As battery technology evolves and demand for efficient energy storage solutions,aqueous zinc ion batteries(AZIBs)have garnered significant attention due to their safety and environmental benefits.However,the stability...As battery technology evolves and demand for efficient energy storage solutions,aqueous zinc ion batteries(AZIBs)have garnered significant attention due to their safety and environmental benefits.However,the stability of cathode materials under high-voltage conditions remains a critical challenge in improving its energy density.This review systematically explores the failure mechanisms of high-voltage cathode materials in AZIBs,including hydrogen evolution reaction,phase transformation and dissolution phenomena.To address these challenges,we propose a range of advanced strategies aimed at improving the stability of cathode materials.These strategies include surface coating and doping techniques designed to fortify the surface properties and structure integrity of the cathode materials under high-voltage conditions.Additionally,we emphasize the importance of designing antioxidant electrolytes,with a focus on understanding and optimizing electrolyte decomposition mechanisms.The review also highlights the significance of modifying conductive agents and employing innovative separators to further enhance the stability of AZIBs.By integrating these cutting-edge approaches,this review anticipates substantial advancements in the stability of high-voltage cathode materials,paving the way for the broader application and development of AZIBs in energy storage.展开更多
In recent years,sodium-ion batteries(SIBs)have become one of the hot discussions and have gradually moved toward industrialization.However,there are still some shortcomings in their performance that have not been well...In recent years,sodium-ion batteries(SIBs)have become one of the hot discussions and have gradually moved toward industrialization.However,there are still some shortcomings in their performance that have not been well addressed,including phase transition,structural degradation,and voltage platform.High entropy materials have recently gained significant attention from researchers due to their effects on thermodynamics,dynamics,structure,and performance.Researchers have attempted to use these materials in sodium-ion batteries to overcome their problems,making it a modification method.This paper aims to discuss the research status of high-entropy cathode materials for sodium-ion batteries and summarize their effects on sodium-ion batteries from three perspectives:Layered oxide,polyanion,and Prussian blue.The infiuence on material structure,the inhibition of phase transition,and the improvement of ion diffusivity are described.Finally,the advantages and disadvantages of high-entropy cathode materials for sodium-ion batteries are summarized,and their future development has prospected.展开更多
A tunable oxidization and reduction strategy was proposed to directly regenerate spent LiFePO_(4)/C cathode materials by oxidizing excessive carbon powders with the addition of FePO_(4).Experimental results indicate t...A tunable oxidization and reduction strategy was proposed to directly regenerate spent LiFePO_(4)/C cathode materials by oxidizing excessive carbon powders with the addition of FePO_(4).Experimental results indicate that spent LiFePO_(4)/C cathode materials with good performance can be regenerated by roasting at 650℃ for 11 h with the addition ofLi_(2)CO_(3),FePO_(4),V_(2)O_(5),and glucose.V_(2)O_(5) is added to improve the cycle performance of regenerated cathode materials.Glucose is used to revitalize the carbon layers on the surface of spent LiFePO_(4)/C particles for improving their conductivity.The regenerated V-doped LiFePO_(4)/C shows an excellent electrochemical performance with the discharge specific capacity of 161.36 mA·h/g at 0.2C,under which the capacity retention is 97.85%after 100 cycles.展开更多
Rechargeable magnesium batteries(RMBs)have been considered a promising“post lithium-ion battery”system to meet the rapidly increasing demand of the emerging electric vehicle and grid energy storage market.However,th...Rechargeable magnesium batteries(RMBs)have been considered a promising“post lithium-ion battery”system to meet the rapidly increasing demand of the emerging electric vehicle and grid energy storage market.However,the sluggish diffusion kinetics of bivalent Mg^(2+)in the host material,related to the strong Coulomb effect between Mg^(2+)and host anion lattices,hinders their further development toward practical applications.Defect engineering,regarded as an effective strategy to break through the slow migration puzzle,has been validated in various cathode materials for RMBs.In this review,we first thoroughly understand the intrinsic mechanism of Mg^(2+)diffusion in cathode materials,from which the key factors affecting ion diffusion are further presented.Then,the positive effects of purposely introduced defects,including vacancy and doping,and the corresponding strategies for introducing various defects are discussed.The applications of defect engineering in cathode materials for RMBs with advanced electrochemical properties are also summarized.Finally,the existing challenges and future perspectives of defect engineering in cathode materials for the overall high-performance RMBs are described.展开更多
Na_(3)V_(2)(PO_(4))_(3)(NVP)has garnered great attentions as a prospective cathode material for sodium-ion batteries(SIBs)by virtue of its decent theoretical capacity,superior ion conductivity and high structural stab...Na_(3)V_(2)(PO_(4))_(3)(NVP)has garnered great attentions as a prospective cathode material for sodium-ion batteries(SIBs)by virtue of its decent theoretical capacity,superior ion conductivity and high structural stability.However,the inherently poor electronic conductivity and sluggish sodium-ion diffusion kinetics of NVP material give rise to inferior rate performance and unsatisfactory energy density,which strictly confine its further application in SIBs.Thus,it is of significance to boost the sodium storage performance of NVP cathode material.Up to now,many methods have been developed to optimize the electrochemical performance of NVP cathode material.In this review,the latest advances in optimization strategies for improving the electrochemical performance of NVP cathode material are well summarized and discussed,including carbon coating or modification,foreign-ion doping or substitution and nanostructure and morphology design.The foreign-ion doping or substitution is highlighted,involving Na,V,and PO_(4)^(3−)sites,which include single-site doping,multiple-site doping,single-ion doping,multiple-ion doping and so on.Furthermore,the challenges and prospects of high-performance NVP cathode material are also put forward.It is believed that this review can provide a useful reference for designing and developing high-performance NVP cathode material toward the large-scale application in SIBs.展开更多
Rechargeable magnesium batteries(RMBs)are a cutting-edge energy storage solution,with several advantages over the state-of-art lithiumion batteries(LIBs).The use of magnesium(Mg)metal as an anode material provides a m...Rechargeable magnesium batteries(RMBs)are a cutting-edge energy storage solution,with several advantages over the state-of-art lithiumion batteries(LIBs).The use of magnesium(Mg)metal as an anode material provides a much higher gravimetric capacity compared to graphite,which is currently used as the anode material in LIBs.Despite the significant advances in electrolyte,the development of cathode material is limited to materials that operate at low average discharge voltage(<1.0 V vs.Mg/Mg^(2+)),and developing high voltage cathodes remains challenging.Only a few materials have been shown to intercalate Mg^(2+)ions reversibly at high voltage.This review focuses on the structural aspects of cathode material that can operate at high voltage,including the Mg^(2+)intercalation mechanism in relation to its electrochemical properties.The materials are categorized into transition metal oxides and polyanions and subcategorized by the intrinsic Mg^(2+)diffusion path.This review also provides insights into the future development of each material,aiming to stimulate and guide researchers working in this field towards further advancements in high voltage cathodes.展开更多
Polycrystalline perovskite oxide particles are promising candidates for cathode materials in solid oxide fuel cells.However,their limited activity and stability pose significant challenges for practical applications.I...Polycrystalline perovskite oxide particles are promising candidates for cathode materials in solid oxide fuel cells.However,their limited activity and stability pose significant challenges for practical applications.In this study,we demonstrate a novel approach to achieve both high activity and durability in a PrBaCo_(2)O_(5+δ) catalyst through a simple epitaxial layer growth strategy.We found that an amorphous precursor of the highly durable catalyst SmBa_(0.5)Ca_(0.5)CoCuO_(5+δ) can spontaneously adhere to the surface of PrBaCo_(2)O_(5+δ) particles.Upon heat treatment,it grows along the perovskite lattice,forming a heteroepitaxial layer with just a few atomic layers thickness.This heterostructure enhances the operational stability of PrBaCo_(2)O_(5+δ) transforming a 78% decrease over 100 h into a 7% increase.After 100 h,the power output density of the cell with the modified sample is more than 500% higher than that of unmodified PrBaCo_(2)O_(5+δ.)This work presents a new strategy for fabricating heteroepitaxial layers on polycrystalline ceramic catalysts and introduces a pioneering approach for developing high-performance oxygen reduction catalysts and related materials.展开更多
Sodium-ion batteries have emerged as promising alternatives to lithium-ion batteries due to their abundant raw material reserves,low cost,enhanced safety,and environmental sustainability.Na_(2)Fe_(2)OS_(2),featuring a...Sodium-ion batteries have emerged as promising alternatives to lithium-ion batteries due to their abundant raw material reserves,low cost,enhanced safety,and environmental sustainability.Na_(2)Fe_(2)OS_(2),featuring a layered anti-perovskite structure,has attracted significant interest for its high capacity and facile synthesis.In this study,density functional theory calculations were performed to systematically investigate the phase stability,ionic conductivity,and voltage characteristics of Na_(2)Fe_(2)OS_(2)as a model system for anti-perovskite layered cathode materials.The compound exhibits excellent phase stability,and its equilibrium potential was calculated for the series Na_(x)Fe_(2)OCh_(2)(0<±<2)(where Ch represents chalcogenides).Naion transport analysis using the climbing image nudged elastic band method reveals a relatively low migration barrier(~0.47eV)along a dingonal pathway,indicating efficient Na^(+)mobility.To expand the materials design space,we systematically explored the effects of substituting Fe with various transition metals and replacing S with Se in NaaTM_(2)OCh_(2)structures.Among the variants studied,Na_(2)Mn_(2)OS_(2) demonstrates the most favorable combination of high voltage(~2.51V),robust phase stability,and superior energy density(~427 W-h/kg).This comprehensive comparison of transition metal substitutions provides vnluable insights for the rational design and experimental development of next-generation anti-perovskite layered cathode materials for sodium-ion batteries.展开更多
The development of appropriate cathode materials with stable structures and fast diffusion kinetics of zinc ions is crucial for aqueous zinc-ion batteries(AZIBs)but remains significantly challenging.Herein,the design ...The development of appropriate cathode materials with stable structures and fast diffusion kinetics of zinc ions is crucial for aqueous zinc-ion batteries(AZIBs)but remains significantly challenging.Herein,the design and synthesis of defect-rich and prismatic-shaped nanohybrids composed of vanadium oxynitride nanoparticles confined in the porous nitrogen-doped carbon framework(VN_(x)O_(y)@NC)are reported.Its unique structural advantages,including enriched defect sites that effectively enhance electrical conductivity,accelerate charge transfer kinetics,and improve structural stability.Additionally,the introduction of structural defects in VN_(x)O_(y)@NC increases the adsorption energy and reduces the hopping barrier of Zn ion,as evidenced by density functional theory(DFT)calculations.The H^(+)and Zn^(2+)co-insertion/extraction mechanism was systematically validated by ex-situ X-ray diffraction and ex-situ X-ray photoelectron spectroscopy tests.Consequently,the VN_(x)O_(y)@NC//Zn batteries exhibit an exceptional capacity of 570.9 mAh g^(-1)at 0.2 A g^(-1),a superior rate capability of 446.7 mAh g^(-1)at 20 A g^(-1),and long cycling life.Furthermore,the corresponding quasisolid-state battery delivers an ultra-high energy density of 271.9 Wh kg^(-1),demonstrating potential for practical applications.This work presents an effective structural and defect engineering strategy for designing advanced electrode materials with promising applications in AZIBs.展开更多
Sluggish conversion reaction kinetics and spontaneous shuttle effect of lithium polysulfides(LiPSs)are deemed as the two big mountains that hinder the practical application of lithium-sulfur batteries(LSBs).Herein,dua...Sluggish conversion reaction kinetics and spontaneous shuttle effect of lithium polysulfides(LiPSs)are deemed as the two big mountains that hinder the practical application of lithium-sulfur batteries(LSBs).Herein,dual-defect engineering strategy is implemented by introducing boron-doping and phosphorusvacancy sites with MoP@NC composite as the precursor.Based on the experimental characterizations and theoretical calculations,B-MoP_(1-x)@NC-based electrode presents low oxidation potential,high lithium diffusivity,small Tafel slope and strong adsorption capability for polysulfides,which is beneficial to enhance the adsorption capability for LiPSs,reduce the lithium diffusion energy barriers and Gibbs free energy for the conversion reactions of LiPSs.As demonstrated,the corresponding Li-S/B-MoP1-x@NC batteries can remain high reversible capacity of 753 mAh/g at 0.5 C after 300 cycles,and keep a stable capacity of 520 mAh/g at 0.5 C after 100 cycles even at the high-loading content of 5.1mg/cm^(2).According to the results of in-situ UV–vis spectra,the satisfactory battery performance majorly originates from the existence of dual-defect characteristics in B-MoP1-x@NC catalyst,which effectively promotes the conversion reaction kinetics of LiPSs,and restrains the shuttle behavior of LiPSs.The key ideas of this work will enlighten the development of catalytic cathode materials for sulfur-based secondary batteries.展开更多
Ni-rich cathode materials have become the mainstream choice in the mileage electric vehicle sector due to their high specific capacity and safety factor.However,the volume changes occurring during charging and dischar...Ni-rich cathode materials have become the mainstream choice in the mileage electric vehicle sector due to their high specific capacity and safety factor.However,the volume changes occurring during charging and discharging lead to microcracking and surface remodeling,posing challenges to achieving such as high specific capacity and long cycle stability.This paper reviews existing modification strategies for Ni-rich layered oxide cathode materials.Unlike previous reviews and related papers,we comprehensively discuss a variety of modification strategies and deeply discuss the synergistic modification effect of surface coating and bulk doping,which is how to improve the cycling stability of the Ni-rich cathode.In addition,based on recent research advances,the prospects and challenges of modifying Ni-rich layered cathodes for cycle stability upgrading of the lithium-ion battery,as well as the potential application prospects in the field of power automobiles,are comprehensively analyzed.展开更多
With large-scale commercial applications of lithium-ion batteries(LIBs),lots of spent LIBs will be produced and cause huge waste of resources and greatly increased environmental problems.Thus,recycling spent LIB mater...With large-scale commercial applications of lithium-ion batteries(LIBs),lots of spent LIBs will be produced and cause huge waste of resources and greatly increased environmental problems.Thus,recycling spent LIB materials is inevitable.Due to high added-value features,converting spent LIB cathode materials into catalysts exhibits broad application prospects.Inspired by this,we review the high-added-value reutilization of spent LIB materials toward catalysts of energy conversion.First,the failure mechanism of spent LIB cathode materials are discussed,and then the transformation and modification strategies are summarized and analyzed to improve the transformation efficiency of failed cathode materials and the catalytic performance of catalysts,respectively.Moreover,the electrochemical applications of failed cathode material derived catalysts are introduced,and the key problems and countermeasures are analyzed and proposed.Finally,the future development trend and prospect of high-added-value reutilization for spent LIB cathode materials toward catalysts are also given.This review will predictably advance the awareness of valorizing spent lithium-ion battery cathode materials for catalysis.展开更多
Arising from the increasing demand for electric vehicles(EVs),Ni-rich LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM,x+y+z=1,x≥0.8)cathode with greatly increased energy density are being researched and commercialized for lithium-ion ...Arising from the increasing demand for electric vehicles(EVs),Ni-rich LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM,x+y+z=1,x≥0.8)cathode with greatly increased energy density are being researched and commercialized for lithium-ion batteries(LIBs).However,parasitic crack formation during the discharge–charge cycling process remains as a major degradation mechanism.Cracking leads to increase in the specific surface area,loss of electrical contact between the primary particles,and facilitates liquid electrolyte infiltration into the cathode active material,accelerating capacity fading and decrease in lifetime.In contrast,Ni-rich NCM when used as a single crystal exhibits superior cycling performances due to its rigid mechanical property that resists cracking during long charge–discharge process even under harsh conditions.In this paper,we present comparative investigation between single crystal Ni-rich LiNi_(0.92)Co_(0.04)Mn_(0.04)O_(2)(SC)and polycrystalline Ni-rich LiNi_(0.92)Co_(0.04)Mn_(0.04)O_(2)(PC).The relatively improved cycling performances of SC are attributed to smaller anisotropic volume change,higher reversibility of phase transition,and resistance to crack formation.The superior properties of SC are demonstrated by in situ characterization and battery tests.Consequently,it is inferred from the results obtained that optimization of preparation conditions can be regarded as a key approach to obtain well crystallized and superior electrochemical performances.展开更多
Iron-based sulfates have emerged as promising cathode materials for potassium-ion batteries due to their low cost,high working potential,and environmentally friendly.However,the relatively large ionic radius and slugg...Iron-based sulfates have emerged as promising cathode materials for potassium-ion batteries due to their low cost,high working potential,and environmentally friendly.However,the relatively large ionic radius and sluggish diffusion coefficient of K-ion pose significant challenges to the electrochemical performance and structural stability of cathode materials in potassium-ion batteries(PIBs).In this work,we successfully synthesis a new iron-based sulfate cathode material,potassium sodium iron sulfate(K1.66Na1.02Fe1.66(SO4)3,KNFS),through an electro-chemical ion exchange method.As a cathode material,it exhibits a reversible specific capacity of 83 mAh·g^(−1) and an average working potential of 3.84 V(vs.K/K^(+))at 0.1 C in PIBs.Even at 2 C,it still demonstrates a reversible specific capacity of 52 mAh·g^(−1) with a capacity retention ratio of 88.2%after 300 cycles.The in-situ X-ray diffraction(XRD)and ex-situ X-ray absorption spectroscopy reveal that the K-ion storage mechanism in KNFS is predominantly governed by the reversible Fe3+/Fe2+redox couple,which provides a theoretical specific capacity of 94 mAh·g^(−1) and involves minimal volume change(2.57%).The first-principles calculations combined with XRD results indicate that the KNFS cathode exhibits a typical alluaudite-type crystal structure with multiple fast K-ion migration channels along the three-dimensional orientation.展开更多
Magnesium-ion batteries hold promise as future energy storage solutions,yet current Mg cathodes are challenged by low voltage and specific capacity.Herein,we present an AI-driven workflow for discovering high-performa...Magnesium-ion batteries hold promise as future energy storage solutions,yet current Mg cathodes are challenged by low voltage and specific capacity.Herein,we present an AI-driven workflow for discovering high-performance Mg cathode materials.Utilizing the common characteristics of various ionic intercalation-type electrodes,we design and train a Crystal Graph Convolutional Neural Network model that can accurately predict electrode voltages for various ions with mean absolute errors(MAE)between0.25 and 0.33 V.By deploying the trained model to stable Mg compounds from Materials Project and GNoME AI dataset,we identify 160 high voltage structures out of 15,308 candidates with voltages above3.0 V and volumetric capacity over 800 mA h/cm^(3).We further train a precise NequIP model to facilitate accurate and rapid simulations of Mg ionic conductivity.From the 160 high voltage structures,the machine learning molecular dynamics simulations have selected 23 cathode materials with both high energy density and high ionic conductivity.This Al-driven workflow dramatically boosts the efficiency and precision of material discovery for multivalent ion batteries,paving the way for advanced Mg battery development.展开更多
Although lithium-ion batteries(LIBs)currently dominate a wide spectrum of energy storage applications,they face challenges such as fast cycle life decay and poor stability that hinder their further application.To addr...Although lithium-ion batteries(LIBs)currently dominate a wide spectrum of energy storage applications,they face challenges such as fast cycle life decay and poor stability that hinder their further application.To address these limitations,element doping has emerged as a prevalent strategy to enhance the discharge capacity and extend the durability of Li-Ni-Co-Mn(LNCM)ternary compounds.This study utilized a machine learning-driven feature screening method to effectively pinpoint four key features crucially impacting the initial discharge capacity(IC)of Li-Ni-Co-Mn(LNCM)ternary cathode materials.These features were also proved highly predictive for the 50^(th)cycle discharge capacity(EC).Additionally,the application of SHAP value analysis yielded an in-depth understanding of the interplay between these features and discharge performance.This insight offers valuable direction for future advancements in the development of LNCM cathode materials,effectively promoting this field toward greater efficiency and sustainability.展开更多
With the rapid development of new energy and the high proportion of new energy connected to the grid,energy storage has become the leading technology driving significant adjustments in the global energy landscape.Elec...With the rapid development of new energy and the high proportion of new energy connected to the grid,energy storage has become the leading technology driving significant adjustments in the global energy landscape.Electrochemical energy storage,as the most popular and promising energy storage method,has received extensive attention.Currently,the most widely used energy storage method is metal-ion secondary batteries,whose performance mainly depends on the cathode material.Prussian blue analogues(PBAs)have a unique open framework structures that allow quick and reversible insertion/extraction of metal ions such as Na^(+),K^(+),Zn^(2+),Li^(+)etc.,thus attracting widespread attention.The advantages of simple synthesis process,abundant resources,and low cost also distinguish it from its counterparts.Unfortunately,the crystal water and structural defects in the PBAs lattice that is generated during the synthesis process,as well as the low Na content,significantly affect their electrochemical performance.This paper focuses on PBAs’synthesis methods,crystal structure,modification strategies,and their potential applications as cathode materials for various metal ion secondary batteries and looks forward to their future development direction.展开更多
To improve the slow kinetics and poor mechanical strength of aqueous silver peroxide−aluminum(AgO−Al)battery cathode materials,the effects of different binders including polytetrafluoroethylene(PTFE)and polyvinylpyrro...To improve the slow kinetics and poor mechanical strength of aqueous silver peroxide−aluminum(AgO−Al)battery cathode materials,the effects of different binders including polytetrafluoroethylene(PTFE)and polyvinylpyrrolidone(PVP)on the AgO cathode material were investigated.The samples were characterized by scanning electron microscopy(SEM),transmission electron microscopy(TEM),cyclic voltammetry(CV),electrochemical impedance spectrum(EIS),and galvanostatic discharge.In contrast to the pure AgO and AgO−PTFE electrodes,the results demonstrated that the PVP effectively bound the electrode materials together.The prepared AgO−PVP as the cathode material of AgO−Al batteries could improve the battery capacity,exhibiting a high specific capacity(389.95 mA·h/g at 500 mA/cm^(2)),a high operating voltage(1.75 V at 500 mA/cm^(2)),a maximum energy density(665.65 W·h/kg),and a maximum power density(5236 W/kg).Furthermore,the electrochemical mechanism of the AgO−PVP cathode material was examined,revealing that the electrode exhibited rapid ion diffusion and effective interfacial ion/electron transport.展开更多
A collaborative optimization method for the sintering schedule of ternary cathode materials was proposed under microscopic coupling constraints.An oxygen vacancy concentration prediction model based on microscopic the...A collaborative optimization method for the sintering schedule of ternary cathode materials was proposed under microscopic coupling constraints.An oxygen vacancy concentration prediction model based on microscopic thermodynamics and a growth kinetics model based on neural networks were established.Then,optimization formulations were constructed in three stages to obtain an optimal sintering schedule that minimized energy consumption for different requirements.Simulations demonstrate that the models accurately predict the oxygen vacancy concentrations and grain size,with root mean square errors of approximately 5%and 3%,respectively.Furthermore,the optimized sintering schedule not only meets the required quality standards but also reduces sintering time by 12.31%and keeping temperature by 11.96%.This research provides new insights and methods for the preparation of ternary cathode materials.展开更多
Facilitating anion redox chemistry is an effective strategy to increase the capacity of layered oxides for sodium-ion batteries.Nevertheless,there remains a paucity of literature pertaining to the oxygen redox chemist...Facilitating anion redox chemistry is an effective strategy to increase the capacity of layered oxides for sodium-ion batteries.Nevertheless,there remains a paucity of literature pertaining to the oxygen redox chemistry of O3-type layered oxide cathode materials.This work systematically investigates the effect of Fe doping on the anionic oxygen redox chemistry and electrochemical reactions in O3-NaNi_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1)O_(2).The results of the density functional theory(DFT)calculations indicate that the electrons of the O 2p occupy a higher energy level.In the ex-situ X-ray photoelectron spectrometer(XPS)of O 1s,the addition of Fe facilitates the lattice oxygen(O^(n-))to exhibit enhanced activity at 4.45 V.The in-situ X-ray diffraction(XRD)demonstrates that the doping of Fe effectively suppresses the Y phase transition at high voltages.Furthermore,the Galvanostatic Intermittent Titration Technique(GITT)data indicate that Fe doping significantly increases the Na~+migration rate at high voltages.Consequently,the substitution of Fe can elevate the cut-off voltage to 4.45 V,thereby facilitating electron migration from O^(2-).The redox of O^(2-)/O^(n-)(n<2)contributes to the overall capacity.O3-Na(Ni_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1))_(0.92)Fe_(0.08)O_(2)provides an initial discharge specific capacity of 180.55 mA h g^(-1)and71.6%capacity retention at 0.5 C(1 C=240 mA g^(-1)).This work not only demonstrates the beneficial impact of Fe substitution for promoting the redox activity and reversibility of O^(2-)in 03-type layered oxides,but also guarantees the structural integrity of the cathode materials at high voltages(>4.2 V).It offers a novel avenue for investigating the anionic redox reaction in O3-type layered oxides to design advanced cathode materials.展开更多
基金supported by the Exchange Program of Highend Foreign Experts of Ministry of Science and Technology of People’s Republic of China(No.G2023041003L)the Natural Science Foundation of Shaanxi Provincial Department of Education(No.23JK0367)+1 种基金the Scientific Research Startup Program for Introduced Talents of Shaanxi University of Technology(Nos.SLGRCQD2208,SLGRCQD2306,SLGRCQD2133)Contaminated Soil Remediation and Resource Utilization Innovation Team at Shaanxi University of Technology。
文摘As battery technology evolves and demand for efficient energy storage solutions,aqueous zinc ion batteries(AZIBs)have garnered significant attention due to their safety and environmental benefits.However,the stability of cathode materials under high-voltage conditions remains a critical challenge in improving its energy density.This review systematically explores the failure mechanisms of high-voltage cathode materials in AZIBs,including hydrogen evolution reaction,phase transformation and dissolution phenomena.To address these challenges,we propose a range of advanced strategies aimed at improving the stability of cathode materials.These strategies include surface coating and doping techniques designed to fortify the surface properties and structure integrity of the cathode materials under high-voltage conditions.Additionally,we emphasize the importance of designing antioxidant electrolytes,with a focus on understanding and optimizing electrolyte decomposition mechanisms.The review also highlights the significance of modifying conductive agents and employing innovative separators to further enhance the stability of AZIBs.By integrating these cutting-edge approaches,this review anticipates substantial advancements in the stability of high-voltage cathode materials,paving the way for the broader application and development of AZIBs in energy storage.
基金the National Natural Science Foundation of China Key Program(No.U22A20420)Changzhou Leading Innovative Talents Introduction and Cultivation Project(No.CQ20230109)for supporting our work。
文摘In recent years,sodium-ion batteries(SIBs)have become one of the hot discussions and have gradually moved toward industrialization.However,there are still some shortcomings in their performance that have not been well addressed,including phase transition,structural degradation,and voltage platform.High entropy materials have recently gained significant attention from researchers due to their effects on thermodynamics,dynamics,structure,and performance.Researchers have attempted to use these materials in sodium-ion batteries to overcome their problems,making it a modification method.This paper aims to discuss the research status of high-entropy cathode materials for sodium-ion batteries and summarize their effects on sodium-ion batteries from three perspectives:Layered oxide,polyanion,and Prussian blue.The infiuence on material structure,the inhibition of phase transition,and the improvement of ion diffusivity are described.Finally,the advantages and disadvantages of high-entropy cathode materials for sodium-ion batteries are summarized,and their future development has prospected.
基金National Natural Science Foundation of China(Nos.52174269,52374293)Science and Technology Innovation Program of Hunan Province,China(Nos.2024CK1009,2022RC1123)。
文摘A tunable oxidization and reduction strategy was proposed to directly regenerate spent LiFePO_(4)/C cathode materials by oxidizing excessive carbon powders with the addition of FePO_(4).Experimental results indicate that spent LiFePO_(4)/C cathode materials with good performance can be regenerated by roasting at 650℃ for 11 h with the addition ofLi_(2)CO_(3),FePO_(4),V_(2)O_(5),and glucose.V_(2)O_(5) is added to improve the cycle performance of regenerated cathode materials.Glucose is used to revitalize the carbon layers on the surface of spent LiFePO_(4)/C particles for improving their conductivity.The regenerated V-doped LiFePO_(4)/C shows an excellent electrochemical performance with the discharge specific capacity of 161.36 mA·h/g at 0.2C,under which the capacity retention is 97.85%after 100 cycles.
基金support of the National Natural Science Foundation of China(Grant No.22225801,22178217 and 22308216)supported by the Fundamental Research Funds for the Central Universities,conducted at Tongji University.
文摘Rechargeable magnesium batteries(RMBs)have been considered a promising“post lithium-ion battery”system to meet the rapidly increasing demand of the emerging electric vehicle and grid energy storage market.However,the sluggish diffusion kinetics of bivalent Mg^(2+)in the host material,related to the strong Coulomb effect between Mg^(2+)and host anion lattices,hinders their further development toward practical applications.Defect engineering,regarded as an effective strategy to break through the slow migration puzzle,has been validated in various cathode materials for RMBs.In this review,we first thoroughly understand the intrinsic mechanism of Mg^(2+)diffusion in cathode materials,from which the key factors affecting ion diffusion are further presented.Then,the positive effects of purposely introduced defects,including vacancy and doping,and the corresponding strategies for introducing various defects are discussed.The applications of defect engineering in cathode materials for RMBs with advanced electrochemical properties are also summarized.Finally,the existing challenges and future perspectives of defect engineering in cathode materials for the overall high-performance RMBs are described.
基金partly supported by the National Natural Science Foundation of China(Grant No.52272225).
文摘Na_(3)V_(2)(PO_(4))_(3)(NVP)has garnered great attentions as a prospective cathode material for sodium-ion batteries(SIBs)by virtue of its decent theoretical capacity,superior ion conductivity and high structural stability.However,the inherently poor electronic conductivity and sluggish sodium-ion diffusion kinetics of NVP material give rise to inferior rate performance and unsatisfactory energy density,which strictly confine its further application in SIBs.Thus,it is of significance to boost the sodium storage performance of NVP cathode material.Up to now,many methods have been developed to optimize the electrochemical performance of NVP cathode material.In this review,the latest advances in optimization strategies for improving the electrochemical performance of NVP cathode material are well summarized and discussed,including carbon coating or modification,foreign-ion doping or substitution and nanostructure and morphology design.The foreign-ion doping or substitution is highlighted,involving Na,V,and PO_(4)^(3−)sites,which include single-site doping,multiple-site doping,single-ion doping,multiple-ion doping and so on.Furthermore,the challenges and prospects of high-performance NVP cathode material are also put forward.It is believed that this review can provide a useful reference for designing and developing high-performance NVP cathode material toward the large-scale application in SIBs.
基金supported by the Nano&Material Technology Development Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(RS-2024-00446825)by the Technology Innovation Program(RS-2024-00418815)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea).
文摘Rechargeable magnesium batteries(RMBs)are a cutting-edge energy storage solution,with several advantages over the state-of-art lithiumion batteries(LIBs).The use of magnesium(Mg)metal as an anode material provides a much higher gravimetric capacity compared to graphite,which is currently used as the anode material in LIBs.Despite the significant advances in electrolyte,the development of cathode material is limited to materials that operate at low average discharge voltage(<1.0 V vs.Mg/Mg^(2+)),and developing high voltage cathodes remains challenging.Only a few materials have been shown to intercalate Mg^(2+)ions reversibly at high voltage.This review focuses on the structural aspects of cathode material that can operate at high voltage,including the Mg^(2+)intercalation mechanism in relation to its electrochemical properties.The materials are categorized into transition metal oxides and polyanions and subcategorized by the intrinsic Mg^(2+)diffusion path.This review also provides insights into the future development of each material,aiming to stimulate and guide researchers working in this field towards further advancements in high voltage cathodes.
基金financially supported by the National Natural Science Foundation of China (U2032157, 22209061)the Natural Science Foundation of Jiangsu Province (BK20201425)the Start-up Fund for Senior Talents in Jiangsu University(21JDG060)。
文摘Polycrystalline perovskite oxide particles are promising candidates for cathode materials in solid oxide fuel cells.However,their limited activity and stability pose significant challenges for practical applications.In this study,we demonstrate a novel approach to achieve both high activity and durability in a PrBaCo_(2)O_(5+δ) catalyst through a simple epitaxial layer growth strategy.We found that an amorphous precursor of the highly durable catalyst SmBa_(0.5)Ca_(0.5)CoCuO_(5+δ) can spontaneously adhere to the surface of PrBaCo_(2)O_(5+δ) particles.Upon heat treatment,it grows along the perovskite lattice,forming a heteroepitaxial layer with just a few atomic layers thickness.This heterostructure enhances the operational stability of PrBaCo_(2)O_(5+δ) transforming a 78% decrease over 100 h into a 7% increase.After 100 h,the power output density of the cell with the modified sample is more than 500% higher than that of unmodified PrBaCo_(2)O_(5+δ.)This work presents a new strategy for fabricating heteroepitaxial layers on polycrystalline ceramic catalysts and introduces a pioneering approach for developing high-performance oxygen reduction catalysts and related materials.
基金supported by the National Natural Science Foundation of China(Grant Nos.12404264 and 22209067)Shenzhen Basic Research Program(Natural Science Foundation)Key Project of Basic Research(Grant No.JCYJ20241202123916023)Shenzhen Science and Technology Program(Grant No.KQTD20200820113047086)。
文摘Sodium-ion batteries have emerged as promising alternatives to lithium-ion batteries due to their abundant raw material reserves,low cost,enhanced safety,and environmental sustainability.Na_(2)Fe_(2)OS_(2),featuring a layered anti-perovskite structure,has attracted significant interest for its high capacity and facile synthesis.In this study,density functional theory calculations were performed to systematically investigate the phase stability,ionic conductivity,and voltage characteristics of Na_(2)Fe_(2)OS_(2)as a model system for anti-perovskite layered cathode materials.The compound exhibits excellent phase stability,and its equilibrium potential was calculated for the series Na_(x)Fe_(2)OCh_(2)(0<±<2)(where Ch represents chalcogenides).Naion transport analysis using the climbing image nudged elastic band method reveals a relatively low migration barrier(~0.47eV)along a dingonal pathway,indicating efficient Na^(+)mobility.To expand the materials design space,we systematically explored the effects of substituting Fe with various transition metals and replacing S with Se in NaaTM_(2)OCh_(2)structures.Among the variants studied,Na_(2)Mn_(2)OS_(2) demonstrates the most favorable combination of high voltage(~2.51V),robust phase stability,and superior energy density(~427 W-h/kg).This comprehensive comparison of transition metal substitutions provides vnluable insights for the rational design and experimental development of next-generation anti-perovskite layered cathode materials for sodium-ion batteries.
基金financially supported by the National Natural Science Foundation of China(Nos.22225902,U22A20436,and 22209185)the National key Research&Development Program of China(Nos.2022YFE0115900 and 2021YFA1501500)+1 种基金the Postdoctoral Fellowship Program of CPSF,China(No.GZB20230758)Fujian Key Laboratory of Green Extraction and High-value Utilization of New Energy Metals(No.2023-KFKT-2)
文摘The development of appropriate cathode materials with stable structures and fast diffusion kinetics of zinc ions is crucial for aqueous zinc-ion batteries(AZIBs)but remains significantly challenging.Herein,the design and synthesis of defect-rich and prismatic-shaped nanohybrids composed of vanadium oxynitride nanoparticles confined in the porous nitrogen-doped carbon framework(VN_(x)O_(y)@NC)are reported.Its unique structural advantages,including enriched defect sites that effectively enhance electrical conductivity,accelerate charge transfer kinetics,and improve structural stability.Additionally,the introduction of structural defects in VN_(x)O_(y)@NC increases the adsorption energy and reduces the hopping barrier of Zn ion,as evidenced by density functional theory(DFT)calculations.The H^(+)and Zn^(2+)co-insertion/extraction mechanism was systematically validated by ex-situ X-ray diffraction and ex-situ X-ray photoelectron spectroscopy tests.Consequently,the VN_(x)O_(y)@NC//Zn batteries exhibit an exceptional capacity of 570.9 mAh g^(-1)at 0.2 A g^(-1),a superior rate capability of 446.7 mAh g^(-1)at 20 A g^(-1),and long cycling life.Furthermore,the corresponding quasisolid-state battery delivers an ultra-high energy density of 271.9 Wh kg^(-1),demonstrating potential for practical applications.This work presents an effective structural and defect engineering strategy for designing advanced electrode materials with promising applications in AZIBs.
基金financial support from National Natural Science Foundation of China(No.52101250)Hebei Provincial Natural Science Foundation(Nos.E2021208031 and B2021208069)+6 种基金S&T program of Hebei(Nos.215A4401D and 225A4404D)Research Fund of the Innovation Platform for Academicians of Hainan Province(No.YSPTZX202315)Collaborative Innovation Center of Marine Science and Technology of Hainan University(No.XTCX2022HYC14)partially supported by the Pico Election Microscopy Center of Hainan UniversityFundamental Research Funds for the Hebei University(No.2021YWF11)Science Research Project of Hebei Education Department(No.QN2024087)Xingtai City Natural Science Foundation(No.2023ZZ027)
文摘Sluggish conversion reaction kinetics and spontaneous shuttle effect of lithium polysulfides(LiPSs)are deemed as the two big mountains that hinder the practical application of lithium-sulfur batteries(LSBs).Herein,dual-defect engineering strategy is implemented by introducing boron-doping and phosphorusvacancy sites with MoP@NC composite as the precursor.Based on the experimental characterizations and theoretical calculations,B-MoP_(1-x)@NC-based electrode presents low oxidation potential,high lithium diffusivity,small Tafel slope and strong adsorption capability for polysulfides,which is beneficial to enhance the adsorption capability for LiPSs,reduce the lithium diffusion energy barriers and Gibbs free energy for the conversion reactions of LiPSs.As demonstrated,the corresponding Li-S/B-MoP1-x@NC batteries can remain high reversible capacity of 753 mAh/g at 0.5 C after 300 cycles,and keep a stable capacity of 520 mAh/g at 0.5 C after 100 cycles even at the high-loading content of 5.1mg/cm^(2).According to the results of in-situ UV–vis spectra,the satisfactory battery performance majorly originates from the existence of dual-defect characteristics in B-MoP1-x@NC catalyst,which effectively promotes the conversion reaction kinetics of LiPSs,and restrains the shuttle behavior of LiPSs.The key ideas of this work will enlighten the development of catalytic cathode materials for sulfur-based secondary batteries.
基金supported by the Science and Technology Research Project of Changchun City(24GXYSZZ01)the Natural Science Foundation of Jilin Province(NO.20220101036JC)。
文摘Ni-rich cathode materials have become the mainstream choice in the mileage electric vehicle sector due to their high specific capacity and safety factor.However,the volume changes occurring during charging and discharging lead to microcracking and surface remodeling,posing challenges to achieving such as high specific capacity and long cycle stability.This paper reviews existing modification strategies for Ni-rich layered oxide cathode materials.Unlike previous reviews and related papers,we comprehensively discuss a variety of modification strategies and deeply discuss the synergistic modification effect of surface coating and bulk doping,which is how to improve the cycling stability of the Ni-rich cathode.In addition,based on recent research advances,the prospects and challenges of modifying Ni-rich layered cathodes for cycle stability upgrading of the lithium-ion battery,as well as the potential application prospects in the field of power automobiles,are comprehensively analyzed.
基金supported by the National Key Research and Development Program of China(No.2023YFB3809300).
文摘With large-scale commercial applications of lithium-ion batteries(LIBs),lots of spent LIBs will be produced and cause huge waste of resources and greatly increased environmental problems.Thus,recycling spent LIB materials is inevitable.Due to high added-value features,converting spent LIB cathode materials into catalysts exhibits broad application prospects.Inspired by this,we review the high-added-value reutilization of spent LIB materials toward catalysts of energy conversion.First,the failure mechanism of spent LIB cathode materials are discussed,and then the transformation and modification strategies are summarized and analyzed to improve the transformation efficiency of failed cathode materials and the catalytic performance of catalysts,respectively.Moreover,the electrochemical applications of failed cathode material derived catalysts are introduced,and the key problems and countermeasures are analyzed and proposed.Finally,the future development trend and prospect of high-added-value reutilization for spent LIB cathode materials toward catalysts are also given.This review will predictably advance the awareness of valorizing spent lithium-ion battery cathode materials for catalysis.
基金supported by the Technology Innovation Program(RS-2023-00256202Development of MLCB design and manufacturing process technology for board mounting)funded By the Ministry of Trade,Industry&Energy(MOTIE,Korea)+2 种基金supported by the Technology Innovation Program(or Industrial Strategic Technology Development Program-Public-private joint investment semiconductor R&D program(K-CHIPS)to foster high-quality human resources)(RS-2023-00237003,High selectivity etching technology using cryoetch)funded By the Ministry of Trade,Industry&Energy(MOTIE,Korea)supported by 2022 Research Grant from Kangwon National University(No.202203080001)supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(RS-2023-00280367).
文摘Arising from the increasing demand for electric vehicles(EVs),Ni-rich LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM,x+y+z=1,x≥0.8)cathode with greatly increased energy density are being researched and commercialized for lithium-ion batteries(LIBs).However,parasitic crack formation during the discharge–charge cycling process remains as a major degradation mechanism.Cracking leads to increase in the specific surface area,loss of electrical contact between the primary particles,and facilitates liquid electrolyte infiltration into the cathode active material,accelerating capacity fading and decrease in lifetime.In contrast,Ni-rich NCM when used as a single crystal exhibits superior cycling performances due to its rigid mechanical property that resists cracking during long charge–discharge process even under harsh conditions.In this paper,we present comparative investigation between single crystal Ni-rich LiNi_(0.92)Co_(0.04)Mn_(0.04)O_(2)(SC)and polycrystalline Ni-rich LiNi_(0.92)Co_(0.04)Mn_(0.04)O_(2)(PC).The relatively improved cycling performances of SC are attributed to smaller anisotropic volume change,higher reversibility of phase transition,and resistance to crack formation.The superior properties of SC are demonstrated by in situ characterization and battery tests.Consequently,it is inferred from the results obtained that optimization of preparation conditions can be regarded as a key approach to obtain well crystallized and superior electrochemical performances.
基金funded by the Science and Technology Commission of Shanghai Municipality(No.19D.Z.2271100)the China Postdoctoral Science Foundation(No.2024M750490)The authors would like to express their sincere gratitude to Ms.Li from Scientific Compass(www.shiyanjia.com)for her valuable assistance in XPS testing.
文摘Iron-based sulfates have emerged as promising cathode materials for potassium-ion batteries due to their low cost,high working potential,and environmentally friendly.However,the relatively large ionic radius and sluggish diffusion coefficient of K-ion pose significant challenges to the electrochemical performance and structural stability of cathode materials in potassium-ion batteries(PIBs).In this work,we successfully synthesis a new iron-based sulfate cathode material,potassium sodium iron sulfate(K1.66Na1.02Fe1.66(SO4)3,KNFS),through an electro-chemical ion exchange method.As a cathode material,it exhibits a reversible specific capacity of 83 mAh·g^(−1) and an average working potential of 3.84 V(vs.K/K^(+))at 0.1 C in PIBs.Even at 2 C,it still demonstrates a reversible specific capacity of 52 mAh·g^(−1) with a capacity retention ratio of 88.2%after 300 cycles.The in-situ X-ray diffraction(XRD)and ex-situ X-ray absorption spectroscopy reveal that the K-ion storage mechanism in KNFS is predominantly governed by the reversible Fe3+/Fe2+redox couple,which provides a theoretical specific capacity of 94 mAh·g^(−1) and involves minimal volume change(2.57%).The first-principles calculations combined with XRD results indicate that the KNFS cathode exhibits a typical alluaudite-type crystal structure with multiple fast K-ion migration channels along the three-dimensional orientation.
基金supported by the National Key R&D Program of China(2022YFA1203400)the National Natural Science Foundation of China(W2441009)。
文摘Magnesium-ion batteries hold promise as future energy storage solutions,yet current Mg cathodes are challenged by low voltage and specific capacity.Herein,we present an AI-driven workflow for discovering high-performance Mg cathode materials.Utilizing the common characteristics of various ionic intercalation-type electrodes,we design and train a Crystal Graph Convolutional Neural Network model that can accurately predict electrode voltages for various ions with mean absolute errors(MAE)between0.25 and 0.33 V.By deploying the trained model to stable Mg compounds from Materials Project and GNoME AI dataset,we identify 160 high voltage structures out of 15,308 candidates with voltages above3.0 V and volumetric capacity over 800 mA h/cm^(3).We further train a precise NequIP model to facilitate accurate and rapid simulations of Mg ionic conductivity.From the 160 high voltage structures,the machine learning molecular dynamics simulations have selected 23 cathode materials with both high energy density and high ionic conductivity.This Al-driven workflow dramatically boosts the efficiency and precision of material discovery for multivalent ion batteries,paving the way for advanced Mg battery development.
基金supported by the National Natural Science Foundation of China(Nos.52122408,52071023)the Program for Science&Technology Innovation Talents in the University of Henan Province(No.22HASTIT1006)+2 种基金the Program for Central Plains Talents(No.ZYYCYU202012172)the Ministry of Education,Singapore(No.RG70/20)the Opening Project of National Joint Engineering Research Center for Abrasion Control and Molding of Metal Materials,Henan University of Science and Technology(No.HKDNM201906).
文摘Although lithium-ion batteries(LIBs)currently dominate a wide spectrum of energy storage applications,they face challenges such as fast cycle life decay and poor stability that hinder their further application.To address these limitations,element doping has emerged as a prevalent strategy to enhance the discharge capacity and extend the durability of Li-Ni-Co-Mn(LNCM)ternary compounds.This study utilized a machine learning-driven feature screening method to effectively pinpoint four key features crucially impacting the initial discharge capacity(IC)of Li-Ni-Co-Mn(LNCM)ternary cathode materials.These features were also proved highly predictive for the 50^(th)cycle discharge capacity(EC).Additionally,the application of SHAP value analysis yielded an in-depth understanding of the interplay between these features and discharge performance.This insight offers valuable direction for future advancements in the development of LNCM cathode materials,effectively promoting this field toward greater efficiency and sustainability.
基金supported by the National Natural Science Foundation of China(No.52072217)the National Key Research and Development Program of China(No.2022YFB3807700)+2 种基金the Joint Funds of the Hubei Natural Science Foundation Innovation and Development(No.2022CFD034)Hubei Natural Science Foundation Innovation Group Project(No.2022CFA020)the Major Technological Innovation Project of Hubei Science and Technology Department(No.2019AAA164).
文摘With the rapid development of new energy and the high proportion of new energy connected to the grid,energy storage has become the leading technology driving significant adjustments in the global energy landscape.Electrochemical energy storage,as the most popular and promising energy storage method,has received extensive attention.Currently,the most widely used energy storage method is metal-ion secondary batteries,whose performance mainly depends on the cathode material.Prussian blue analogues(PBAs)have a unique open framework structures that allow quick and reversible insertion/extraction of metal ions such as Na^(+),K^(+),Zn^(2+),Li^(+)etc.,thus attracting widespread attention.The advantages of simple synthesis process,abundant resources,and low cost also distinguish it from its counterparts.Unfortunately,the crystal water and structural defects in the PBAs lattice that is generated during the synthesis process,as well as the low Na content,significantly affect their electrochemical performance.This paper focuses on PBAs’synthesis methods,crystal structure,modification strategies,and their potential applications as cathode materials for various metal ion secondary batteries and looks forward to their future development direction.
基金supported by the Fundamental Research Funds for the Central Universities of Central South University,China(No.2022XQLH046)the Technical Area Fund of Foundation Strengthening,China(No.2022-JCJQ-ZD-174-00-20)National Defense Basic Scientific Research Projects,China,and Central South University−Zijin Mining Technical Cooperation Development Project,China.
文摘To improve the slow kinetics and poor mechanical strength of aqueous silver peroxide−aluminum(AgO−Al)battery cathode materials,the effects of different binders including polytetrafluoroethylene(PTFE)and polyvinylpyrrolidone(PVP)on the AgO cathode material were investigated.The samples were characterized by scanning electron microscopy(SEM),transmission electron microscopy(TEM),cyclic voltammetry(CV),electrochemical impedance spectrum(EIS),and galvanostatic discharge.In contrast to the pure AgO and AgO−PTFE electrodes,the results demonstrated that the PVP effectively bound the electrode materials together.The prepared AgO−PVP as the cathode material of AgO−Al batteries could improve the battery capacity,exhibiting a high specific capacity(389.95 mA·h/g at 500 mA/cm^(2)),a high operating voltage(1.75 V at 500 mA/cm^(2)),a maximum energy density(665.65 W·h/kg),and a maximum power density(5236 W/kg).Furthermore,the electrochemical mechanism of the AgO−PVP cathode material was examined,revealing that the electrode exhibited rapid ion diffusion and effective interfacial ion/electron transport.
基金supported by the National Natural Science Foundation of China(No.62033014)the Application Projects of Integrated Standardization and New Paradigm for Intelligent Manufacturing from the Ministry of Industry and Information Technology of China in 2016,and the Fundamental Research Funds for the Central Universities of Central South University,China(No.2021zzts0700).
文摘A collaborative optimization method for the sintering schedule of ternary cathode materials was proposed under microscopic coupling constraints.An oxygen vacancy concentration prediction model based on microscopic thermodynamics and a growth kinetics model based on neural networks were established.Then,optimization formulations were constructed in three stages to obtain an optimal sintering schedule that minimized energy consumption for different requirements.Simulations demonstrate that the models accurately predict the oxygen vacancy concentrations and grain size,with root mean square errors of approximately 5%and 3%,respectively.Furthermore,the optimized sintering schedule not only meets the required quality standards but also reduces sintering time by 12.31%and keeping temperature by 11.96%.This research provides new insights and methods for the preparation of ternary cathode materials.
基金financial support from the Natural Science Foundation of Shandong Province of China(ZR2023ME051,ZR2019MEM020)。
文摘Facilitating anion redox chemistry is an effective strategy to increase the capacity of layered oxides for sodium-ion batteries.Nevertheless,there remains a paucity of literature pertaining to the oxygen redox chemistry of O3-type layered oxide cathode materials.This work systematically investigates the effect of Fe doping on the anionic oxygen redox chemistry and electrochemical reactions in O3-NaNi_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1)O_(2).The results of the density functional theory(DFT)calculations indicate that the electrons of the O 2p occupy a higher energy level.In the ex-situ X-ray photoelectron spectrometer(XPS)of O 1s,the addition of Fe facilitates the lattice oxygen(O^(n-))to exhibit enhanced activity at 4.45 V.The in-situ X-ray diffraction(XRD)demonstrates that the doping of Fe effectively suppresses the Y phase transition at high voltages.Furthermore,the Galvanostatic Intermittent Titration Technique(GITT)data indicate that Fe doping significantly increases the Na~+migration rate at high voltages.Consequently,the substitution of Fe can elevate the cut-off voltage to 4.45 V,thereby facilitating electron migration from O^(2-).The redox of O^(2-)/O^(n-)(n<2)contributes to the overall capacity.O3-Na(Ni_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1))_(0.92)Fe_(0.08)O_(2)provides an initial discharge specific capacity of 180.55 mA h g^(-1)and71.6%capacity retention at 0.5 C(1 C=240 mA g^(-1)).This work not only demonstrates the beneficial impact of Fe substitution for promoting the redox activity and reversibility of O^(2-)in 03-type layered oxides,but also guarantees the structural integrity of the cathode materials at high voltages(>4.2 V).It offers a novel avenue for investigating the anionic redox reaction in O3-type layered oxides to design advanced cathode materials.
