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 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
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
Sodium-based dual-ion batteries(SDIBs)have been attracting increasing attention in recent years owing to their low cost,environmental benignancy,and high operating voltage.However,the sluggish ion kinetics of conventi...Sodium-based dual-ion batteries(SDIBs)have been attracting increasing attention in recent years owing to their low cost,environmental benignancy,and high operating voltage.However,the sluggish ion kinetics of conventional carbon anodes that cannot match the fast capacitive anion intercalation behavior of graphite cathodes constraints on improving power density of SDIBs.Herein,we present an ingenious carbon microdomain engineering strategy to fabricate high-performance carbon anode with ion-mediated high-activity nitrogen species and molecular-scale closed-pore architectures.Experimental characterizations and theoretical investigations demonstrate that Zn^(2+)-mediated structural engineering tailors oxidized nitrogen species,which proficiently accelerate the sodium-ion desolvation kinetics;meanwhile the acetate-mediated pore-forming process modulates closed pores,which synergistically afford abundant sodium storage sites for high plateau-region capacity.As a result,the optimized microdomain engineered carbon material(MEC_(3))tailored with the optimal amount of zinc acetate demonstrates an outstanding plateau-region capacity of 253 mAh g^(-1)even at 1 C,among the highest reported values.Consequently,the MEC_(3)||expanded graphite dual-ion battery exhibits an unprecedented cycling stability at high current rate,maintaining 80.6%capacity retention after 10,000 cycles at 10 C,among the best reports.This microdomain engineering strategy provides a new design principle for overcoming kinetic limitations of carbonaceous materials in plateau-dominated sodium storage systems.展开更多
Aqueous zinc(Zn)-ion batteries hold great promise as renewable energy storage system for carbon-neutral energy transition.However,Zn anodes suffer from poor Zn plating/stripping reversibility due to Zn dendrite growth...Aqueous zinc(Zn)-ion batteries hold great promise as renewable energy storage system for carbon-neutral energy transition.However,Zn anodes suffer from poor Zn plating/stripping reversibility due to Zn dendrite growth and side reactions.Existing Zn interfacial modification strategies based on single-component or homogeneous structure are insufficient to address these issues comprehensively.Herein,we rationally designed an organic-inorganic hybrid interfacial layer with rigid-to-soft graded structure for dendrite-free and stable Zn anodes.A liquid plasma-assisted oxidation technology is developed to rapidly construct a porous ZnO inner framework in situ.This ZnO layer offers high interfacial energy,mechanical robustness,and an open structure that facilitates ion transport while firmly anchoring a subsequently coated soft polymer layer.The resulting architecture presents a structurally graded and functionally complementary interface,enabling effective dendrite suppression,continuous Zn ion transport,and enhanced corrosion resistance.As a result,a long cycling stability of more than 6000 h can be achieved at 1 mA cm^(-2)for 1 mAh cm^(-2)in symmetric cells.When used as anodes for zinc-iodine full battery,the hybrid interlayer can effectively prevent the Zn anodes from the corrosion by polyiodine,enabling stable cycling and negligible capacity decay(~0.02‰per cycle)for over 10,000 cycles at 2.0 A g^(-1).This work demonstrates a promising interfacial design strategy and introduces a novel liquid plasma-assisted oxidation route for fabricating high-performance Zn anodes towards next-generation aqueous batteries.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
The electric double layer(EDL)at the electrochemical interface is crucial for ion transport,charge transfer,and surface reactions in aqueous rechargeable zinc batteries(ARZBs).However,Zn anodes routinely encounter per...The electric double layer(EDL)at the electrochemical interface is crucial for ion transport,charge transfer,and surface reactions in aqueous rechargeable zinc batteries(ARZBs).However,Zn anodes routinely encounter persistent dendrite growth and parasitic reactions,driven by the inhomogeneous charge distribution and water-dominated environment within the EDL.Compounding this,classical EDL theory,rooted in meanfield approximations,further fails to resolve molecular-scale interfacial dynamics under battery-operating conditions,limiting mechanistic insights.Herein,we established a multiscale theoretical calculation framework from single molecular characteristics to interfacial ion distribution,revealing the EDL’s structure and interactions between different ions and molecules,which helps us understand the parasitic processes in depth.Simulations demonstrate that water dipole and sulfate ion adsorption at the inner Helmholtz plane drives severe hydrogen evolution and by-product formation.Guided by these insights,we engineered a“water-poor and anion-expelled”EDL using 4,1’,6’-trichlorogalactosucrose(TGS)as an electrolyte additive.As a result,Zn||Zn symmetric cells with TGS exhibited stable cycling for over 4700 h under a current density of 1 mA cm^(−2),while NaV_(3)O_(8)·1.5H_(2)O-based full cells kept 90.4%of the initial specific capacity after 800 cycles at 5 A g^(−1).This work highlights the power of multiscale theoretical frameworks to unravel EDL complexities and guide high-performance ARZB design through integrated theory-experiment approaches.展开更多
Aqueous zinc ion batteries(AZIBs)are considered promising candidates owing to their inherent safety and low cost.However,the conventional glass fiber(GF)separator used in AZIBs suffers from poor physicochemical proper...Aqueous zinc ion batteries(AZIBs)are considered promising candidates owing to their inherent safety and low cost.However,the conventional glass fiber(GF)separator used in AZIBs suffers from poor physicochemical properties,leading to uncontrolled zinc(Zn)dendrite formation and undesirable side reactions.To address these limitations and enhance the electrochemical performance of AZIBs,a precisely designed functional separator is developed by incorporating UiO-66-(COOH)_(2)into a poly(vinylidene fluoride)(PVDF)framework(U-PVDF)via a direct in situ growth method.This approach enables uniform distribution of UiO-66-(COOH)_(2)both on the surface and within the PVDF backbone,without increasing separator thickness.Owing to the strong interaction between Zn^(2+)and the abundant carboxyl groups in UiO-66-(COOH)_(2),the U-PVDF separator regulates the Zn^(2+)solvation structure toward a contact ion pair-dominated structure by reducing coordinated water molecules,which effectively mitigates water-induced parasitic reactions and promotes compact Zn deposition.Consequently,a Zn/Zn symmetric cell employing the U-PVDF separator demonstrates superior cycling stability over 1500 cycles without internal short-circuiting at a current density of 6 mA cm^(−2)and an areal capacity of 2 mAh cm^(−2).Moreover,Zn/NaV_(3)O_(8)·xH_(2)O(NVO)cell with the U-PVDF separator exhibits markedly improved cyclability and rate performance compared with those using conventional GF separator.展开更多
The rapid expansion of the photovoltaic industry has generated heavily oxidized waste silicon(wSi),which hinders efficient recycling owing to its small particle size and uncontrolled surface oxidation.This study intro...The rapid expansion of the photovoltaic industry has generated heavily oxidized waste silicon(wSi),which hinders efficient recycling owing to its small particle size and uncontrolled surface oxidation.This study introduces a molten salt electrochemical strategy for converting photovoltaic wSi into NiSi_(2)-silicon nanorods(NiSi_(2)-SiNRs)as high-performance anode materials for lithium-ion batteries.A stable oxidized passivation layer is formed on the wSi surface via controlled oxidation,and further in situ generated highly active NiSi_(2) droplets.The molten salt electric field modulates the surface energy of silicon,while particle integration drives localized directional growth,enabling the self-assembly of NiSi_(2)-SiNRs composites.These NiSi_(2)-SiNRs anodes exhibit rapid ion transport and effective strain buffering.The high aspect ratio of SiNRs and the presence of retained NiSi_(2) facilitate both longitudinal and transverse Li^(+) diffusion.Owing to their robust structural design,the NiSi_(2)-SiNRs anode achieves an excellent initial Coulombic efficiency of 91.61%and retains 72.99%of its capacity after 800 cycles at 2 A·g^(−1).This study establishes a model system for investigating silicide/silicon interfaces in molten salt electrochemical synthesis and provides an effective strategy for upcycling photovoltaic wSi into high-performance lithium-ion battery anodes.展开更多
Halide perovskite materials have received considerable attention for solar cells,LEDs,lasers etc.owing to their controllable physicochemical properties and structural advantages.However,little research has focused on ...Halide perovskite materials have received considerable attention for solar cells,LEDs,lasers etc.owing to their controllable physicochemical properties and structural advantages.However,little research has focused on energy storage and conversion applications,such as use as anodes in lithium-ion batteries.In this paper,all-inorganic lead-free halide perovskite Cs_(3)Bi_(2)Cl_(9)powders were synthesized by the grinding method,and the lattice was successfully adjusted via introducing Mn^(2+).The characterization results show that Mn-ion substitution can cause local lattice distortion to restructure the lattice,which will cause a mixed arrangement of[BiCl_(6)]octahedra to improve the performance of the anode material.This new material can provide a feasible solution for solving the problem of low specific capacity anode materials caused by unstable crystal structures,and also indicates that such perovskites with unique crystal structures and lattice tunability have broad application prospects in lithium-ion batteries.展开更多
Sodium-ion batteries (SIBs) with organic electrodes are an emerging research direction due to the sustainability of organic materials based on elements like C,H,O,and sodium ions.Currently,organic electrode materials ...Sodium-ion batteries (SIBs) with organic electrodes are an emerging research direction due to the sustainability of organic materials based on elements like C,H,O,and sodium ions.Currently,organic electrode materials for SIBs are mainly used as cathodes because of their relatively high redox potentials(>1 V).Organic electrodes with low redox potential that can be used as anode are rare.Herein,a novel organic anode material (tetrasodium 1,4,5,8-naphthalenetetracarboxylate,Na_(4)TDC) has been developed with low redox potential (<0.7 V) and excellent cyclic stability.Its three-sodium storage mechanism was demonstrated with various in-situ/ex-situ spectroscopy and theoretical calculations,showing a high capacity of 208 mAh/g and an average decay rate of merely 0.022%per cycle.Moreover,the Na_(4)TDC-hard carbon composite can further acquire improved capacity and cycling stability for 1200 cycles even with a high mass loading of up to 20 mg cm^(-2).By pairing with a thick Na_(3)V_(2)(PO_(4))_(3)cathode (20.6 mg cm^(-2)),the as-fabricated full cell exhibited high operating voltage (2.8 V),excellent rate performance and cycling stability with a high capacity retention of 88.7% after 200 cycles,well highlighting the Na_(4)TDC anode material for SIBs.展开更多
With the increasing prevalence of lithium-ion batteries(LIBs)applications,the demand for high-capacity next-generation materials has also increased.SiO_(x)is currently considered a promising anode material due to its ...With the increasing prevalence of lithium-ion batteries(LIBs)applications,the demand for high-capacity next-generation materials has also increased.SiO_(x)is currently considered a promising anode material due to its exceptionally high capacity for LIBs.However,the significant volumetric changes of SiO_(x)during cycling and its initial Coulombic efficiency(ICE)complicate its use,whether alone or in combination with graphite materials.In this study,a three-dimensional conductive binder network with high electronic conductivity and robust elasticity for graphite/SiO_(x)blended anodes was proposed by chemically anchoring carbon nanotubes and carboxymethyl cellulose binders using tannic acid as a chemical cross-linker.In addition,a dehydrogenation-based prelithiation strategy employing lithium hydride was utilized to enhance the ICE of SiO_(x).The combination of these two strategies increased the CE of SiO_(x)from 74%to87%and effectively mitigated its volume expansion in the graphite/SiO_(x)blended electrode,resulting in an efficient electron-conductive binder network.This led to a remarkable capacity retention of 94%after30 cycles,even under challenging conditions,with a high capacity of 550 mA h g^(-1)and a current density of 4 mA cm^(-2).Furthermore,to validate the feasibility of utilizing prelithiated SiO_(x)anode materials and the conductive binder network in LIBs,a full cell incorporating these materials and a single-crystalline Ni-rich cathode was used.This cell demonstrated a~27.3%increase in discharge capacity of the first cycle(~185.7 mA h g^(-1))and exhibited a cycling stability of 300 cycles.Thus,this study reports a simple,feasible,and insightful method for designing high-performance LIB electrodes.展开更多
The replacement of non-aqueous organic electrolytes with solid-state electrolytes(SSEs)in solid-state lithium metal batteries(SLMBs)is considered a promising strategy to address the constraints of lithium-ion batterie...The replacement of non-aqueous organic electrolytes with solid-state electrolytes(SSEs)in solid-state lithium metal batteries(SLMBs)is considered a promising strategy to address the constraints of lithium-ion batteries,especially in terms of energy density and reliability.Nevertheless,few SLMBs can deliver the required cycling performance and long-term stability for practical use,primarily due to suboptimal interface properties.Given the diverse solidification pathways leading to different interface characteristics,it is crucial to pinpoint the source of interface deterioration and develop appropriate remedies.This review focuses on Li|SSE interface issues between lithium metal anode and SSE,discussing recent advancements in the understanding of(electro)chemistry,the impact of defects,and interface evolutions that vary among different SSE species.The state-ofthe-art strategies concerning modified SEI,artificial interlayer,surface architecture,and composite structure are summarized and delved into the internal relationships between interface characteristics and performance enhancements.The current challenges and opportunities in characterizing and modifying the Li|SSE interface are suggested as potential directions for achieving practical SLMBs.展开更多
To meet the demand for enhanced energy density and improved safety in batteries,anode-free aqueous zinc metal batteries(AF-AZMBs)have garnered significant research interest and attention.Compared with conventional aqu...To meet the demand for enhanced energy density and improved safety in batteries,anode-free aqueous zinc metal batteries(AF-AZMBs)have garnered significant research interest and attention.Compared with conventional aqueous Zn batteries,AF-AZMBs provide higher theoretical energy density,a more simplified structural design,and improved cost-effectiveness.However,AF-AZMBs are confronted with severe capacity degradation and lifespan reduction due to the absence of an excess zinc inventory.In recent years,extensive research efforts have been devoted to addressing these challenges,resulting in significant advancements.Therefore,there is highly warranted for a comprehensive discussion on AF-AZMBs.Herein,this review provides a thorough analysis and in-depth investigation of recent developments in AF-AZMBs from the perspectives of current collectors,electrolytes,and cathodes.Specifically,the working mechanisms and advantageous features of AF-AZMBs are summarized.The major scientific issues affecting capacity degradation and lifespan reduction are discussed,including inhomogeneous Zn deposition/stripping kinetics,unstable SEI layer,and irreversible cathode material loss.Furthermore,the corresponding strategies to address these issues are highlighted,such as anodic current collector design,electrolyte engineering,and cathodic modification.Finally,several promising directions are explored for the future advancement of AF-AZMBs,including developing high-performance Zn-rich cathodes,regulating solid-state electrolytes,and designing dual-electrode-free zinc-metal batteries.Additionally,exploring advanced characterization and analysis techniques and optimizing pouch cells under practical operating conditions are also mentioned,highlighting the urgent need for further research to address existing bottlenecks.展开更多
H_(2)O-induced side reactions and dendrite growth occurring at the Zn anode-electrolyte interface(AEI)limit the electrochemical performances of aqueous zinc ion batteries.Herein,methionine(Met)is introduced as an elec...H_(2)O-induced side reactions and dendrite growth occurring at the Zn anode-electrolyte interface(AEI)limit the electrochemical performances of aqueous zinc ion batteries.Herein,methionine(Met)is introduced as an electrolyte additive to solve the above issues by three aspects:Firstly,Met is anchored on Zn anode by amino/methylthio groups to form a H_(2)O-poor AEI,thus increasing the overpotential of hydrogen evolution reaction(HER);secondly,Met serves as a pH buffer to neutralize the HER generated OH-,thereby preventing the formation of by-products(e.g.Zn_(4)SO_(4)(OH)_(6)·xH_(2)O);thirdly,Zn^(2+) could be captured by carboxyl group of the anchored Met through electrostatic interaction,which promotes the dense and flat Zn deposition.Consequently,the Zn||Zn symmetric cell obtains a long cycle life of 3200 h at 1.0 mA cm^(-2),1.0 mAh cm^(-2),and 1400 h at 5.0 mA cm^(-2),5.0 mAh cm^(-2).Moreover,Zn||VO_(2) full cell exhibits a capacity retention of 91.0%after operating for 7000 cycles at 5.0 A g^(-1).This study offers a novel strategy for modulating the interface microenvironment of AEI via integrating the molecular adsorption,pH buffer,and Zn^(2+) capture strategies to design advanced industrial-oriented batteries.展开更多
Sodium metal has been widely studied in the field of batteries due to its high theoretical specific capacity(~1,166 m Ah/g),low redox potential(-2.71 V compared to standard hydrogen electrode),and lowcost advantages.H...Sodium metal has been widely studied in the field of batteries due to its high theoretical specific capacity(~1,166 m Ah/g),low redox potential(-2.71 V compared to standard hydrogen electrode),and lowcost advantages.However,problems such as unstable solid electrolyte interface(SEI),uncontrolled dendrite growth,and side reactions between solid-liquid interfaces have hindered the practical application of sodium metal anodes(SMAs).Currently,lots of strategies have been developed to achieve stabilized sodium metal anodes.Among these strategies,modified metal current collectors(MCCs)stand out due to their unique role in accommodating volumetric fluctuations with superior structure,lowering the energy barrier for sodium nucleation,and providing guided uniform sodium deposition.In this review,we first introduced three common metal-based current collectors applied to SMAs.Then,we summarized strategies to improve sodium deposition behavior by optimally engineering the surface of MCCs,including surface loading,surface structural design,and surface engineering for functional modification.We have followed the latest research progress and summarized surface optimization cases on different MCCs and their applications in battery systems.展开更多
Metal foils have emerged as one of the promising materials for anode-free batteries due to their high energy density and scalability in production.The unclear lithium plating/stripping kinetics of metal foil current c...Metal foils have emerged as one of the promising materials for anode-free batteries due to their high energy density and scalability in production.The unclear lithium plating/stripping kinetics of metal foil current collectors in anode-free batteries was addressed by using the non-destructive distribution of relaxation times(DRT)analysis to systematically investigate the lithium transport behavior of 14 metal foils and its correlation with electrochemical performance.By integrating energy-dispersive spectro scopy(EDS),cyclic voltammetry(CV),and galvanostatic testing,the exceptional properties of indium(In),tin(Sn),and silver(Ag)were revealed:the Li-In alloying reaction exhibits high reversibility,Li-Sn alloys demonstrate outstanding cycling stability,and the Li-Ag solid-solution mechanism provides an ideal lithium deposition interface on the silver substrate.The DRT separates the polarization internal resistance of lithium ions passing through the SEI layer(R_(sei),τ2)and the polarization internal resistance of lithium ions undergoing charge transfer reaction at the electrolyte/electrode interface(R_(ct),τ3)by decoupling the electrochemical impedance spectroscopy(EIS).For the first time,the correlation betweenτ2,τ3,and the cycle life/Coulombic efficiency of alloy/solid-solution metals was established,while non-alloy metals are not suitable for this method due to differences in lithium deposition mechanisms.This study not only illuminates the structure-property relationship governing the lithium kinetics of metal foil electrodes but also provides a novel non-destructive analytical strategy and theoretical guidance for the rational design of stable anodes in high-energy-density batteries,facilitating the efficient screening and optimization of anode-free battery.展开更多
Carbon materials are widely recognized as highly promising electrode materials for various energy storage system applications.Coal tar residues(CTR),as a type of carbon-rich solid waste with high value-added utilizati...Carbon materials are widely recognized as highly promising electrode materials for various energy storage system applications.Coal tar residues(CTR),as a type of carbon-rich solid waste with high value-added utilization,are crucially important for the development of a more sustainable world.In this study,we employed a straightforward direct carbonization method within the temperature range of 700-1000℃to convert the worthless solid waste CTR into economically valuable carbon materials as anodes for potassium-ion batteries(PIBs).The effect of carbonization temperature on the microstructure and the potassium ions storage properties of CTR-derived carbons(CTRCs)were systematically explored by structural and morphological characterization,alongside electrochemical performances assessment.Based on the co-regulation between the turbine layers,crystal structure,pore structure,functional groups,and electrical conductivity of CTR-derived carbon carbonized at 900℃(CTRC-900H),the electrode material with high reversible capacity of 265.6m Ah·g^(-1)at 50 m A·g^(-1),a desirable cycling stability with 93.8%capacity retention even after 100 cycles,and the remarkable rate performance for PIBs were obtained.Furthermore,cyclic voltammetry(CV)at different scan rates and galvanostatic intermittent titration technique(GITT)have been employed to explore the potassium ions storage mechanism and electrochemical kinetics of CTRCs.Results indicate that the electrode behavior is predominantly governed by surface-induced capacitive processes,particularly under high current densities,with the potassium storage mechanism characterized by an“adsorption-weak intercalation”mechanism.This work highlights the potential of CTR-based carbon as a promising electrode material category suitable for high-performance PIBs electrodes,while also provides valuable insights into the new avenues for the high value-added utilization of CTR.展开更多
In this work,the combined addition of strontium/indium(Sr/In)to the magnesium anode for Mg-Air Cells is investigated to improve discharge performance by modifying the anode/electrolyte interface.Indium exists as solid...In this work,the combined addition of strontium/indium(Sr/In)to the magnesium anode for Mg-Air Cells is investigated to improve discharge performance by modifying the anode/electrolyte interface.Indium exists as solid solution atoms in theα-Mg matrix without its second-phase generation,and at the same time facilitates grain refinement,dendritic segregation and Mg17Sr2-phases precipitation.During discharge operation,Sr modifies the film composition via its compounds and promoted the redeposition of In at the substrate/film interface;their co-deposition behavior on the anodic reaction surface enhances anode reaction kinetics,suppresses the negative difference effect(NDE)and mitigates the“chunk effect”(CE),which is contributed to uniform dissolution and low self-corrosion hydrogen evolution rate(HER).Therefore,Mg-Sr-xIn alloy anodes show excellent discharge performance,e.g.,0.5Sr-1.0In shows an average discharge voltage of 1.4234 V and a specific energy density of 1990.71 Wh kg^(-1)at 10 mA cm^(-2).Furthermore,the decisive factor(CE and self-discharge HE)for anodic efficiency are quantitively analyzed,the self-discharge is the main factor of cell efficiency loss.Surprisingly,all Mg-Sr-xIn anodes show anodic efficiency greater than 60%at high current density(≥10 mA cm^(-2)),making them excellent candidate anodes for Mg-Air cells at high-power output.展开更多
The dominated contradiction in optimizing the performance of magnesium-air battery anode lies in the difficulty of achieving a good balance between activation and passivation during discharge process.To further reconci...The dominated contradiction in optimizing the performance of magnesium-air battery anode lies in the difficulty of achieving a good balance between activation and passivation during discharge process.To further reconcile this contradiction,two Mg-0.1Sc-0.1Y-0.1Ag anodes with different residual strain distribution through extrusion with/without annealing are fabricated.The results indicate that annealing can significantly lessen the“pseudo-anode”regions,thereby changing the dissolution mode of the matrix and achieving an effective dissolution during discharge.Additionally,p-type semiconductor characteristic of discharge productfilm could suppress the self-corrosion reaction without reducing the polarization of anode.The magnesium-air battery utilizing annealed Mg-0.1Sc-0.1Y-0.1Ag as anode achieves a synergistic improvement in specific capacity(1388.89 mA h g^(-1))and energy density(1960.42 mW h g^(-1)).This anode modification method accelerates the advancement of high efficiency and long lifespan magnesium-air batteries,offering renewable and cost-effective energy solutions for electronics and emergency equipment.展开更多
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financially supported by the National Natural Science Foundation of China (52272209)
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support from the National Key R&D Program of China(2022YFB2402600)the National Natural Science Foundation of China(52125105,52572282,52472269,52273312,22309200)+3 种基金Guangdong Basic and Applied Basic Research Foundation(2024A1515010201,2024A1515012379,2024A1515011670,2023A1515011519)Guangdong Special Support Program Outstanding Young Talents in Science and Technology Innovation(2021TQ05L894)Shenzhen Science and Technology Planning Project(JSGG20220831104004008,SGDX20230116092055008,KCXST20221021111606016)the NSRF via the Program Management Unit for Human Resources&Institutional Development,Research and Innovation(B49G680115).
文摘Sodium-based dual-ion batteries(SDIBs)have been attracting increasing attention in recent years owing to their low cost,environmental benignancy,and high operating voltage.However,the sluggish ion kinetics of conventional carbon anodes that cannot match the fast capacitive anion intercalation behavior of graphite cathodes constraints on improving power density of SDIBs.Herein,we present an ingenious carbon microdomain engineering strategy to fabricate high-performance carbon anode with ion-mediated high-activity nitrogen species and molecular-scale closed-pore architectures.Experimental characterizations and theoretical investigations demonstrate that Zn^(2+)-mediated structural engineering tailors oxidized nitrogen species,which proficiently accelerate the sodium-ion desolvation kinetics;meanwhile the acetate-mediated pore-forming process modulates closed pores,which synergistically afford abundant sodium storage sites for high plateau-region capacity.As a result,the optimized microdomain engineered carbon material(MEC_(3))tailored with the optimal amount of zinc acetate demonstrates an outstanding plateau-region capacity of 253 mAh g^(-1)even at 1 C,among the highest reported values.Consequently,the MEC_(3)||expanded graphite dual-ion battery exhibits an unprecedented cycling stability at high current rate,maintaining 80.6%capacity retention after 10,000 cycles at 10 C,among the best reports.This microdomain engineering strategy provides a new design principle for overcoming kinetic limitations of carbonaceous materials in plateau-dominated sodium storage systems.
基金support from the Australian Research Council Discovery Program(DP220103416,DP240102177)Australian Research Council Future Fellowships(FT200100730,FT210100804).
文摘Aqueous zinc(Zn)-ion batteries hold great promise as renewable energy storage system for carbon-neutral energy transition.However,Zn anodes suffer from poor Zn plating/stripping reversibility due to Zn dendrite growth and side reactions.Existing Zn interfacial modification strategies based on single-component or homogeneous structure are insufficient to address these issues comprehensively.Herein,we rationally designed an organic-inorganic hybrid interfacial layer with rigid-to-soft graded structure for dendrite-free and stable Zn anodes.A liquid plasma-assisted oxidation technology is developed to rapidly construct a porous ZnO inner framework in situ.This ZnO layer offers high interfacial energy,mechanical robustness,and an open structure that facilitates ion transport while firmly anchoring a subsequently coated soft polymer layer.The resulting architecture presents a structurally graded and functionally complementary interface,enabling effective dendrite suppression,continuous Zn ion transport,and enhanced corrosion resistance.As a result,a long cycling stability of more than 6000 h can be achieved at 1 mA cm^(-2)for 1 mAh cm^(-2)in symmetric cells.When used as anodes for zinc-iodine full battery,the hybrid interlayer can effectively prevent the Zn anodes from the corrosion by polyiodine,enabling stable cycling and negligible capacity decay(~0.02‰per cycle)for over 10,000 cycles at 2.0 A g^(-1).This work demonstrates a promising interfacial design strategy and introduces a novel liquid plasma-assisted oxidation route for fabricating high-performance Zn anodes towards next-generation aqueous batteries.
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(52471240)the Natural Science Foundation of Zhejiang Province(LZ23B030003)+2 种基金the Fundamental Research Funds for the Central Universities(226-2024-00075)support from the Engineering and Physical Sciences Research Council(EPSRC,UK)RiR grant-RIR18221018-1EU COST CA23155。
文摘The electric double layer(EDL)at the electrochemical interface is crucial for ion transport,charge transfer,and surface reactions in aqueous rechargeable zinc batteries(ARZBs).However,Zn anodes routinely encounter persistent dendrite growth and parasitic reactions,driven by the inhomogeneous charge distribution and water-dominated environment within the EDL.Compounding this,classical EDL theory,rooted in meanfield approximations,further fails to resolve molecular-scale interfacial dynamics under battery-operating conditions,limiting mechanistic insights.Herein,we established a multiscale theoretical calculation framework from single molecular characteristics to interfacial ion distribution,revealing the EDL’s structure and interactions between different ions and molecules,which helps us understand the parasitic processes in depth.Simulations demonstrate that water dipole and sulfate ion adsorption at the inner Helmholtz plane drives severe hydrogen evolution and by-product formation.Guided by these insights,we engineered a“water-poor and anion-expelled”EDL using 4,1’,6’-trichlorogalactosucrose(TGS)as an electrolyte additive.As a result,Zn||Zn symmetric cells with TGS exhibited stable cycling for over 4700 h under a current density of 1 mA cm^(−2),while NaV_(3)O_(8)·1.5H_(2)O-based full cells kept 90.4%of the initial specific capacity after 800 cycles at 5 A g^(−1).This work highlights the power of multiscale theoretical frameworks to unravel EDL complexities and guide high-performance ARZB design through integrated theory-experiment approaches.
基金supported by the Basic Science Research Program(RS-2024-00455177)through the National Research Foundation of Korea(NRF)funded by the Ministry of Science,ICT.
文摘Aqueous zinc ion batteries(AZIBs)are considered promising candidates owing to their inherent safety and low cost.However,the conventional glass fiber(GF)separator used in AZIBs suffers from poor physicochemical properties,leading to uncontrolled zinc(Zn)dendrite formation and undesirable side reactions.To address these limitations and enhance the electrochemical performance of AZIBs,a precisely designed functional separator is developed by incorporating UiO-66-(COOH)_(2)into a poly(vinylidene fluoride)(PVDF)framework(U-PVDF)via a direct in situ growth method.This approach enables uniform distribution of UiO-66-(COOH)_(2)both on the surface and within the PVDF backbone,without increasing separator thickness.Owing to the strong interaction between Zn^(2+)and the abundant carboxyl groups in UiO-66-(COOH)_(2),the U-PVDF separator regulates the Zn^(2+)solvation structure toward a contact ion pair-dominated structure by reducing coordinated water molecules,which effectively mitigates water-induced parasitic reactions and promotes compact Zn deposition.Consequently,a Zn/Zn symmetric cell employing the U-PVDF separator demonstrates superior cycling stability over 1500 cycles without internal short-circuiting at a current density of 6 mA cm^(−2)and an areal capacity of 2 mAh cm^(−2).Moreover,Zn/NaV_(3)O_(8)·xH_(2)O(NVO)cell with the U-PVDF separator exhibits markedly improved cyclability and rate performance compared with those using conventional GF separator.
基金supported by the Yunnan Province Basic Research General Program,China(No.202201BE070001-002)the Major Science and Technology Projects in Yunnan Province,China(No.202402AF 080005).
文摘The rapid expansion of the photovoltaic industry has generated heavily oxidized waste silicon(wSi),which hinders efficient recycling owing to its small particle size and uncontrolled surface oxidation.This study introduces a molten salt electrochemical strategy for converting photovoltaic wSi into NiSi_(2)-silicon nanorods(NiSi_(2)-SiNRs)as high-performance anode materials for lithium-ion batteries.A stable oxidized passivation layer is formed on the wSi surface via controlled oxidation,and further in situ generated highly active NiSi_(2) droplets.The molten salt electric field modulates the surface energy of silicon,while particle integration drives localized directional growth,enabling the self-assembly of NiSi_(2)-SiNRs composites.These NiSi_(2)-SiNRs anodes exhibit rapid ion transport and effective strain buffering.The high aspect ratio of SiNRs and the presence of retained NiSi_(2) facilitate both longitudinal and transverse Li^(+) diffusion.Owing to their robust structural design,the NiSi_(2)-SiNRs anode achieves an excellent initial Coulombic efficiency of 91.61%and retains 72.99%of its capacity after 800 cycles at 2 A·g^(−1).This study establishes a model system for investigating silicide/silicon interfaces in molten salt electrochemical synthesis and provides an effective strategy for upcycling photovoltaic wSi into high-performance lithium-ion battery anodes.
基金supported by the Foundation of Yunnan Province(Nos.202301AU070021,202201BE070001-027)the Test Foundation of KUST(No.2022T20210208).
文摘Halide perovskite materials have received considerable attention for solar cells,LEDs,lasers etc.owing to their controllable physicochemical properties and structural advantages.However,little research has focused on energy storage and conversion applications,such as use as anodes in lithium-ion batteries.In this paper,all-inorganic lead-free halide perovskite Cs_(3)Bi_(2)Cl_(9)powders were synthesized by the grinding method,and the lattice was successfully adjusted via introducing Mn^(2+).The characterization results show that Mn-ion substitution can cause local lattice distortion to restructure the lattice,which will cause a mixed arrangement of[BiCl_(6)]octahedra to improve the performance of the anode material.This new material can provide a feasible solution for solving the problem of low specific capacity anode materials caused by unstable crystal structures,and also indicates that such perovskites with unique crystal structures and lattice tunability have broad application prospects in lithium-ion batteries.
基金National Key Research and Development Program of China (2022YFB2402200)National Natural Science Foundation of China (22225201,22379028)+2 种基金Fundamental Research Funds for the Central Universities (20720220010)Shanghai Pilot Program for Basic Research–Fudan University 21TQ1400100 (21TQ009)Key Basic Research Program of Science and Technology Commission of Shanghai Municipality (23520750400)。
文摘Sodium-ion batteries (SIBs) with organic electrodes are an emerging research direction due to the sustainability of organic materials based on elements like C,H,O,and sodium ions.Currently,organic electrode materials for SIBs are mainly used as cathodes because of their relatively high redox potentials(>1 V).Organic electrodes with low redox potential that can be used as anode are rare.Herein,a novel organic anode material (tetrasodium 1,4,5,8-naphthalenetetracarboxylate,Na_(4)TDC) has been developed with low redox potential (<0.7 V) and excellent cyclic stability.Its three-sodium storage mechanism was demonstrated with various in-situ/ex-situ spectroscopy and theoretical calculations,showing a high capacity of 208 mAh/g and an average decay rate of merely 0.022%per cycle.Moreover,the Na_(4)TDC-hard carbon composite can further acquire improved capacity and cycling stability for 1200 cycles even with a high mass loading of up to 20 mg cm^(-2).By pairing with a thick Na_(3)V_(2)(PO_(4))_(3)cathode (20.6 mg cm^(-2)),the as-fabricated full cell exhibited high operating voltage (2.8 V),excellent rate performance and cycling stability with a high capacity retention of 88.7% after 200 cycles,well highlighting the Na_(4)TDC anode material for SIBs.
基金supported by the National Research Foundation(NRF)of Korea grant funded by the Korean government(MSIT)(No.NRF-2021 M3 H4A1A02045962).
文摘With the increasing prevalence of lithium-ion batteries(LIBs)applications,the demand for high-capacity next-generation materials has also increased.SiO_(x)is currently considered a promising anode material due to its exceptionally high capacity for LIBs.However,the significant volumetric changes of SiO_(x)during cycling and its initial Coulombic efficiency(ICE)complicate its use,whether alone or in combination with graphite materials.In this study,a three-dimensional conductive binder network with high electronic conductivity and robust elasticity for graphite/SiO_(x)blended anodes was proposed by chemically anchoring carbon nanotubes and carboxymethyl cellulose binders using tannic acid as a chemical cross-linker.In addition,a dehydrogenation-based prelithiation strategy employing lithium hydride was utilized to enhance the ICE of SiO_(x).The combination of these two strategies increased the CE of SiO_(x)from 74%to87%and effectively mitigated its volume expansion in the graphite/SiO_(x)blended electrode,resulting in an efficient electron-conductive binder network.This led to a remarkable capacity retention of 94%after30 cycles,even under challenging conditions,with a high capacity of 550 mA h g^(-1)and a current density of 4 mA cm^(-2).Furthermore,to validate the feasibility of utilizing prelithiated SiO_(x)anode materials and the conductive binder network in LIBs,a full cell incorporating these materials and a single-crystalline Ni-rich cathode was used.This cell demonstrated a~27.3%increase in discharge capacity of the first cycle(~185.7 mA h g^(-1))and exhibited a cycling stability of 300 cycles.Thus,this study reports a simple,feasible,and insightful method for designing high-performance LIB electrodes.
基金Financial support from National Key R&D Program(2022YFB2404600)Natural Science Foundation of China(Key Project of 52131306)+1 种基金Project on Carbon Emission Peak and Neutrality of Jiangsu Province(BE2022031-4)the Big Data Computing Center of Southeast University are greatly appreciated.
文摘The replacement of non-aqueous organic electrolytes with solid-state electrolytes(SSEs)in solid-state lithium metal batteries(SLMBs)is considered a promising strategy to address the constraints of lithium-ion batteries,especially in terms of energy density and reliability.Nevertheless,few SLMBs can deliver the required cycling performance and long-term stability for practical use,primarily due to suboptimal interface properties.Given the diverse solidification pathways leading to different interface characteristics,it is crucial to pinpoint the source of interface deterioration and develop appropriate remedies.This review focuses on Li|SSE interface issues between lithium metal anode and SSE,discussing recent advancements in the understanding of(electro)chemistry,the impact of defects,and interface evolutions that vary among different SSE species.The state-ofthe-art strategies concerning modified SEI,artificial interlayer,surface architecture,and composite structure are summarized and delved into the internal relationships between interface characteristics and performance enhancements.The current challenges and opportunities in characterizing and modifying the Li|SSE interface are suggested as potential directions for achieving practical SLMBs.
基金supported by the National Natural Science Foundation of China(22209006)the Fundamental Research Funds for the Central Universities(buctrc202307)the Natural Science Foundation of Shandong Province(ZR2022QE009)。
文摘To meet the demand for enhanced energy density and improved safety in batteries,anode-free aqueous zinc metal batteries(AF-AZMBs)have garnered significant research interest and attention.Compared with conventional aqueous Zn batteries,AF-AZMBs provide higher theoretical energy density,a more simplified structural design,and improved cost-effectiveness.However,AF-AZMBs are confronted with severe capacity degradation and lifespan reduction due to the absence of an excess zinc inventory.In recent years,extensive research efforts have been devoted to addressing these challenges,resulting in significant advancements.Therefore,there is highly warranted for a comprehensive discussion on AF-AZMBs.Herein,this review provides a thorough analysis and in-depth investigation of recent developments in AF-AZMBs from the perspectives of current collectors,electrolytes,and cathodes.Specifically,the working mechanisms and advantageous features of AF-AZMBs are summarized.The major scientific issues affecting capacity degradation and lifespan reduction are discussed,including inhomogeneous Zn deposition/stripping kinetics,unstable SEI layer,and irreversible cathode material loss.Furthermore,the corresponding strategies to address these issues are highlighted,such as anodic current collector design,electrolyte engineering,and cathodic modification.Finally,several promising directions are explored for the future advancement of AF-AZMBs,including developing high-performance Zn-rich cathodes,regulating solid-state electrolytes,and designing dual-electrode-free zinc-metal batteries.Additionally,exploring advanced characterization and analysis techniques and optimizing pouch cells under practical operating conditions are also mentioned,highlighting the urgent need for further research to address existing bottlenecks.
基金supported by the National Natural Science Foundation of China(22479031,22162004)the Natural Science Foundation of Guangxi(2022JJD120011).
文摘H_(2)O-induced side reactions and dendrite growth occurring at the Zn anode-electrolyte interface(AEI)limit the electrochemical performances of aqueous zinc ion batteries.Herein,methionine(Met)is introduced as an electrolyte additive to solve the above issues by three aspects:Firstly,Met is anchored on Zn anode by amino/methylthio groups to form a H_(2)O-poor AEI,thus increasing the overpotential of hydrogen evolution reaction(HER);secondly,Met serves as a pH buffer to neutralize the HER generated OH-,thereby preventing the formation of by-products(e.g.Zn_(4)SO_(4)(OH)_(6)·xH_(2)O);thirdly,Zn^(2+) could be captured by carboxyl group of the anchored Met through electrostatic interaction,which promotes the dense and flat Zn deposition.Consequently,the Zn||Zn symmetric cell obtains a long cycle life of 3200 h at 1.0 mA cm^(-2),1.0 mAh cm^(-2),and 1400 h at 5.0 mA cm^(-2),5.0 mAh cm^(-2).Moreover,Zn||VO_(2) full cell exhibits a capacity retention of 91.0%after operating for 7000 cycles at 5.0 A g^(-1).This study offers a novel strategy for modulating the interface microenvironment of AEI via integrating the molecular adsorption,pH buffer,and Zn^(2+) capture strategies to design advanced industrial-oriented batteries.
基金supported by the National Natural Science Foundation of China(Nos.52102291,52271011,and 51701142)supported by a grant from the Cangzhou Institute of Tiangong University(No.TGCYY-F-0201)。
文摘Sodium metal has been widely studied in the field of batteries due to its high theoretical specific capacity(~1,166 m Ah/g),low redox potential(-2.71 V compared to standard hydrogen electrode),and lowcost advantages.However,problems such as unstable solid electrolyte interface(SEI),uncontrolled dendrite growth,and side reactions between solid-liquid interfaces have hindered the practical application of sodium metal anodes(SMAs).Currently,lots of strategies have been developed to achieve stabilized sodium metal anodes.Among these strategies,modified metal current collectors(MCCs)stand out due to their unique role in accommodating volumetric fluctuations with superior structure,lowering the energy barrier for sodium nucleation,and providing guided uniform sodium deposition.In this review,we first introduced three common metal-based current collectors applied to SMAs.Then,we summarized strategies to improve sodium deposition behavior by optimally engineering the surface of MCCs,including surface loading,surface structural design,and surface engineering for functional modification.We have followed the latest research progress and summarized surface optimization cases on different MCCs and their applications in battery systems.
基金supported by the Quzhou Science and Technology Bureau Project(2023D023,2023D030,2023D002,and2024D028)the Joint Funds of the Zhejiang Provincial Natural Science Foundation of China(LZY23B030002)+3 种基金the Shijiazhuang Shangtai Technology Co.,Ltd.Hebei Provincial Department of Science and Technology(24291101Z)the International Cooperation Projects of Sichuan Provincial Department of Science and Technology(2021YFH0126)the Sichuan Provincial Science and Technology Department's key research project(2023YFG0203)。
文摘Metal foils have emerged as one of the promising materials for anode-free batteries due to their high energy density and scalability in production.The unclear lithium plating/stripping kinetics of metal foil current collectors in anode-free batteries was addressed by using the non-destructive distribution of relaxation times(DRT)analysis to systematically investigate the lithium transport behavior of 14 metal foils and its correlation with electrochemical performance.By integrating energy-dispersive spectro scopy(EDS),cyclic voltammetry(CV),and galvanostatic testing,the exceptional properties of indium(In),tin(Sn),and silver(Ag)were revealed:the Li-In alloying reaction exhibits high reversibility,Li-Sn alloys demonstrate outstanding cycling stability,and the Li-Ag solid-solution mechanism provides an ideal lithium deposition interface on the silver substrate.The DRT separates the polarization internal resistance of lithium ions passing through the SEI layer(R_(sei),τ2)and the polarization internal resistance of lithium ions undergoing charge transfer reaction at the electrolyte/electrode interface(R_(ct),τ3)by decoupling the electrochemical impedance spectroscopy(EIS).For the first time,the correlation betweenτ2,τ3,and the cycle life/Coulombic efficiency of alloy/solid-solution metals was established,while non-alloy metals are not suitable for this method due to differences in lithium deposition mechanisms.This study not only illuminates the structure-property relationship governing the lithium kinetics of metal foil electrodes but also provides a novel non-destructive analytical strategy and theoretical guidance for the rational design of stable anodes in high-energy-density batteries,facilitating the efficient screening and optimization of anode-free battery.
基金financially supported by the Research Project Supported by Shanxi Scholarship Council of China(No.2022-049)the Natural Science Foundation of Shanxi Province,China(No.20210302123167)。
文摘Carbon materials are widely recognized as highly promising electrode materials for various energy storage system applications.Coal tar residues(CTR),as a type of carbon-rich solid waste with high value-added utilization,are crucially important for the development of a more sustainable world.In this study,we employed a straightforward direct carbonization method within the temperature range of 700-1000℃to convert the worthless solid waste CTR into economically valuable carbon materials as anodes for potassium-ion batteries(PIBs).The effect of carbonization temperature on the microstructure and the potassium ions storage properties of CTR-derived carbons(CTRCs)were systematically explored by structural and morphological characterization,alongside electrochemical performances assessment.Based on the co-regulation between the turbine layers,crystal structure,pore structure,functional groups,and electrical conductivity of CTR-derived carbon carbonized at 900℃(CTRC-900H),the electrode material with high reversible capacity of 265.6m Ah·g^(-1)at 50 m A·g^(-1),a desirable cycling stability with 93.8%capacity retention even after 100 cycles,and the remarkable rate performance for PIBs were obtained.Furthermore,cyclic voltammetry(CV)at different scan rates and galvanostatic intermittent titration technique(GITT)have been employed to explore the potassium ions storage mechanism and electrochemical kinetics of CTRCs.Results indicate that the electrode behavior is predominantly governed by surface-induced capacitive processes,particularly under high current densities,with the potassium storage mechanism characterized by an“adsorption-weak intercalation”mechanism.This work highlights the potential of CTR-based carbon as a promising electrode material category suitable for high-performance PIBs electrodes,while also provides valuable insights into the new avenues for the high value-added utilization of CTR.
文摘In this work,the combined addition of strontium/indium(Sr/In)to the magnesium anode for Mg-Air Cells is investigated to improve discharge performance by modifying the anode/electrolyte interface.Indium exists as solid solution atoms in theα-Mg matrix without its second-phase generation,and at the same time facilitates grain refinement,dendritic segregation and Mg17Sr2-phases precipitation.During discharge operation,Sr modifies the film composition via its compounds and promoted the redeposition of In at the substrate/film interface;their co-deposition behavior on the anodic reaction surface enhances anode reaction kinetics,suppresses the negative difference effect(NDE)and mitigates the“chunk effect”(CE),which is contributed to uniform dissolution and low self-corrosion hydrogen evolution rate(HER).Therefore,Mg-Sr-xIn alloy anodes show excellent discharge performance,e.g.,0.5Sr-1.0In shows an average discharge voltage of 1.4234 V and a specific energy density of 1990.71 Wh kg^(-1)at 10 mA cm^(-2).Furthermore,the decisive factor(CE and self-discharge HE)for anodic efficiency are quantitively analyzed,the self-discharge is the main factor of cell efficiency loss.Surprisingly,all Mg-Sr-xIn anodes show anodic efficiency greater than 60%at high current density(≥10 mA cm^(-2)),making them excellent candidate anodes for Mg-Air cells at high-power output.
基金the National Natural Science:Foundation of China(52375370)the Open Project of Salt Lake Chemical Engineering Research Complex,Qinghai University(2023-DXSSKF-Z02)+2 种基金the Nat-ural Science Foundation of Shanxi(202103021224049)GDAS Projects of International cooperation platform of Sci-ence and Technology(2022GDASZH-2022010203-003)Guangdong province Science and Technology Plan Projects(2023B1212060045).
文摘The dominated contradiction in optimizing the performance of magnesium-air battery anode lies in the difficulty of achieving a good balance between activation and passivation during discharge process.To further reconcile this contradiction,two Mg-0.1Sc-0.1Y-0.1Ag anodes with different residual strain distribution through extrusion with/without annealing are fabricated.The results indicate that annealing can significantly lessen the“pseudo-anode”regions,thereby changing the dissolution mode of the matrix and achieving an effective dissolution during discharge.Additionally,p-type semiconductor characteristic of discharge productfilm could suppress the self-corrosion reaction without reducing the polarization of anode.The magnesium-air battery utilizing annealed Mg-0.1Sc-0.1Y-0.1Ag as anode achieves a synergistic improvement in specific capacity(1388.89 mA h g^(-1))and energy density(1960.42 mW h g^(-1)).This anode modification method accelerates the advancement of high efficiency and long lifespan magnesium-air batteries,offering renewable and cost-effective energy solutions for electronics and emergency equipment.
