The solvent-free in situ polymerization technique has the potential to tailor-make conformal interfaces that are essential for developing durable and safe lithium metal polymer batteries(LMPBs).Hence,much attention ha...The solvent-free in situ polymerization technique has the potential to tailor-make conformal interfaces that are essential for developing durable and safe lithium metal polymer batteries(LMPBs).Hence,much attention has been given to the eco-friendly and rapid ultraviolet(UV)-induced in situ photopolymerization process to prepare solid-state polymer electrolytes.In this respect,an innovative method is proposed here to overcome the challenges of UV-induced photopolymerization(UV-curing)in the zones where UV-light cannot penetrate,especially in LMPBs where thick electrodes are used.The proposed frontal-inspired photopolymerization(FIPP)process is a diverged frontal-based technique that uses two classes(dual)of initiators to improve the slow reaction kinetics of allyl-based monomers/oligomers by at least 50%compared with the conventional UV-curing process.The possible reaction mechanism occurring in FIPP is demonstrated using density functional theory calculations and spectroscopic investigations.Indeed,the initiation mechanism identified for the FIPP relies on a photochemical pathway rather than an exothermic propagating front forms during the UV-irradiation step as the case with the classical frontal photopolymerization technique.Besides,the FIPP-based in situ cell fabrication using dual initiators is advantageous over both the sandwich cell assembly and conventional in situ photopolymerization in overcoming the limitations of mass transport and active material utilization in high energy and high power LMPBs that use thick electrodes.Furthermore,the LMPB cells fabricated using the in situ-FIPP process with high mass loading LiFePO_(4)electrodes(5.2 mg cm^(-2))demonstrate higher rate capability,and a 50%increase in specific capacity against a sandwich cell encouraging the use of this innovative process in large-scale solid-state battery production.展开更多
Aqueous zinc-halogen batteries are promising candidates for large-scale energy storage due to their abundant resources,intrinsic safety,and high theoretical capacity.Nevertheless,the uncontrollable zinc dendrite growt...Aqueous zinc-halogen batteries are promising candidates for large-scale energy storage due to their abundant resources,intrinsic safety,and high theoretical capacity.Nevertheless,the uncontrollable zinc dendrite growth and spontaneous shuttle effect of active species have prohibited their practical implementation.Herein,a double-layered protective film based on zinc-ethylenediamine tetramethylene phosphonic acid(ZEA)artificial film and ZnF2-rich solid electrolyte interphase(SEI)layer has been successfully fabricated on the zinc metal anode via electrode/electrolyte synergistic optimization.The ZEA-based artificial film shows strong affinity for the ZnF2-rich SEI layer,therefore effectively suppressing the SEI breakage and facilitating the construction of double-layered protective film on the zinc metal anode.Such double-layered architecture not only modulates Zn2+flux and suppresses the zinc dendrite growth,but also blocks the direct contact between the metal anode and electrolyte,thus mitigating the corrosion from the active species.When employing optimized metal anodes and electrolytes,the as-developed zinc-(dual)halogen batteries present high areal capacity and satisfactory cycling stability.This work provides a new avenue for developing aqueous zinc-(dual)halogen batteries.展开更多
The development of lithium-ion batteries with high-energy densities is substantially hampered by the graphite anode's low theoretical capacity(372 mAh g^(-1)).There is an urgent need to explore novel anode materia...The development of lithium-ion batteries with high-energy densities is substantially hampered by the graphite anode's low theoretical capacity(372 mAh g^(-1)).There is an urgent need to explore novel anode materials for lithium-ion batteries.Silicon(Si),the second-largest element outside of Earth,has an exceptionally high specific capacity(3579 mAh g^(-1)),regarded as an excellent choice for the anode material in high-capacity lithium-ion batteries.However,it is low intrinsic conductivity and volume amplification during service status,prevented it from developing further.These difficulties can be successfully overcome by incorporating carbon into pure Si systems to form a composite anode and constructing a buffer structure.This review looks at the diffusion mechanism,various silicon-based anode material configurations(including sandwich,core-shell,yolk-shell,and other 3D mesh/porous structures),as well as the appropriate binders and electrolytes.Finally,a summary and viewpoints are offered on the characteristics and structural layout of various structures,metal/non-metal doping,and the compatibility and application of various binders and electrolytes for silicon-based anodes.This review aims to provide valuable insights into the research and development of silicon-based carbon anodes for high-performance lithium-ion batteries,as well as their integration with binders and electrolyte.展开更多
All-solid-state Li batteries(ASSLBs)using solid electrolytes(SEs)have gained significant attention in recent years considering the safety issue and their high energy density.Despite these advantages,the commercializat...All-solid-state Li batteries(ASSLBs)using solid electrolytes(SEs)have gained significant attention in recent years considering the safety issue and their high energy density.Despite these advantages,the commercialization of ASSLBs still faces challenges regarding the electrolyte/electrodes interfaces and growth of Li dendrites.Elemental doping is an effective and direct method to enhance the performance of SEs.Here,we report an Al-F co-doping strategy to improve the overall properties including ion conductivity,high voltage stability,and cathode and anode compatibility.Particularly,the Al-F co-doping enables the formation of a thin Li-Al alloy layer and fluoride interphases,thereby constructing a relatively stable interface and promoting uniform Li deposition.The similar merits of Al-F co-doping are also revealed in the Li-argyrodite series.ASSLBs assembled with these optimized electrolytes gain good electrochemical performance,demonstrating the universality of Al-F co-doping towards advanced SEs.展开更多
The development of flexible supercapacitors(FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and elec...The development of flexible supercapacitors(FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and electrode materials stand as two key components that significantly impact the efficacy of hightemperature-tolerant FSCs(HT-FSCs). They should not only exhibit high electrochemical performance and excellent flexibility, but also withstand intense thermal stress. Considerable efforts have been devoted to enhancing their thermal stability while maintaining high electrochemical and mechanical performance. In this review, the fundamentals of HT-FSCs are outlined. A comprehensive overview of state-of-the-art progress and achievements in HT-FSCs, with a focus on thermally stable gel polymer electrolytes and electrode materials is provided. Finally, challenges and future perspectives regarding HT-FSCs are discussed, alongside strategies for elevating operational temperatures and performance.This review offers both theoretical foundations and practical guidelines for designing and manufacturing HT-FSCs, further promoting their widespread adoption across diverse fields.展开更多
Electron transfer processes at polymer electrolyte/electrode interfaces play a central role in modern electrochemical devices of energy conversion,however,current understanding of electron transfers through electroche...Electron transfer processes at polymer electrolyte/electrode interfaces play a central role in modern electrochemical devices of energy conversion,however,current understanding of electron transfers through electrochemical interfaces was established exclusively based on the studies of liquid/solid electrochemical interfaces.Thus,similarities and differences of liquid and polymer electrolyte/electrode interfaces need to be mapped out to guide the design of device level electrochemical interfaces.In this work,we employ the sulfonate adsorption/desorption as a probe reaction to understand the electron-transfer steps in polymer and liquid electrolytes.Through cyclic voltametric investigations on the well-define single-crystal Pd_(ML)Pt(111)electrode,we demonstrate that the oxidative adsorption and reductive desorption of sulfonates at the polymer electrolyte/electrode interface are chemically distinct from those in liquid electrolytes,with the former occurring mostly via the proton-coupled pathway while the latter proceeding mainly through the solvation-mediated pathway.Importantly,the sulfonate adsorption/desorption behaviors of alkylsulfonates become increasingly similar to those in Nafion with longer alkyl chains,suggesting that the interfacial hydrophobicity and solvation environment conferred by the perfluorinated polymer play a decisive role in the electron-transfer mechanism.Results reported in this study highlight the mechanistic distinctions between electron-transfer processes at electrochemical interfaces involving polymer and liquid electrolytes,and provide a framework for understanding electron-transfer processes at polymer electrolyte/electrode interfaces.展开更多
The publisher regrets to inform that in the article of Advanced Powder Materials 4(2025)100261,the published Figs.3 and 5 belong to the initially submitted version,which should be replaced by the final version.The dif...The publisher regrets to inform that in the article of Advanced Powder Materials 4(2025)100261,the published Figs.3 and 5 belong to the initially submitted version,which should be replaced by the final version.The differences between the initial and final versions of these figures are described below.展开更多
Solid-state Na metal batteries(SSNBs),known for the low cost,high safety,and high energy density,hold a significant position in the next generation of rechargeable batteries.However,the urgent challenge of poor interf...Solid-state Na metal batteries(SSNBs),known for the low cost,high safety,and high energy density,hold a significant position in the next generation of rechargeable batteries.However,the urgent challenge of poor interfacial contact in solid-state electrolytes has hindered the commercialization of SSNBs.Driven by the concept of intimate electrode-electrolyte interface design,this study employs a combination of sodium-potassium(NaK)alloy and carbon nanotubes to prepare a semi-solid NaK(NKC)anode.Unlike traditional Na anodes,the paintable paste-like NKC anode exhibits superior adhesion and interface compatibility with both current collectors and gel electrolytes,significantly enhancing the physical contact of the electrode-electrolyte interface.Additionally,the filling of SiO_(2) nanoparticles improves the wettability of NaK alloy on gel polymer electrolytes,further achieving a conformal interface contact.Consequently,the overpotential of the NKC symmetric cell is markedly lower than that of the Na symmetric cell when subjected to a long cycle of 300 hrs.The full cell coupled with Na_(3)V_(2)(PO_(4))_(2) cathodes had an initial discharge capacity of 106.8 mAh·g^(-1) with a capacity retention of 89.61%after 300 cycles,and a high discharge capacity of 88.1 mAh·g^(-1) even at a high rate of 10 C.The outstanding electrochemical performance highlights the promising application potential of the NKC electrode.展开更多
Metal coating is a prevalent strategy for enhancing surface properties.Among the numerous methods for preparing coatings,electrodeposition stands out due to its simplicity,cost-effectiveness,and high efficiency,making...Metal coating is a prevalent strategy for enhancing surface properties.Among the numerous methods for preparing coatings,electrodeposition stands out due to its simplicity,cost-effectiveness,and high efficiency,making it widely utilized in various metal coating applications.By meticulously selecting appropriate electrolytes and electrodeposition parameters,metal coatings with diverse structures and morphologies can be obtained,and tailored to meet specific performance requirements.As the demand for superior metal coating performance continues to rise,it is imperative to summarize and forecast electrodeposition techniques to meet the criteria for high quality and precision.This review delves into the electrodeposition preparation of several typical metal coatings in diverse electrolyte systems,including aqueous solutions,ionic liquids,deep eutectic solvents,and molten salts.We also examine the electrodeposition process on the cathode,elucidate the correlation between parameters and coating quality,and suggest future research directions.This review aims to provide valuable insights and guidance for the electrodeposition preparation of metal coatings.展开更多
The silicon-graphite(Si-C)composite electrode is considered a promising candidate for next-generation commercial electrodes due to its high capacity.However,lithium-ion batteries with silicon electrodes often experien...The silicon-graphite(Si-C)composite electrode is considered a promising candidate for next-generation commercial electrodes due to its high capacity.However,lithium-ion batteries with silicon electrodes often experience capacity fading and poor cyclic performance,primarily due to the mechanical degradation of the solid-electrolyte interphase(SEI).In this work,we present a homogenized constitutive model for Si-C composite electrodes under finite deformation,incorporating lithium-ion concentration-dependent properties.We perform a wrinkling analysis and systematically examine the influence of key parameters,such as modulus and thickness ratios,on the critical conditions for instability.Additionally,we investigate the ratcheting effect across varying silicon contents.Our findings reveal that maintaining the silicon content within an optimal range effectively reduces plastic accumulation during charge–discharge cycles.These insights provide crucial guidance for optimizing the design and fabrication of Si–C electrode systems,enhancing their durability and performance.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)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
Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temp...Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temperature(LT)operation.Therefore,a more comprehensive and systematic understanding of LIB behavior at LT is urgently required.This review article comprehensively reviews recent advancements in electrolyte engineering strategies aimed at improving the low-temperature operational capabilities of LIBs.The study methodically examines critical performance-limiting mechanisms through fundamental analysis of four primary challenges:insufficient ionic conductivity under cryogenic conditions,kinetically hindered charge transfer processes,Li+transport limitations across the solidelectrolyte interphase(SEI),and uncontrolled lithium dendrite growth.The work elaborates on innovative optimization approaches encompassing lithium salt molecular design with tailored dissociation characteristics,solvent matrix optimization through dielectric constant and viscosity regulation,interfacial engineering additives for constructing low-impedance SEI layers,and gel-polymer composite electrolyte systems.Notably,particular emphasis is placed on emerging machine learning-guided electrolyte formulation strategies that enable high-throughput virtual screening of constituent combinations and prediction of structure-property relationships.These artificial intelligence-assisted rational design frameworks demonstrate significant potential for accelerating the development of next-generation LT electrolytes by establishing quantitative composition-performance correlations through advanced data-driven methodologies.展开更多
Electrolytes play a key role in determining the electrochemical performance,safety,and lifespan of potassium-based batteries,making their selection and optimization a critical area of research.This study systematicall...Electrolytes play a key role in determining the electrochemical performance,safety,and lifespan of potassium-based batteries,making their selection and optimization a critical area of research.This study systematically investigates the effects of two major potassium-based battery electrolytes,potassium hexafluorophosphate(KPF_(6))and potassium difluorosulfonimide(KFSI)in ethylene carbonate/diethyl carbonate(EC/DEC)solvents,on battery performance,solid electrolyte interphase(SEI)stability,aluminum(Al)current collector corrosion behavior,electrochemical stability window,and dendrite growth issue.Experimental results reveal that KFSI electrolyte significantly outperforms KPF_(6)in terms of cycling stability,rate capability,and Coulombic efficiency(CE),primarily due to the formation of a high-quality SEI on electrode surface.Through X-ray photoelectron spectroscopy(XPS)and time-of-flight secondary ion mass spectrometry(TOF-SIMS)analyses,we construct the SEI structure for both electrolytes,and find that the SEI formed by KFSI is more uniform and stable.Additionally,KPF_(6)exhibits weaker corrosivity towards the Al current collector compared to KFSI due to the formation of an AlF_(3) layer with higher oxidation stability on Al surface.Furthermore,in-situ optical microscopy observations indicate that the dendrite growth in KFSI electrolyte is more uniform,preventing the aggregates.These findings provide essential experimental evidence and theoretical support for optimizing the electrolyte in potassium-based batteries.展开更多
The pursuit of high energy density and sustainable energy storage devices has been the target of many researchers.However,safety issues such as the susceptibility of conventional liquid electrolytes to leakage and fla...The pursuit of high energy density and sustainable energy storage devices has been the target of many researchers.However,safety issues such as the susceptibility of conventional liquid electrolytes to leakage and flammability,as well as performance degradation due to uncontrollable dendrite growth in liquid electrolytes,have been limiting the further development of energy storage devices.In this regard,gel polymer electrolytes(GPEs)based on lignocellulosic(cellulose,hemicellulose,lignin)have attracted great interest due to their high thermal stability,excellent electrolyte wettability,and natural abundance.Therefore,in this critical review,a comprehensive overview of the current challenges faced by GPEs is presented,followed by a detailed description of the opportunities and advantages of lignocellulosic materials for the fabrication of GPEs for energy storage devices.Notably,the key properties and corresponding construction strategies of GPEs for energy storage are analyzed and discussed from the perspective of lignocellulose for the first time.Moreover,the future challenges and prospects of lignocellulose-mediated GPEs in energy storage applications are also critically reviewed and discussed.We sincerely hope this review will stimulate further research on lignocellulose-mediated GPEs in energy storage and provide meaningful directions for the strategy of designing advanced GPEs.展开更多
Chloride-based solid electrolytes are considered promising candidates for next-generation high-energy-density all-solid-state batteries(ASSBs).However,their relatively low oxidative decomposition threshold(~4.2 V vs.L...Chloride-based solid electrolytes are considered promising candidates for next-generation high-energy-density all-solid-state batteries(ASSBs).However,their relatively low oxidative decomposition threshold(~4.2 V vs.Li^(+)/Li)constrains their use in ultrahighvoltage systems(e.g.,4.8 V).In this work,ferroelectric Ba TiO_(3)(BTO)nanoparticles with optimized thickness of~50-100 nm were successfully coated onto Li_(2.5)Y_(0.5)Zr_(0.5)Cl_(6)(LYZC@5BTO)electrolytes using a time-efficient ball-milling process.The nanoparticle-induced interfacial ionic conduction enhancement mechanism contributed to the preservation of LYZC’s high ionic conductivity,which remained at 1.06 m S cm^(-1)for LYZC@5BTO.Furthermore,this surface electric field engineering strategy effectively mitigates the voltage-induced self-decomposition of chloride-based solid electrolytes,suppresses parasitic interfacial reactions with single-crystal NCM811(SCNCM811),and inhibits the irreversible phase transition of SCNCM811.Consequently,the cycling stability of LYZC under high-voltage conditions(4.8 V vs.Li+/Li)is significantly improved.Specifically,ASSB cells employing LYZC@5BTO exhibited a superior discharge capacity of 95.4 m Ah g^(-1)over 200 cycles at 1 C,way outperforming cell using pristine LYZC that only shows a capacity of 55.4 m Ah g^(-1).Furthermore,time-of-flight secondary ion mass spectrometry and X-ray photoelectron spectroscopy analysis revealed that Metal-O-Cl by-products from cumulative interfacial side reactions accounted for 6% of the surface species initially,rising to 26% after 200 cycles in pristine LYZC.In contrast,LYZC@5BTO limited this increase to only 14%,confirming the effectiveness of BTO in stabilizing the interfacial chemistry.This electric field modulation strategy offers a promising route toward the commercialization of high-voltage solid-state electrolytes and energy-dense ASSBs.展开更多
Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving...Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving the overall performance of CPEs due to their difficulty in achieving robust electrochemical and mechanical interfaces simultaneously.Here,by regulating the surface charge characteristics of halloysite nanotube(HNT),we propose a concept of lithium-ion dynamic interface(Li^(+)-DI)engineering in nano-charged CPE(NCCPE).Results show that the surface charge characteristics of HNTs fundamentally change the Li^(+)-DI,and thereof the mechanical and ion-conduction behaviors of the NCCPEs.Particularly,the HNTs with positively charged surface(HNTs+)lead to a higher Li^(+)transference number(0.86)than that of HNTs-(0.73),but a lower toughness(102.13 MJ m^(-3)for HNTs+and 159.69 MJ m^(-3)for HNTs-).Meanwhile,a strong interface compatibilization effect by Li^(+)is observed for especially the HNTs+-involved Li^(+)-DI,which improves the toughness by 2000%compared with the control.Moreover,HNTs+are more effective to weaken the Li^(+)-solvation strength and facilitate the formation of Li F-rich solid-electrolyte interphase of Li metal compared to HNTs-.The resultant Li|NCCPE|LiFePO4cell delivers a capacity of 144.9 m Ah g^(-1)after 400 cycles at 0.5 C and a capacity retention of 78.6%.This study provides deep insights into understanding the roles of surface charges of nanofillers in regulating the mechanical and electrochemical interfaces in ASSLMBs.展开更多
To meet the growing needs of flexible and wearable electronics,stretchable energy storage devices—especially supercapacitors(SCs)—have become a key focus in advanced energy storage research.However,achieving both me...To meet the growing needs of flexible and wearable electronics,stretchable energy storage devices—especially supercapacitors(SCs)—have become a key focus in advanced energy storage research.However,achieving both mechanical stretchability and high capacitance in SC still faces great challenges,and the crucial factors lie in creating superior electrode materials that exhibit high electrochemical performance as well as excellent mechanical stretchability.Covalent organic frameworks(COFs)possess considerable potential as electrode materials for SCs by virtue of stable organic frameworks,open channels and designable functional groups.Nevertheless,their applications in flexible SCs are greatly hindered by their rigid characteristics.Here a novel COFs@conductive polymer hydrogels(CPHs)@poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)complexes,which integrate the pseudocapacitance of PDITAPA COF,mechanical stretchability of hydrogels and high conductivity of PEDOT:PSS,has been developed as stretchable electrode of SCs.Physically cross-linked PEDOT nanofibers,with their interlinked and entangled architecture,collectively boost mechanical,electrical,and electrochemical performance.The COFs@CPHs@PEDOT:PSS simultaneously demonstrates outstanding mechanical stretchability,high electrical behaviors,and superior swelling characteristics.The resulting SC exhibits advantages of simple structures,facile assembly processes,high specific capacitance,excellent cycling stability,and arbitrary deformation,which holds great application prospects for wearable electronic products.Owing to its uncomplicated structure,ease of production,high energy storage capacity,robust cycling performance,and adaptability to deformation,this fabricated SC is well-suited for next-generation wearable technologies.展开更多
To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as wel...To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as well.Herein,we suggest an effective approach to control the micropore structure of silicon oxide(SiO_(x))/artificial graphite(AG)composite electrodes using a perforated current collector.The electrode features a unique pore structure,where alternating high-porosity domains and low-porosity domains markedly reduce overall electrode resistance,leading to a 20%improvement in rate capability at a 5C-rate discharge condition.Using microstructure-resolved modeling and simulations,we demonstrate that the patterned micropore structure enhances lithium-ion transport,mitigating the electrolyte concentration gradient of lithium-ion.Additionally,perforating current collector with a chemical etching process increases the number of hydrogen bonding sites and enlarges the interface with the SiO_(x)/AG composite electrode,significantly improving adhesion strength.This,in turn,suppresses mechanical degradation and leads to a 50%higher capacity retention.Thus,regularly arranged micropore structure enabled by the perforated current collector successfully improves both rate capability and cycle life in SiO_(x)/AG composite electrodes,providing valuable insights into electrode engineering.展开更多
A novel type of porous magnesium electrode with a stable 3D copper foam as current collectors for the organic magnesium-air battery was prepared by both amperostatic and pulsed electrodeposition of magnesium on copper...A novel type of porous magnesium electrode with a stable 3D copper foam as current collectors for the organic magnesium-air battery was prepared by both amperostatic and pulsed electrodeposition of magnesium on copper foam substrates in an electrolyte of 1 mol/L EtMgBr/THF solution, respectively. Optimal parameters of the pulsed electrodeposition were obtained using a bending cathode at the right angle. The surface morphology of the porous electrode was investigated by SEM, and the discharging performance of the porous magnesium electrode was detected by the chronoamperometric measurement. The electrochemical stability of 3D copper foam current collectors was examined by cyclic voltammetry, SEM and ICP-OES analyses. The results show that the rate capability of the porous magnesium electrode with a stable 3D copper foam as a current collector is better than that of the planar magnesium electrode, and the rate capability of the porous magnesium electrode prepared by the pulsed electrodeposition is superior to that of the porous magnesium electrode prepared by the amperostatic electrodeposition. The 3D structure of copper foam current collectors of the porous magnesium electrode could keep stable during the discharging process.展开更多
基金The support provided by the German Federal Ministry of Education and Research(BMBF)within the project“Benchbatt”(03XP0047B)is gratefully acknowledged.
文摘The solvent-free in situ polymerization technique has the potential to tailor-make conformal interfaces that are essential for developing durable and safe lithium metal polymer batteries(LMPBs).Hence,much attention has been given to the eco-friendly and rapid ultraviolet(UV)-induced in situ photopolymerization process to prepare solid-state polymer electrolytes.In this respect,an innovative method is proposed here to overcome the challenges of UV-induced photopolymerization(UV-curing)in the zones where UV-light cannot penetrate,especially in LMPBs where thick electrodes are used.The proposed frontal-inspired photopolymerization(FIPP)process is a diverged frontal-based technique that uses two classes(dual)of initiators to improve the slow reaction kinetics of allyl-based monomers/oligomers by at least 50%compared with the conventional UV-curing process.The possible reaction mechanism occurring in FIPP is demonstrated using density functional theory calculations and spectroscopic investigations.Indeed,the initiation mechanism identified for the FIPP relies on a photochemical pathway rather than an exothermic propagating front forms during the UV-irradiation step as the case with the classical frontal photopolymerization technique.Besides,the FIPP-based in situ cell fabrication using dual initiators is advantageous over both the sandwich cell assembly and conventional in situ photopolymerization in overcoming the limitations of mass transport and active material utilization in high energy and high power LMPBs that use thick electrodes.Furthermore,the LMPB cells fabricated using the in situ-FIPP process with high mass loading LiFePO_(4)electrodes(5.2 mg cm^(-2))demonstrate higher rate capability,and a 50%increase in specific capacity against a sandwich cell encouraging the use of this innovative process in large-scale solid-state battery production.
基金support from the National Natural Science Foundation of China(22209089,22178187)Natural Science Foundation of Shandong Province(ZR2022QB048,ZR2021MB006)+2 种基金Excellent Youth Science Foundation of Shandong Province(Overseas)(2023HWYQ-089)the Taishan Scholars Program of Shandong Province(tsqn201909091)Open Research Fund of School of Chemistry and Chemical Engineering,Henan Normal University.
文摘Aqueous zinc-halogen batteries are promising candidates for large-scale energy storage due to their abundant resources,intrinsic safety,and high theoretical capacity.Nevertheless,the uncontrollable zinc dendrite growth and spontaneous shuttle effect of active species have prohibited their practical implementation.Herein,a double-layered protective film based on zinc-ethylenediamine tetramethylene phosphonic acid(ZEA)artificial film and ZnF2-rich solid electrolyte interphase(SEI)layer has been successfully fabricated on the zinc metal anode via electrode/electrolyte synergistic optimization.The ZEA-based artificial film shows strong affinity for the ZnF2-rich SEI layer,therefore effectively suppressing the SEI breakage and facilitating the construction of double-layered protective film on the zinc metal anode.Such double-layered architecture not only modulates Zn2+flux and suppresses the zinc dendrite growth,but also blocks the direct contact between the metal anode and electrolyte,thus mitigating the corrosion from the active species.When employing optimized metal anodes and electrolytes,the as-developed zinc-(dual)halogen batteries present high areal capacity and satisfactory cycling stability.This work provides a new avenue for developing aqueous zinc-(dual)halogen batteries.
基金supported by National Natural Science Foundation of China(No.22205182)National Science Fund for Distinguished Young Scholars(No.52025034)+2 种基金China Postdoctoral Science Foundation(Nos.2022M722594/2024T171170)Guangdong Basic and Applied Basic Research Foundation(No.2024A1515011516)financially supported by Innovation Team of Shaanxi Sanqin Scholars。
文摘The development of lithium-ion batteries with high-energy densities is substantially hampered by the graphite anode's low theoretical capacity(372 mAh g^(-1)).There is an urgent need to explore novel anode materials for lithium-ion batteries.Silicon(Si),the second-largest element outside of Earth,has an exceptionally high specific capacity(3579 mAh g^(-1)),regarded as an excellent choice for the anode material in high-capacity lithium-ion batteries.However,it is low intrinsic conductivity and volume amplification during service status,prevented it from developing further.These difficulties can be successfully overcome by incorporating carbon into pure Si systems to form a composite anode and constructing a buffer structure.This review looks at the diffusion mechanism,various silicon-based anode material configurations(including sandwich,core-shell,yolk-shell,and other 3D mesh/porous structures),as well as the appropriate binders and electrolytes.Finally,a summary and viewpoints are offered on the characteristics and structural layout of various structures,metal/non-metal doping,and the compatibility and application of various binders and electrolytes for silicon-based anodes.This review aims to provide valuable insights into the research and development of silicon-based carbon anodes for high-performance lithium-ion batteries,as well as their integration with binders and electrolyte.
基金supported by the National Natural Science Foundation of China(Nos.52172243,52371215)。
文摘All-solid-state Li batteries(ASSLBs)using solid electrolytes(SEs)have gained significant attention in recent years considering the safety issue and their high energy density.Despite these advantages,the commercialization of ASSLBs still faces challenges regarding the electrolyte/electrodes interfaces and growth of Li dendrites.Elemental doping is an effective and direct method to enhance the performance of SEs.Here,we report an Al-F co-doping strategy to improve the overall properties including ion conductivity,high voltage stability,and cathode and anode compatibility.Particularly,the Al-F co-doping enables the formation of a thin Li-Al alloy layer and fluoride interphases,thereby constructing a relatively stable interface and promoting uniform Li deposition.The similar merits of Al-F co-doping are also revealed in the Li-argyrodite series.ASSLBs assembled with these optimized electrolytes gain good electrochemical performance,demonstrating the universality of Al-F co-doping towards advanced SEs.
基金Fundamental Research Funds for the Central Universities of China(Grant No. SWU-KT22030)Scientific and Technological Research Program of Chongqing Municipal Education Commission of China (No.KJQN202300205)financial support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under the project of 457444676。
文摘The development of flexible supercapacitors(FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and electrode materials stand as two key components that significantly impact the efficacy of hightemperature-tolerant FSCs(HT-FSCs). They should not only exhibit high electrochemical performance and excellent flexibility, but also withstand intense thermal stress. Considerable efforts have been devoted to enhancing their thermal stability while maintaining high electrochemical and mechanical performance. In this review, the fundamentals of HT-FSCs are outlined. A comprehensive overview of state-of-the-art progress and achievements in HT-FSCs, with a focus on thermally stable gel polymer electrolytes and electrode materials is provided. Finally, challenges and future perspectives regarding HT-FSCs are discussed, alongside strategies for elevating operational temperatures and performance.This review offers both theoretical foundations and practical guidelines for designing and manufacturing HT-FSCs, further promoting their widespread adoption across diverse fields.
基金supported by the National Key R&D Program of China(No.2021YFA1501003)。
文摘Electron transfer processes at polymer electrolyte/electrode interfaces play a central role in modern electrochemical devices of energy conversion,however,current understanding of electron transfers through electrochemical interfaces was established exclusively based on the studies of liquid/solid electrochemical interfaces.Thus,similarities and differences of liquid and polymer electrolyte/electrode interfaces need to be mapped out to guide the design of device level electrochemical interfaces.In this work,we employ the sulfonate adsorption/desorption as a probe reaction to understand the electron-transfer steps in polymer and liquid electrolytes.Through cyclic voltametric investigations on the well-define single-crystal Pd_(ML)Pt(111)electrode,we demonstrate that the oxidative adsorption and reductive desorption of sulfonates at the polymer electrolyte/electrode interface are chemically distinct from those in liquid electrolytes,with the former occurring mostly via the proton-coupled pathway while the latter proceeding mainly through the solvation-mediated pathway.Importantly,the sulfonate adsorption/desorption behaviors of alkylsulfonates become increasingly similar to those in Nafion with longer alkyl chains,suggesting that the interfacial hydrophobicity and solvation environment conferred by the perfluorinated polymer play a decisive role in the electron-transfer mechanism.Results reported in this study highlight the mechanistic distinctions between electron-transfer processes at electrochemical interfaces involving polymer and liquid electrolytes,and provide a framework for understanding electron-transfer processes at polymer electrolyte/electrode interfaces.
文摘The publisher regrets to inform that in the article of Advanced Powder Materials 4(2025)100261,the published Figs.3 and 5 belong to the initially submitted version,which should be replaced by the final version.The differences between the initial and final versions of these figures are described below.
基金National Natural Science Foundation of China (52073253)。
文摘Solid-state Na metal batteries(SSNBs),known for the low cost,high safety,and high energy density,hold a significant position in the next generation of rechargeable batteries.However,the urgent challenge of poor interfacial contact in solid-state electrolytes has hindered the commercialization of SSNBs.Driven by the concept of intimate electrode-electrolyte interface design,this study employs a combination of sodium-potassium(NaK)alloy and carbon nanotubes to prepare a semi-solid NaK(NKC)anode.Unlike traditional Na anodes,the paintable paste-like NKC anode exhibits superior adhesion and interface compatibility with both current collectors and gel electrolytes,significantly enhancing the physical contact of the electrode-electrolyte interface.Additionally,the filling of SiO_(2) nanoparticles improves the wettability of NaK alloy on gel polymer electrolytes,further achieving a conformal interface contact.Consequently,the overpotential of the NKC symmetric cell is markedly lower than that of the Na symmetric cell when subjected to a long cycle of 300 hrs.The full cell coupled with Na_(3)V_(2)(PO_(4))_(2) cathodes had an initial discharge capacity of 106.8 mAh·g^(-1) with a capacity retention of 89.61%after 300 cycles,and a high discharge capacity of 88.1 mAh·g^(-1) even at a high rate of 10 C.The outstanding electrochemical performance highlights the promising application potential of the NKC electrode.
基金financial support from the Project supported by the Southern Marine Science and Engineering Guangdong Lab-oratory(Zhuhai)(No.SML2023SP242)the National Natural Sci-ence Foundation of China(Nos.52274291 and 52204305)the Beijing Institute of Technology Research Fund Program for Young Scholars(No.1740011182102).
文摘Metal coating is a prevalent strategy for enhancing surface properties.Among the numerous methods for preparing coatings,electrodeposition stands out due to its simplicity,cost-effectiveness,and high efficiency,making it widely utilized in various metal coating applications.By meticulously selecting appropriate electrolytes and electrodeposition parameters,metal coatings with diverse structures and morphologies can be obtained,and tailored to meet specific performance requirements.As the demand for superior metal coating performance continues to rise,it is imperative to summarize and forecast electrodeposition techniques to meet the criteria for high quality and precision.This review delves into the electrodeposition preparation of several typical metal coatings in diverse electrolyte systems,including aqueous solutions,ionic liquids,deep eutectic solvents,and molten salts.We also examine the electrodeposition process on the cathode,elucidate the correlation between parameters and coating quality,and suggest future research directions.This review aims to provide valuable insights and guidance for the electrodeposition preparation of metal coatings.
基金supported by the National Natural Science Foundation of China(Grants Nos.12172102 and 12372097)the Fundamental Research Funds for the Central Universities(Grant No.HIT.OCEF.2022013).
文摘The silicon-graphite(Si-C)composite electrode is considered a promising candidate for next-generation commercial electrodes due to its high capacity.However,lithium-ion batteries with silicon electrodes often experience capacity fading and poor cyclic performance,primarily due to the mechanical degradation of the solid-electrolyte interphase(SEI).In this work,we present a homogenized constitutive model for Si-C composite electrodes under finite deformation,incorporating lithium-ion concentration-dependent properties.We perform a wrinkling analysis and systematically examine the influence of key parameters,such as modulus and thickness ratios,on the critical conditions for instability.Additionally,we investigate the ratcheting effect across varying silicon contents.Our findings reveal that maintaining the silicon content within an optimal range effectively reduces plastic accumulation during charge–discharge cycles.These insights provide crucial guidance for optimizing the design and fabrication of Si–C electrode systems,enhancing their durability and performance.
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 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 financial support from the Key Project of Shaanxi Provincial Natural Science Foundation-Key Project of Laboratory(2025SYS-SYSZD-117)the Natural Science Basic Research Program of Shaanxi(2025JCYBQN-125)+8 种基金Young Talent Fund of Xi'an Association for Science and Technology(0959202513002)the Key Industrial Chain Technology Research Program of Xi'an(24ZDCYJSGG0048)the Key Research and Development Program of Xianyang(L2023-ZDYF-SF-077)Postdoctoral Fellowship Program of CPSF(GZC20241442)Shaanxi Postdoctoral Science Foundation(2024BSHSDZZ070)Research Funds for the Interdisciplinary Projects,CHU(300104240913)the Fundamental Research Funds for the Central Universities,CHU(300102385739,300102384201,300102384103)the Scientific Innovation Practice Project of Postgraduate of Chang'an University(300103725063)the financial support from the Australian Research Council。
文摘Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temperature(LT)operation.Therefore,a more comprehensive and systematic understanding of LIB behavior at LT is urgently required.This review article comprehensively reviews recent advancements in electrolyte engineering strategies aimed at improving the low-temperature operational capabilities of LIBs.The study methodically examines critical performance-limiting mechanisms through fundamental analysis of four primary challenges:insufficient ionic conductivity under cryogenic conditions,kinetically hindered charge transfer processes,Li+transport limitations across the solidelectrolyte interphase(SEI),and uncontrolled lithium dendrite growth.The work elaborates on innovative optimization approaches encompassing lithium salt molecular design with tailored dissociation characteristics,solvent matrix optimization through dielectric constant and viscosity regulation,interfacial engineering additives for constructing low-impedance SEI layers,and gel-polymer composite electrolyte systems.Notably,particular emphasis is placed on emerging machine learning-guided electrolyte formulation strategies that enable high-throughput virtual screening of constituent combinations and prediction of structure-property relationships.These artificial intelligence-assisted rational design frameworks demonstrate significant potential for accelerating the development of next-generation LT electrolytes by establishing quantitative composition-performance correlations through advanced data-driven methodologies.
基金supported by the Innovation Capability Support Program of Shaanxi(No.2024CX-GXPT-12)the National Natural Science Foundation of China(No.22403074).
文摘Electrolytes play a key role in determining the electrochemical performance,safety,and lifespan of potassium-based batteries,making their selection and optimization a critical area of research.This study systematically investigates the effects of two major potassium-based battery electrolytes,potassium hexafluorophosphate(KPF_(6))and potassium difluorosulfonimide(KFSI)in ethylene carbonate/diethyl carbonate(EC/DEC)solvents,on battery performance,solid electrolyte interphase(SEI)stability,aluminum(Al)current collector corrosion behavior,electrochemical stability window,and dendrite growth issue.Experimental results reveal that KFSI electrolyte significantly outperforms KPF_(6)in terms of cycling stability,rate capability,and Coulombic efficiency(CE),primarily due to the formation of a high-quality SEI on electrode surface.Through X-ray photoelectron spectroscopy(XPS)and time-of-flight secondary ion mass spectrometry(TOF-SIMS)analyses,we construct the SEI structure for both electrolytes,and find that the SEI formed by KFSI is more uniform and stable.Additionally,KPF_(6)exhibits weaker corrosivity towards the Al current collector compared to KFSI due to the formation of an AlF_(3) layer with higher oxidation stability on Al surface.Furthermore,in-situ optical microscopy observations indicate that the dendrite growth in KFSI electrolyte is more uniform,preventing the aggregates.These findings provide essential experimental evidence and theoretical support for optimizing the electrolyte in potassium-based batteries.
基金supported by the National Natural Science Foundation of China(32501592,32271814,32301530,32471806)Young Elite Scientist Sponsorship Program by Cast(No.YESS20230242)+3 种基金Natural Science Foundation of Tianjin(23JCZDJC00630,24JCZDJC00630)the China Postdoctoral Science Foundation(2023M740563)Tianjin Enterprise Technology Commissioner Project(25YDTPJC00690)China Scholarship Council(202408120091,202408120105).
文摘The pursuit of high energy density and sustainable energy storage devices has been the target of many researchers.However,safety issues such as the susceptibility of conventional liquid electrolytes to leakage and flammability,as well as performance degradation due to uncontrollable dendrite growth in liquid electrolytes,have been limiting the further development of energy storage devices.In this regard,gel polymer electrolytes(GPEs)based on lignocellulosic(cellulose,hemicellulose,lignin)have attracted great interest due to their high thermal stability,excellent electrolyte wettability,and natural abundance.Therefore,in this critical review,a comprehensive overview of the current challenges faced by GPEs is presented,followed by a detailed description of the opportunities and advantages of lignocellulosic materials for the fabrication of GPEs for energy storage devices.Notably,the key properties and corresponding construction strategies of GPEs for energy storage are analyzed and discussed from the perspective of lignocellulose for the first time.Moreover,the future challenges and prospects of lignocellulose-mediated GPEs in energy storage applications are also critically reviewed and discussed.We sincerely hope this review will stimulate further research on lignocellulose-mediated GPEs in energy storage and provide meaningful directions for the strategy of designing advanced GPEs.
基金financially supported by Shenzhen Science and Technology Program(JCYJ20240813142900001)Guangdong Provincial Key Laboratory of New Energy Materials Service Safety。
文摘Chloride-based solid electrolytes are considered promising candidates for next-generation high-energy-density all-solid-state batteries(ASSBs).However,their relatively low oxidative decomposition threshold(~4.2 V vs.Li^(+)/Li)constrains their use in ultrahighvoltage systems(e.g.,4.8 V).In this work,ferroelectric Ba TiO_(3)(BTO)nanoparticles with optimized thickness of~50-100 nm were successfully coated onto Li_(2.5)Y_(0.5)Zr_(0.5)Cl_(6)(LYZC@5BTO)electrolytes using a time-efficient ball-milling process.The nanoparticle-induced interfacial ionic conduction enhancement mechanism contributed to the preservation of LYZC’s high ionic conductivity,which remained at 1.06 m S cm^(-1)for LYZC@5BTO.Furthermore,this surface electric field engineering strategy effectively mitigates the voltage-induced self-decomposition of chloride-based solid electrolytes,suppresses parasitic interfacial reactions with single-crystal NCM811(SCNCM811),and inhibits the irreversible phase transition of SCNCM811.Consequently,the cycling stability of LYZC under high-voltage conditions(4.8 V vs.Li+/Li)is significantly improved.Specifically,ASSB cells employing LYZC@5BTO exhibited a superior discharge capacity of 95.4 m Ah g^(-1)over 200 cycles at 1 C,way outperforming cell using pristine LYZC that only shows a capacity of 55.4 m Ah g^(-1).Furthermore,time-of-flight secondary ion mass spectrometry and X-ray photoelectron spectroscopy analysis revealed that Metal-O-Cl by-products from cumulative interfacial side reactions accounted for 6% of the surface species initially,rising to 26% after 200 cycles in pristine LYZC.In contrast,LYZC@5BTO limited this increase to only 14%,confirming the effectiveness of BTO in stabilizing the interfacial chemistry.This electric field modulation strategy offers a promising route toward the commercialization of high-voltage solid-state electrolytes and energy-dense ASSBs.
基金the financial support from the National Natural Science Foundation of China(52203123 and 52473248)State Key Laboratory of Polymer Materials Engineering(sklpme2024-2-04)+1 种基金the Fundamental Research Funds for the Central Universitiessponsored by the Double First-Class Construction Funds of Sichuan University。
文摘Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving the overall performance of CPEs due to their difficulty in achieving robust electrochemical and mechanical interfaces simultaneously.Here,by regulating the surface charge characteristics of halloysite nanotube(HNT),we propose a concept of lithium-ion dynamic interface(Li^(+)-DI)engineering in nano-charged CPE(NCCPE).Results show that the surface charge characteristics of HNTs fundamentally change the Li^(+)-DI,and thereof the mechanical and ion-conduction behaviors of the NCCPEs.Particularly,the HNTs with positively charged surface(HNTs+)lead to a higher Li^(+)transference number(0.86)than that of HNTs-(0.73),but a lower toughness(102.13 MJ m^(-3)for HNTs+and 159.69 MJ m^(-3)for HNTs-).Meanwhile,a strong interface compatibilization effect by Li^(+)is observed for especially the HNTs+-involved Li^(+)-DI,which improves the toughness by 2000%compared with the control.Moreover,HNTs+are more effective to weaken the Li^(+)-solvation strength and facilitate the formation of Li F-rich solid-electrolyte interphase of Li metal compared to HNTs-.The resultant Li|NCCPE|LiFePO4cell delivers a capacity of 144.9 m Ah g^(-1)after 400 cycles at 0.5 C and a capacity retention of 78.6%.This study provides deep insights into understanding the roles of surface charges of nanofillers in regulating the mechanical and electrochemical interfaces in ASSLMBs.
基金granted by the National Natural Science Foundation of China(Nos.52533008,21835003,62274097,and 62004106)National Key Research and Development Program of China(Nos.2024YFB3612500,2024YFB3612600,and 2023YFB3608900)+2 种基金Basic Research Program of Jiangsu Province(No.BK20243057)Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX25_1213)the Natural Science Foundation of Nanjing Universityof Posts and Telecommunications(No.NY225135).
文摘To meet the growing needs of flexible and wearable electronics,stretchable energy storage devices—especially supercapacitors(SCs)—have become a key focus in advanced energy storage research.However,achieving both mechanical stretchability and high capacitance in SC still faces great challenges,and the crucial factors lie in creating superior electrode materials that exhibit high electrochemical performance as well as excellent mechanical stretchability.Covalent organic frameworks(COFs)possess considerable potential as electrode materials for SCs by virtue of stable organic frameworks,open channels and designable functional groups.Nevertheless,their applications in flexible SCs are greatly hindered by their rigid characteristics.Here a novel COFs@conductive polymer hydrogels(CPHs)@poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)complexes,which integrate the pseudocapacitance of PDITAPA COF,mechanical stretchability of hydrogels and high conductivity of PEDOT:PSS,has been developed as stretchable electrode of SCs.Physically cross-linked PEDOT nanofibers,with their interlinked and entangled architecture,collectively boost mechanical,electrical,and electrochemical performance.The COFs@CPHs@PEDOT:PSS simultaneously demonstrates outstanding mechanical stretchability,high electrical behaviors,and superior swelling characteristics.The resulting SC exhibits advantages of simple structures,facile assembly processes,high specific capacitance,excellent cycling stability,and arbitrary deformation,which holds great application prospects for wearable electronic products.Owing to its uncomplicated structure,ease of production,high energy storage capacity,robust cycling performance,and adaptability to deformation,this fabricated SC is well-suited for next-generation wearable technologies.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.NRF-2021M3H4A1A02048529)the Ministry of Trade,Industry and Energy(MOTIE)of the Korean government under grant No.RS-2022-00155854support from the DGIST Supercomputing and Big Data Center.
文摘To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as well.Herein,we suggest an effective approach to control the micropore structure of silicon oxide(SiO_(x))/artificial graphite(AG)composite electrodes using a perforated current collector.The electrode features a unique pore structure,where alternating high-porosity domains and low-porosity domains markedly reduce overall electrode resistance,leading to a 20%improvement in rate capability at a 5C-rate discharge condition.Using microstructure-resolved modeling and simulations,we demonstrate that the patterned micropore structure enhances lithium-ion transport,mitigating the electrolyte concentration gradient of lithium-ion.Additionally,perforating current collector with a chemical etching process increases the number of hydrogen bonding sites and enlarges the interface with the SiO_(x)/AG composite electrode,significantly improving adhesion strength.This,in turn,suppresses mechanical degradation and leads to a 50%higher capacity retention.Thus,regularly arranged micropore structure enabled by the perforated current collector successfully improves both rate capability and cycle life in SiO_(x)/AG composite electrodes,providing valuable insights into electrode engineering.
基金Project(20973124)supported by the National Natural Science Foundation of ChinaProject supported by Key Laboratory of Superlight Materials and Surface Technology,Ministry of Education(Harbin Engineering University),China
文摘A novel type of porous magnesium electrode with a stable 3D copper foam as current collectors for the organic magnesium-air battery was prepared by both amperostatic and pulsed electrodeposition of magnesium on copper foam substrates in an electrolyte of 1 mol/L EtMgBr/THF solution, respectively. Optimal parameters of the pulsed electrodeposition were obtained using a bending cathode at the right angle. The surface morphology of the porous electrode was investigated by SEM, and the discharging performance of the porous magnesium electrode was detected by the chronoamperometric measurement. The electrochemical stability of 3D copper foam current collectors was examined by cyclic voltammetry, SEM and ICP-OES analyses. The results show that the rate capability of the porous magnesium electrode with a stable 3D copper foam as a current collector is better than that of the planar magnesium electrode, and the rate capability of the porous magnesium electrode prepared by the pulsed electrodeposition is superior to that of the porous magnesium electrode prepared by the amperostatic electrodeposition. The 3D structure of copper foam current collectors of the porous magnesium electrode could keep stable during the discharging process.
