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
High-voltage sodium-ion batteries(SIBs)are emerging as promising candidates for large-scale energy storage systems due to their abundant sodium source and high energy density.However,the instability of the electrode e...High-voltage sodium-ion batteries(SIBs)are emerging as promising candidates for large-scale energy storage systems due to their abundant sodium source and high energy density.However,the instability of the electrode electrolyte interphase remains a critical barrier to the potential use of high-voltage SIBs.Herein,sodium difluorophosphate(NaDFP)and fluoroethylene carbonate(FEC)serve as functional electrolyte additives to stabilize the interface of the high-voltage cathode.The oxidative competition between FEC and NaDFP facilitates the robust formation of the cathode-electrolyte interface(CEI)layer,enriched with inorganic components such as NaF/NaPO_(x)F_(y).The highly conductive NaF/NaPO_(x)F_(y)and inorganics provide fast ion transport pathways and mechanical strength,thereby mitigating the decomposition of carbonates and NaPF_(6).The half-cell equipped with BE 2 F+0.5 DFP demonstrates 93.9%capacity retention at 4.3 V across 600 cycles,showcasing excellent cycling capability.Full HC||NVOPF cells exhibit sustained performance with 91.69%capacity retention and a capacity of 91.57 mA·h/g over 1000 cycles at a 5 C rate.This study is poised to garner increased scholarly interest in the domain of rational electrolyte formulation for practical applications.展开更多
High energy density lithium-ion batteries using Ni-rich cathode(such as LiNi0.6Co0.2Mn0.2O2) suffer from severe capacity decay.P-toluenesulfonyl fluoride(pTSF) has been investigated as a novel film-forming electrolyte...High energy density lithium-ion batteries using Ni-rich cathode(such as LiNi0.6Co0.2Mn0.2O2) suffer from severe capacity decay.P-toluenesulfonyl fluoride(pTSF) has been investigated as a novel film-forming electrolyte additive to enhance the cycling performances of graphite/LiNi0.6Co0.2Mn0.2O2 pouch cell.In comparison with the baseline electrolyte,a small dose of pTSF can significantly improve the cyclic stability of the cell.Theoretical calculations together with experimental results indicate that pTSF would be oxidized and reduced to construct protective interphase film on the surfaces of LiNi0.6Co0.2Mn0.2O2 cathode and graphite anode,respectively.These S-containing surface films derived from pTSF effectively mitigate the decomposition of electrolyte,reduce the interphasial impedance,as well as prevent the dissolution of transition metal ions from Ni-rich cathode upon cycling at high voltage.This finding is beneficial for the practical application of high energy density graphite/LiNi0.6Co0.2Mn0.2O2 cells.展开更多
Since the electrode/electrolyte interface(EEI)is the main redox center of electrochemical processes,proper manipulation of the EEI microenvironment is crucial to stabilize interfacial behaviors.Here,a finger-paint met...Since the electrode/electrolyte interface(EEI)is the main redox center of electrochemical processes,proper manipulation of the EEI microenvironment is crucial to stabilize interfacial behaviors.Here,a finger-paint method is proposed to enable quick physical modification of glass-fiber separator without complicated chemical technology to modulate EEI of bilateral electrodes for aqueous zinc-ion batteries(ZIBs).An elaborate biochar derived from Aspergillus Niger is exploited as the modification agent of EEI,in which the multi-functional groups assist to accelerate Zn^(2+)desolvation and create a hydrophobic environment to homogenize the deposition behavior of Zn anode.Importantly,the finger-paint interface on separator can effectively protect cathodes from abnormal capacity fluctuation and/or rapid attenuation induced by H_(2)O molecular on the interface,which is demonstrated in modified MnO_(2),V_(2)O_(5),and KMn HCF-based cells.The as-proposed finger-paint method opens a new idea of bilateral interface engineering to facilitate the access to the practical application of the stable zinc electrochemistry.展开更多
Si(111)electrode has been widely used in electrochemical and photoelectrochemical studies.The potential dependent measurements of the second harmonic generation(SHG)were performed to study Si(111)electrode interface.A...Si(111)electrode has been widely used in electrochemical and photoelectrochemical studies.The potential dependent measurements of the second harmonic generation(SHG)were performed to study Si(111)electrode interface.At different azimuthal angles of the Si(111)and under different polarization combinations,the curve of the intensity of SHG with extern potential has a different form of line or parabola.Quantitative analysis showed that these differences in the potential-dependence can be explained by the isotropic and anisotropic contribution of the Si(111)electrode.The change in the isotropic and anisotropic contribution of the Si(111)electrode may be attributed to the increase in the doping concentration of Si(111)electrodes.展开更多
The high concentration electrolytes with specific solvation structure could passivate the electrodes to prolong battery cycle life but at the expense of increased cost,which limits the wide application in commercializ...The high concentration electrolytes with specific solvation structure could passivate the electrodes to prolong battery cycle life but at the expense of increased cost,which limits the wide application in commercialization.The regular concentration(1_(M))electrolytes with suitable properties(viscosity,ionic conductivity,etc.)are cost-guaranteed,but undesired reactions would always occur and lead to battery degradation during long cycles.To promote the long-term cycle stability in a cost-effective way,this work constructs bidirectional fluorine-rich electrode/electrolyte interphase(EEI)by redistribution of solvents and electrochemical induction.The fluorinated effect with reasonable zoning planning restricts morphological disintegration,meanwhile,forms spatial confinement on cathode.In particular,the obtained cathode electrolyte interphase(CEI)gets the ample ability of Na^(+)transport,which benefits from the fluorinated organics arranged in the epitaxy and the hemi-carbonate content acting on the thickness.Thus,the electrochemical long cycling performance of F-NVPOFⅡF-CC full cells is significantly enhanced(the decay rate at 1 C per cycle is as low as 0.01%).Such a fluorine-rich EEI engineering is expected to take transitional layers against the degradation of cells and make ultra-long cycle batteries possible.展开更多
Electrocatalytic CO_(2) reduction(ECR)is a promising approach to converting CO_(2) into chemicals and fuels.Among the ECR products,C_(2) products such as ethylene,ethanol,and acetate have been extensively studied due ...Electrocatalytic CO_(2) reduction(ECR)is a promising approach to converting CO_(2) into chemicals and fuels.Among the ECR products,C_(2) products such as ethylene,ethanol,and acetate have been extensively studied due to their high industrial demands.However,the mechanistic understanding of C_(2) product formation remains unclear due to the lack of in situ or operando measurements that can observe the complex and instantaneous atomic evolutions of adsorbates at the electrode/electrolyte interface.Moreover,the sensitivity of ECR reactions to variations at the interface further widens the gap between mechanistic understanding and performance enhancement.To bridge this gap,first-principle studies provide insights into how the interface influences ECR.In this study,we present a review of mechanistic studies investigating the effects of various factors at the interface,with an emphasis on the C_(2) product formation.We begin by introducing ECR and the essential metrics.Next,we discuss the factors classified by their components at the interface,namely,electrocatalyst,electrolyte,and adsorbates,respectively,and their effects on the C_(2) product formation.Due to the interplay among these factors,we aim to deconvolute the influence of each factor and clearly demonstrate their impacts.Finally,we outline the promising directions for mechanistic studies of C_(2) products.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 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
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
The deoxygenation of organic acids, important biomass feedstocks and derivatives, to synthesize hydrocarbon products under mild electrochemical conditions, holds significant importance for the production of carbon-neu...The deoxygenation of organic acids, important biomass feedstocks and derivatives, to synthesize hydrocarbon products under mild electrochemical conditions, holds significant importance for the production of carbon-neutral biofuels. There is still limited research on the influential factors of the electrochemical decarboxylation reaction of medium-chain fatty acids. In this study, n-octanoic acid (OA) was chosen as the research subject to investigate the electrochemical decarboxylation behavior of OA on a platinum electrode, focusing on the influence of different alkali metal cations (Li^(+), Na^(+), K^(+)), common anions (SO^(4)^(2−), Cl^(−)), and electrolyte pH. It was found that KOH as an electrolyte exhibited the best performance for OA. Possibly, the larger size of K^(+) increased the alkalinity of the electrode surface, facilitating OA deprotonation. LiOH electrolyte reduced the solubility of OA, thereby inhibiting the decarboxylation reaction. SO^(4)^(2−) exhibited a weak promoting effect on the decarboxylation reaction of OA, while Cl^(−) showed no adverse effect although Cl^(−) may adsorb on the electrode surface. Furthermore, unlike short-chain fatty acids, medium-chain OA can only achieve efficient decarboxylation under alkaline conditions due to its solubility properties. This study provides references and foundations for future efforts to enhance the efficiency of electrochemical decarboxylation synthesis of hydrocarbon biofuels from medium-chain fatty acids.展开更多
A suitable interface between the electrode and electrolyte is crucial in achieving highly stable electrochemical performance for Li-ion batteries,as facile ionic transport is required.Intriguing research and developme...A suitable interface between the electrode and electrolyte is crucial in achieving highly stable electrochemical performance for Li-ion batteries,as facile ionic transport is required.Intriguing research and development have recently been conducted to form a stable interface between the electrode and electrolyte.Therefore,it is essential to investigate emerging knowledge and contextualize it.The nanoengineering of the electrode-electrolyte interface has been actively researched at the electrode/electrolyte and interphase levels.This review presents and summarizes some recent advances aimed at nanoengineering approaches to build a more stable electrode-electrolyte interface and assess the impact of each approach adopted.Furthermore,future perspectives on the feasibility and practicality of each approach will also be reviewed in detail.Finally,this review aids in projecting a more sustainable research pathway for a nanoengineered interphase design between electrode and electrolyte,which is pivotal for high-performance,thermally stable Li-ion batteries.展开更多
FeS_(2)cathode is promising for all-solid-state lithium batteries due to its ultra-high capacity,low cost,and environmental friendliness.However,the poor performances,induced by limited electrode-electrolyte interface...FeS_(2)cathode is promising for all-solid-state lithium batteries due to its ultra-high capacity,low cost,and environmental friendliness.However,the poor performances,induced by limited electrode-electrolyte interface,severe volume expansion,and polysulfide shuttle,hinder the application of FeS_(2)in all-solid-state lithium batteries.Herein,an integrated 3D FeS_(2)electrode with full infiltration of Li6PS5Cl sulfide electrolytes is designed to address these challenges.Such a 3D integrated design not only achieves intimate and maximized interfacial contact between electrode and sulfide electrolytes,but also effectively buffers the inner volume change of FeS_(2)and completely eliminates the polysulfide shuttle through direct solid-solid conversion of Li2S/S.Besides,the vertical 3D arrays guarantee direct electron transport channels and horizontally shortened ion diffusion paths,endowing the integrated electrode with a remarkably reduced interfacial impedance and enhanced reaction kinetics.Benefiting from these synergies,the integrated all-solid-state lithium battery exhibits the largest reversible capacity(667 mAh g^(-1)),best rate performance,and highest capacity retention of 82%over 500 cycles at 0.1 C compared to both a liquid battery and non-integrated all-solid-state lithium battery.The cycling performance is among the best reported for FeS_(2)-based all-solid-state lithium batteries.This work presents an innovative synergistic strategy for designing long-cycling high-energy all-solid-state lithium batteries,which can be readily applied to other battery systems,such as lithium-sulfur batteries.展开更多
A 2D transient mathematical model was established to separately describe the anode bubble dynamics and the bubbleinduced electrolyte motion in the rare earth electrolysis cell with horizontal electrode.Results indicat...A 2D transient mathematical model was established to separately describe the anode bubble dynamics and the bubbleinduced electrolyte motion in the rare earth electrolysis cell with horizontal electrode.Results indicate that with the increase in the anode inclined angle,the maximum bubble thickness is increased gradually.Furthermore,compared with the conventional anode,the inclined and chamfered anodes are conductive to the bubble length reduction and the bubble velocity improvement.Meanwhile,the bubble-induced electrolyte motion in the electrolysis cell can improve the distribution and transport process of oxyfluorides,thereby enhancing the current efficiency.Finally,a novel feeding method based on the electrolyte flow is proposed.展开更多
The battery energy density can be improved by raising the operating voltage,however,which may lead to rapid capacity decay due to the continuous electrolyte decomposition and the thickening of electrode electrolyte in...The battery energy density can be improved by raising the operating voltage,however,which may lead to rapid capacity decay due to the continuous electrolyte decomposition and the thickening of electrode electrolyte interphases.To address these challenges,we proposed tripropyl phosphate(TPP)as an additive-regulating Li~+solvation structure to construct a stable Li F–rich electrode carbonate-based electrolyte interphases for sustaining 4.6 V Li||LiCoO_(2)batteries.This optimized interphases could help reduce the resistance and achieve better rate performance and cycling stability.As expected,the Li||LiCoO_(2)battery retained 79.4%capacity after 100 cycles at 0.5 C,while the Li||Li symmetric cell also kept a stable plating/stripping process over 450 h at the current density of 1.0 mA/cm^(2)with a deposited amount of0.5 mAh/cm^(2).展开更多
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Project(2023QNRC001)supported by the Young Elite Scientists Sponsorship Program by CAST,ChinaProject(51932011)supported by the National Natural Science Foundation of China+1 种基金Project(2023JJ10060)supported by the Natural Science Foundation of Hunan Province,ChinaProject(23A0003)supported by the Scientific Research Fund of Hunan Provincial Education Department,China。
文摘High-voltage sodium-ion batteries(SIBs)are emerging as promising candidates for large-scale energy storage systems due to their abundant sodium source and high energy density.However,the instability of the electrode electrolyte interphase remains a critical barrier to the potential use of high-voltage SIBs.Herein,sodium difluorophosphate(NaDFP)and fluoroethylene carbonate(FEC)serve as functional electrolyte additives to stabilize the interface of the high-voltage cathode.The oxidative competition between FEC and NaDFP facilitates the robust formation of the cathode-electrolyte interface(CEI)layer,enriched with inorganic components such as NaF/NaPO_(x)F_(y).The highly conductive NaF/NaPO_(x)F_(y)and inorganics provide fast ion transport pathways and mechanical strength,thereby mitigating the decomposition of carbonates and NaPF_(6).The half-cell equipped with BE 2 F+0.5 DFP demonstrates 93.9%capacity retention at 4.3 V across 600 cycles,showcasing excellent cycling capability.Full HC||NVOPF cells exhibit sustained performance with 91.69%capacity retention and a capacity of 91.57 mA·h/g over 1000 cycles at a 5 C rate.This study is poised to garner increased scholarly interest in the domain of rational electrolyte formulation for practical applications.
基金supported by the National Natural Science Foundation of China (21573080)the Guangdong Program for Support of Distinguished Young Scholar (2017B030306013)the Science and Technology Planning Project of Guangdong Province (2017B090901020)。
文摘High energy density lithium-ion batteries using Ni-rich cathode(such as LiNi0.6Co0.2Mn0.2O2) suffer from severe capacity decay.P-toluenesulfonyl fluoride(pTSF) has been investigated as a novel film-forming electrolyte additive to enhance the cycling performances of graphite/LiNi0.6Co0.2Mn0.2O2 pouch cell.In comparison with the baseline electrolyte,a small dose of pTSF can significantly improve the cyclic stability of the cell.Theoretical calculations together with experimental results indicate that pTSF would be oxidized and reduced to construct protective interphase film on the surfaces of LiNi0.6Co0.2Mn0.2O2 cathode and graphite anode,respectively.These S-containing surface films derived from pTSF effectively mitigate the decomposition of electrolyte,reduce the interphasial impedance,as well as prevent the dissolution of transition metal ions from Ni-rich cathode upon cycling at high voltage.This finding is beneficial for the practical application of high energy density graphite/LiNi0.6Co0.2Mn0.2O2 cells.
基金financial support from the National Natural Science Foundation of China (21571080 and 52202253)the Natural Science Foundation of Jiangsu Province (BK20220914)+2 种基金Project funded by China Postdoctoral Science Foundation (2022M721593)the Jiangsu Funding Program for Excellent Postdoctoral Talent (2022ZB193)the financial support from International Center of Future Science,Jilin University,Changchun,P.R.China (ICFS Seed Funding for Young Researchers)。
文摘Since the electrode/electrolyte interface(EEI)is the main redox center of electrochemical processes,proper manipulation of the EEI microenvironment is crucial to stabilize interfacial behaviors.Here,a finger-paint method is proposed to enable quick physical modification of glass-fiber separator without complicated chemical technology to modulate EEI of bilateral electrodes for aqueous zinc-ion batteries(ZIBs).An elaborate biochar derived from Aspergillus Niger is exploited as the modification agent of EEI,in which the multi-functional groups assist to accelerate Zn^(2+)desolvation and create a hydrophobic environment to homogenize the deposition behavior of Zn anode.Importantly,the finger-paint interface on separator can effectively protect cathodes from abnormal capacity fluctuation and/or rapid attenuation induced by H_(2)O molecular on the interface,which is demonstrated in modified MnO_(2),V_(2)O_(5),and KMn HCF-based cells.The as-proposed finger-paint method opens a new idea of bilateral interface engineering to facilitate the access to the practical application of the stable zinc electrochemistry.
基金supported by the National Natural Science Foundation of China(No.21673251,No.21773258,No.21873104,and No.91856121)the Chinese Academy of Sciences(No.JKYYQ20180014)。
文摘Si(111)electrode has been widely used in electrochemical and photoelectrochemical studies.The potential dependent measurements of the second harmonic generation(SHG)were performed to study Si(111)electrode interface.At different azimuthal angles of the Si(111)and under different polarization combinations,the curve of the intensity of SHG with extern potential has a different form of line or parabola.Quantitative analysis showed that these differences in the potential-dependence can be explained by the isotropic and anisotropic contribution of the Si(111)electrode.The change in the isotropic and anisotropic contribution of the Si(111)electrode may be attributed to the increase in the doping concentration of Si(111)electrodes.
基金supported by the National Natural Science Foundation of China(No.91963118 and 52102213)Science Technology Program of Jilin Province(No.20200201066JC)the 111 Project(No.B13013).
文摘The high concentration electrolytes with specific solvation structure could passivate the electrodes to prolong battery cycle life but at the expense of increased cost,which limits the wide application in commercialization.The regular concentration(1_(M))electrolytes with suitable properties(viscosity,ionic conductivity,etc.)are cost-guaranteed,but undesired reactions would always occur and lead to battery degradation during long cycles.To promote the long-term cycle stability in a cost-effective way,this work constructs bidirectional fluorine-rich electrode/electrolyte interphase(EEI)by redistribution of solvents and electrochemical induction.The fluorinated effect with reasonable zoning planning restricts morphological disintegration,meanwhile,forms spatial confinement on cathode.In particular,the obtained cathode electrolyte interphase(CEI)gets the ample ability of Na^(+)transport,which benefits from the fluorinated organics arranged in the epitaxy and the hemi-carbonate content acting on the thickness.Thus,the electrochemical long cycling performance of F-NVPOFⅡF-CC full cells is significantly enhanced(the decay rate at 1 C per cycle is as low as 0.01%).Such a fluorine-rich EEI engineering is expected to take transitional layers against the degradation of cells and make ultra-long cycle batteries possible.
基金supported by the National Research Foundation Singapore Investigatorship Program(Grant No.NRF-NRFI08-2022-0009)A*STAR(Agency for Science,Technology and Research)LCER FI program(Award No.U2102d2002)the E-CO2RR CREATE Program.
文摘Electrocatalytic CO_(2) reduction(ECR)is a promising approach to converting CO_(2) into chemicals and fuels.Among the ECR products,C_(2) products such as ethylene,ethanol,and acetate have been extensively studied due to their high industrial demands.However,the mechanistic understanding of C_(2) product formation remains unclear due to the lack of in situ or operando measurements that can observe the complex and instantaneous atomic evolutions of adsorbates at the electrode/electrolyte interface.Moreover,the sensitivity of ECR reactions to variations at the interface further widens the gap between mechanistic understanding and performance enhancement.To bridge this gap,first-principle studies provide insights into how the interface influences ECR.In this study,we present a review of mechanistic studies investigating the effects of various factors at the interface,with an emphasis on the C_(2) product formation.We begin by introducing ECR and the essential metrics.Next,we discuss the factors classified by their components at the interface,namely,electrocatalyst,electrolyte,and adsorbates,respectively,and their effects on the C_(2) product formation.Due to the interplay among these factors,we aim to deconvolute the influence of each factor and clearly demonstrate their impacts.Finally,we outline the promising directions for mechanistic studies of C_(2) products.
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 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(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The authors gratefully acknowledge the financial support from Shanghai Pujiang Program(20PJ1404800)“Scientific and Technical Innovation Action Plan”Basic Research Field of Shanghai Science and Technology Committee(19JC1410500).
文摘The deoxygenation of organic acids, important biomass feedstocks and derivatives, to synthesize hydrocarbon products under mild electrochemical conditions, holds significant importance for the production of carbon-neutral biofuels. There is still limited research on the influential factors of the electrochemical decarboxylation reaction of medium-chain fatty acids. In this study, n-octanoic acid (OA) was chosen as the research subject to investigate the electrochemical decarboxylation behavior of OA on a platinum electrode, focusing on the influence of different alkali metal cations (Li^(+), Na^(+), K^(+)), common anions (SO^(4)^(2−), Cl^(−)), and electrolyte pH. It was found that KOH as an electrolyte exhibited the best performance for OA. Possibly, the larger size of K^(+) increased the alkalinity of the electrode surface, facilitating OA deprotonation. LiOH electrolyte reduced the solubility of OA, thereby inhibiting the decarboxylation reaction. SO^(4)^(2−) exhibited a weak promoting effect on the decarboxylation reaction of OA, while Cl^(−) showed no adverse effect although Cl^(−) may adsorb on the electrode surface. Furthermore, unlike short-chain fatty acids, medium-chain OA can only achieve efficient decarboxylation under alkaline conditions due to its solubility properties. This study provides references and foundations for future efforts to enhance the efficiency of electrochemical decarboxylation synthesis of hydrocarbon biofuels from medium-chain fatty acids.
基金supported by funding from Bavarian Center for Battery Technology(Baybatt,Hightech Agenda Bayern)and Bayerisch-Tschechische Hochschulagentur(BTHA)(BTHA-AP-202245,BTHA-AP-2023-5,and BTHA-AP-2023-12)supported by the University of Bayreuth-Deakin University Joint Ph.D.Program+1 种基金supported by the Regional Innovation Strategy(RIS)through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(MOE)(2021RIS-003)supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.RS2023-00213749)
文摘A suitable interface between the electrode and electrolyte is crucial in achieving highly stable electrochemical performance for Li-ion batteries,as facile ionic transport is required.Intriguing research and development have recently been conducted to form a stable interface between the electrode and electrolyte.Therefore,it is essential to investigate emerging knowledge and contextualize it.The nanoengineering of the electrode-electrolyte interface has been actively researched at the electrode/electrolyte and interphase levels.This review presents and summarizes some recent advances aimed at nanoengineering approaches to build a more stable electrode-electrolyte interface and assess the impact of each approach adopted.Furthermore,future perspectives on the feasibility and practicality of each approach will also be reviewed in detail.Finally,this review aids in projecting a more sustainable research pathway for a nanoengineered interphase design between electrode and electrolyte,which is pivotal for high-performance,thermally stable Li-ion batteries.
基金supported by the National Natural Science Foundation of China(Grant nos.52272201,52072136,52172229,52302303,and 51972257)Yanchang Petroleum-WHUT Joint Program(yc-whlg-2022ky-05)+1 种基金the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(Wuhan University of Technology,2022-KF-20)Fundamental Research Funds for the Central Universities(2023IVA106)for financial support
文摘FeS_(2)cathode is promising for all-solid-state lithium batteries due to its ultra-high capacity,low cost,and environmental friendliness.However,the poor performances,induced by limited electrode-electrolyte interface,severe volume expansion,and polysulfide shuttle,hinder the application of FeS_(2)in all-solid-state lithium batteries.Herein,an integrated 3D FeS_(2)electrode with full infiltration of Li6PS5Cl sulfide electrolytes is designed to address these challenges.Such a 3D integrated design not only achieves intimate and maximized interfacial contact between electrode and sulfide electrolytes,but also effectively buffers the inner volume change of FeS_(2)and completely eliminates the polysulfide shuttle through direct solid-solid conversion of Li2S/S.Besides,the vertical 3D arrays guarantee direct electron transport channels and horizontally shortened ion diffusion paths,endowing the integrated electrode with a remarkably reduced interfacial impedance and enhanced reaction kinetics.Benefiting from these synergies,the integrated all-solid-state lithium battery exhibits the largest reversible capacity(667 mAh g^(-1)),best rate performance,and highest capacity retention of 82%over 500 cycles at 0.1 C compared to both a liquid battery and non-integrated all-solid-state lithium battery.The cycling performance is among the best reported for FeS_(2)-based all-solid-state lithium batteries.This work presents an innovative synergistic strategy for designing long-cycling high-energy all-solid-state lithium batteries,which can be readily applied to other battery systems,such as lithium-sulfur batteries.
基金National Natural Science Foundation of China(52101165)Inner Mongolia Science and Technology Major Project(2020ZD0010)Key Research Program of the Chinese Academy of Sciences(ZDRW-CN-2021-3)。
文摘A 2D transient mathematical model was established to separately describe the anode bubble dynamics and the bubbleinduced electrolyte motion in the rare earth electrolysis cell with horizontal electrode.Results indicate that with the increase in the anode inclined angle,the maximum bubble thickness is increased gradually.Furthermore,compared with the conventional anode,the inclined and chamfered anodes are conductive to the bubble length reduction and the bubble velocity improvement.Meanwhile,the bubble-induced electrolyte motion in the electrolysis cell can improve the distribution and transport process of oxyfluorides,thereby enhancing the current efficiency.Finally,a novel feeding method based on the electrolyte flow is proposed.
基金supported by the National Natural Science Foundation of China(No.U21A20311)the Distinguished Scientist Fellowship Program(DSFP)at King Saud University,Riyadh,Saudi Arabia。
文摘The battery energy density can be improved by raising the operating voltage,however,which may lead to rapid capacity decay due to the continuous electrolyte decomposition and the thickening of electrode electrolyte interphases.To address these challenges,we proposed tripropyl phosphate(TPP)as an additive-regulating Li~+solvation structure to construct a stable Li F–rich electrode carbonate-based electrolyte interphases for sustaining 4.6 V Li||LiCoO_(2)batteries.This optimized interphases could help reduce the resistance and achieve better rate performance and cycling stability.As expected,the Li||LiCoO_(2)battery retained 79.4%capacity after 100 cycles at 0.5 C,while the Li||Li symmetric cell also kept a stable plating/stripping process over 450 h at the current density of 1.0 mA/cm^(2)with a deposited amount of0.5 mAh/cm^(2).
