grid-scale energy stor-age owing to their intrinsic safety(e.g.,dendrite-free and nonflammable),environmental friendliness,and potential for fast charge/discharge capability.Extensive research has been conducted in recent years to explore high-performance ammonium-ion storage materials and the associated electrochemistry to advance the commercialization of AAIBs.Therefore,it is necessary to review the progress in ammonium-ion storage materials and related electrochemical theories to guide further research on AAIBs.Herein,we systematically summarize the advanced electrode materials for AAIBs by introducing the physicochemical characteristics and ammonium-ion storage behaviors of various electrode materials,such as Prussian blue analogs,organic polymers,and metal oxides,discussing feasible material-design strategies to enhance their ammonium-ion storage performance,and outlining the future development prospects of AAIBs.This review aims to provide valuable insights into the design of advanced electrode materials for high-performance AAIBs.
基金supported by the National Natural Science Foundation of China(Grant No.22461142135,22479046)the Key Programs funded by Science and Technology Department of Shaanxi Provincial Government(Grant:No.2024GX-YBXM-336)+2 种基金the Xi’an Municipal Bureau of Science and Technology(Grant:No.2023JHGXRC-0097)the Yulin Science and Technology Bureau(Grant:No.2024-CXY-161)the Xi’an Beilin District Science and Technology and Industrial Information Bureau(Grant:No.GX2440)。
文摘The development of aqueous zinc-ion batteries is crucial for advancing sustainable energy storage technologies.However,their widespread application is hindered by Zn corrosion and uncontrolled Zn dendrite growth.One promising approach involves creating a functional organic-inorganic interface on the Zn surface.Traditional binders,such as polyvinylidene fluoride(PVDF),fail to regulate water activity and ion migration,limiting the effectiveness of the interface.Herein,we introduce an aqueous dual ionic/electronic conducting binder,poly(3,4-ethylenedioxythiophene):polystyrene sulfonate(PEDOT:PSS),to build a water-scarce,Zn^(2+)-enriched interface.Our findings demonstrate that PEDOT:PSS not only facilitates uniform distribution of inorganic fillers,forming a cohesive and compact interface,but also significantly enhances mechanical integrity.Additionally,the sulfonate groups within the binder matrix disrupt the hydrogen bond network of water molecules,reducing water activity and lowering the desolvation energy barrier of Zn(H_(2)O)_(6)^(2+)clusters.Therefore,the transference number of Zn^(2+)is elevated to 0.81(compared to 0.61 with PVDF),mitigating undesirable side reactions and enabling dendrite-less Zn deposition.Consequently,symmetrical Zn||Zn cells with PEDOT:PSS binder demonstrate a lifetime with 4.2 times longer than those with PVDF.This work underscores the critical role of binder chemistry in stabilizing metal anodes for aqueous batteries.
