Strategies for achieving high-energy-density lithium-ion batteries include using high-capacity materials such as high-nickel NCM,increasing the active material content in the electrode by utilizing high-conductivity c...Strategies for achieving high-energy-density lithium-ion batteries include using high-capacity materials such as high-nickel NCM,increasing the active material content in the electrode by utilizing high-conductivity carbon nanotubes(CNT)conductive materials,and electrode thickening.However,these methods are still limited due to the limitation in the capacity of high-nickel NCM,aggregation of CNT conductive materials,and nonuniform material distribution of thick-film electrodes,which ultimately damage the mechanical and electrical integrity of the electrode,leading to a decrease in electrochemical performance.Here,we present an integrated binder-CNT composite dispersion solution to realize a high-solids-content(>77 wt%)slurry for high-mass-loading electrodes and to mitigate the migration of binder and conductive additives.Indeed,the approach reduces solvent usage by approximately 30%and ensures uniform conductive additive-binder domain distribution during electrode manufacturing,resulting in improved coating quality and adhesive strength for high-mass-loading electrodes(>12 mAh cm^(−2)).In terms of various electrode properties,the presented electrode showed low resistance and excellent electrochemical properties despite the low CNT contents of 0.6 wt%compared to the pristine-applied electrode with 0.85 wt%CNT contents.Moreover,our strategy enables faster drying,which increases the coating speed,thereby offering potential energy savings and supporting carbon neutrality in wet-based electrode manufacturing processes.展开更多
Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temp...Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temperature(LT)operation.Therefore,a more comprehensive and systematic understanding of LIB behavior at LT is urgently required.This review article comprehensively reviews recent advancements in electrolyte engineering strategies aimed at improving the low-temperature operational capabilities of LIBs.The study methodically examines critical performance-limiting mechanisms through fundamental analysis of four primary challenges:insufficient ionic conductivity under cryogenic conditions,kinetically hindered charge transfer processes,Li+transport limitations across the solidelectrolyte interphase(SEI),and uncontrolled lithium dendrite growth.The work elaborates on innovative optimization approaches encompassing lithium salt molecular design with tailored dissociation characteristics,solvent matrix optimization through dielectric constant and viscosity regulation,interfacial engineering additives for constructing low-impedance SEI layers,and gel-polymer composite electrolyte systems.Notably,particular emphasis is placed on emerging machine learning-guided electrolyte formulation strategies that enable high-throughput virtual screening of constituent combinations and prediction of structure-property relationships.These artificial intelligence-assisted rational design frameworks demonstrate significant potential for accelerating the development of next-generation LT electrolytes by establishing quantitative composition-performance correlations through advanced data-driven methodologies.展开更多
As one of the alloy-type lithium-ion electrodes,Bi has outstanding application prospects for large volume capacity(3800 mAh·cm^(-3))and high electronic conductivity(1.4×10^(7)S·m^(-1)).However,the fast-...As one of the alloy-type lithium-ion electrodes,Bi has outstanding application prospects for large volume capacity(3800 mAh·cm^(-3))and high electronic conductivity(1.4×10^(7)S·m^(-1)).However,the fast-charging performance is hindered by significant volume expansion(>218%)and a low rate of phase diffusion.To overcome these two problems,an N-doped carbon nanoflower coating layer was elaborately in-situ reconstructed on a multiple-wall Bi microsphere by hydrothermal methods and subsequent calcination in this study.The carbon nanoflowers greatly increase specific surface area(40.0 m^(2)·g^(-1))and alleviate the volume expansion(130%).In addition,the incorporation of N-doped carbon nanoflowers leads to a gradual enhancement in the Li adsorption energy of Bi during the process of lithium insertion and improves the electrical conductivity.Therefore,the contribution rate of pseudo-capacitance reached 87.5%at the scan rate of 0.8 mV·s^(-1),and the Li-ion diffusion coefficient(D_(Li^(+)))was calculated in the range of 10^(-10)to 10^(-12)cm^(2)·s^(-1).The Bi@CNFs anode provided a high specific volumetric capacity of 2117.0 mAh·cm^(-3)at 5C and a high capacity retention ratio of 93.2%after 800 cycles.The Bi@CNFs//LiFePO_(4)full cell also displayed a stable capacity of 113.9 mAh·g^(-1)and energy density of 296.1 Wh·kg^(-1)after 100 cycles with a Coulombic efficiency of 97.6%.The mechanism of fast-charging lithium storage was verified by distribution of relaxation time analysis and density functional theory calculation.This paper provides a new strategy to increase the pseudo-capacitance and reduce the volume expansion for the preparation of alloy-type fast-charging electrodes.展开更多
SnO_(2)-based anodes for lithium-ion batteries(LIBs)experience volume expansion,leading to rapid capacity decay and low conductivity.To address this problem,a composite consists of C/SnO_(2) with a core-shell structur...SnO_(2)-based anodes for lithium-ion batteries(LIBs)experience volume expansion,leading to rapid capacity decay and low conductivity.To address this problem,a composite consists of C/SnO_(2) with a core-shell structure and a carbonized nitrogen-doped Co-metal organic framework(Co-MOF)(NC)supported on carbon cloth(CC)was designed and prepared,which was denoted as C/SnO_(2)@NC@CC.C/SnO_(2)@NC@CC could be used directly as a flexible anode for LIBs.The combination of core-shell structure centered on carbon spheres,carbonized nitrogen-doped Co-MOF,and CC not only restricts the volume expansion but also functions as conductive networks to improve the electrical conductivity.C/SnO_(2)@NC@CC exhibits excellent electrochemical performance with charge and discharge specific capacities of 2066.0 and 2077.1 mAh/g,respectively,after 120 cycles at a current density of 0.5 A/g.展开更多
When estimating the capacity of lithium-ion batteries offline or online,it is essential to extract a health feature(HF)that can effectively characterize capacity degradation under both conventional ideal and complex d...When estimating the capacity of lithium-ion batteries offline or online,it is essential to extract a health feature(HF)that can effectively characterize capacity degradation under both conventional ideal and complex dynamic operating conditions.However,the extraction of most HFs relies on complete charge-discharge cycle data,making them less adaptable to complex dynamic operating conditions.Existing mechanism HFs,while capable of characterizing capacity degradation from a mechanism perspective,suffer from limitations such as insufficient physical model expressiveness,high dimension,and redundancy of the mechanism HF.These issues increase the complexity of subsequent modeling of the relationship between HFs and capacity,thereby restricting their promotion in engineering practice.To meet this gap,this paper proposes a novel mechanism-based HF.Firstly,a multi-physical fields coupling model is developed to describe the interactions between electrochemical,thermal,and aging behaviors of the battery.Secondly,based on the aging mechanism,the accumulated charge of lithium lost during the formation of the solid electrolyte interphase(SEI)film is extracted as HF to provide a more intuitive representation of capacity degradation.Then,to reduce estimation errors caused by considering only a single aging mechanism,multiple representative regression models are employed to establish the mapping relationship between the mechanism HF and capacity,further enhancing the accuracy of final results.Finally,the proposed method is implemented and validated using real battery data under three different types of operating conditions.Experimental results demonstrate that,compared to other commonly used HFs,the proposed HF exhibits significant competitive advantages in handling incomplete cycle data,unknown operating conditions,and capacity estimation models.The minimum estimation error under ideal conditions is 0.0074,and the minimum estimation error under complex dynamic conditions is 0.0268.展开更多
C/SiO_(x)anode with higher capacity and lower lithiation potential has been recognized as a nextgeneration alternative to graphite for high-energy-density lithium-ion batteries.However,C/SiO_(x)suffers from low initia...C/SiO_(x)anode with higher capacity and lower lithiation potential has been recognized as a nextgeneration alternative to graphite for high-energy-density lithium-ion batteries.However,C/SiO_(x)suffers from low initial Coulombic efficiency(ICE),which significantly hinders its practical application.Herein,we reported a straightforward iodine redox chemistry strategy to realize highly reversible Li storage behavior and remarkably enhanced ICE of high-capacity C/SiO_(x)anode toward long-life lithium-ion batteries.Specifically,I2is introduced into porous C/SiO_(x)via simple fumigation to synthesize their composite(C/SiO_(x)@I),in which I_(2)can effectively inhibit the irreversible lithiation reactions of SiO_(x)through redox reaction.Further,redox reaction intermediates of LiI_(3)and LiIO_(3)can inhibit the decomposition of electrolyte and LiPF6,thereby reducing the thickness of the solid-electrolyte interphase film.Consequently,the obtained C/SiO_(x)@I exhibits a considerable capacity of 1241 mAh g^(-1)with an improved ICE of 88.5%at 0.1 A g^(-1)and impressive cyclability,showing capacity retention of 95%after 700 cycles at5.0 A g^(-1).Besides,the C/SiO_(x)@I with a 12%addition ratio can greatly enhance the capacity of graphite from 352 to 454 mAh g^(-1),with negligible impact on its ICE.When the addition ratio is 9%,the energy density of the 18,650 cylindrical battery composed of graphite and Li[Ni_(0.8)Co_(0.1)Mn_(0.1)]O_(2)can be enhanced by approximately 25 Wh kg^(-1).This study opens a new avenue for developing high ICE in SiO_(x)-based anodes for high-energy-density lithium-ion batteries.展开更多
Precisely estimating the state of health(SOH)of lithium-ion batteries is essential for battery management systems(BMS),as it plays a key role in ensuring the safe and reliable operation of battery systems.However,curr...Precisely estimating the state of health(SOH)of lithium-ion batteries is essential for battery management systems(BMS),as it plays a key role in ensuring the safe and reliable operation of battery systems.However,current SOH estimation methods often overlook the valuable temperature information that can effectively characterize battery aging during capacity degradation.Additionally,the Elman neural network,which is commonly employed for SOH estimation,exhibits several drawbacks,including slow training speed,a tendency to become trapped in local minima,and the initialization of weights and thresholds using pseudo-random numbers,leading to unstable model performance.To address these issues,this study addresses the challenge of precise and effective SOH detection by proposing a method for estimating the SOH of lithium-ion batteries based on differential thermal voltammetry(DTV)and an SSA-Elman neural network.Firstly,two health features(HFs)considering temperature factors and battery voltage are extracted fromthe differential thermal voltammetry curves and incremental capacity curves.Next,the Sparrow Search Algorithm(SSA)is employed to optimize the initial weights and thresholds of the Elman neural network,forming the SSA-Elman neural network model.To validate the performance,various neural networks,including the proposed SSA-Elman network,are tested using the Oxford battery aging dataset.The experimental results demonstrate that the method developed in this study achieves superior accuracy and robustness,with a mean absolute error(MAE)of less than 0.9%and a rootmean square error(RMSE)below 1.4%.展开更多
Electrospinning technology has emerged as a promising method for fabricating flexible lithium-ion batter-ies(FLIBs)due to its ability to create materials with desir-able properties for energy storage applications.FLIB...Electrospinning technology has emerged as a promising method for fabricating flexible lithium-ion batter-ies(FLIBs)due to its ability to create materials with desir-able properties for energy storage applications.FLIBs,which are foldable and have high energy densities,are be-coming increasingly important as power sources for wear-able devices,flexible electronics,and mobile energy applica-tions.Carbon materials,especially carbon nanofibers,are pivotal in improving the performance of FLIBs by increas-ing electrical conductivity,chemical stability,and surface area,as well as reducing costs.These materials also play a significant role in establishing conducting networks and im-proving structural integrity,which are essential for extend-ing the cycle life and enhancing the safety of the batteries.This review considers the role of electrospinning in the fabrication of critical FLIB components,with a particular emphasis on the integration of carbon materials.It explores strategies to optimize FLIB performance by fine-tuning the electrospinning para-meters,such as electric field strength,spinning rate,solution concentration,and carbonization process.Precise control over fiber properties is crucial for enhancing battery reliability and stability during folding and bending.It also highlights the latest research findings in carbon-based electrode materials,high-performance electrolytes,and separator structures,discussing the practical challenges and opportunities these materials present.It underscores the significant impact of carbon materials on the evolution of FLIBs and their potential to shape future energy storage technologies.展开更多
Silicon stands as a key anode material in lithium-ion battery ascribing to its high energy density.Nevertheless,the poor rate performance and limited cycling life remain unresolved through conventional approaches that...Silicon stands as a key anode material in lithium-ion battery ascribing to its high energy density.Nevertheless,the poor rate performance and limited cycling life remain unresolved through conventional approaches that involve carbon composites or nanostructures,primarily due to the un-controllable effects arising from the substantial formation of a solid electrolyte interphase(SEI)during the cycling.Here,an ultra-thin and homogeneous Ti doping alumina oxide catalytic interface is meticulously applied on the porous Si through a synergistic etching and hydrolysis process.This defect-rich oxide interface promotes a selective adsorption of fluoroethylene carbonate,leading to a catalytic reaction that can be aptly described as“molecular concentration-in situ conversion”.The resultant inorganic-rich SEI layer is electrochemical stable and favors ion-transport,particularly at high-rate cycling and high temperature.The robustly shielded porous Si,with a large surface area,achieves a high initial Coulombic efficiency of 84.7%and delivers exceptional high-rate performance at 25 A g^(−1)(692 mAh g^(−1))and a high Coulombic efficiency of 99.7%over 1000 cycles.The robust SEI constructed through a precious catalytic layer promises significant advantages for the fast development of silicon-based anode in fast-charging batteries.展开更多
Halide perovskite materials have received considerable attention for solar cells,LEDs,lasers etc.owing to their controllable physicochemical properties and structural advantages.However,little research has focused on ...Halide perovskite materials have received considerable attention for solar cells,LEDs,lasers etc.owing to their controllable physicochemical properties and structural advantages.However,little research has focused on energy storage and conversion applications,such as use as anodes in lithium-ion batteries.In this paper,all-inorganic lead-free halide perovskite Cs_(3)Bi_(2)Cl_(9)powders were synthesized by the grinding method,and the lattice was successfully adjusted via introducing Mn^(2+).The characterization results show that Mn-ion substitution can cause local lattice distortion to restructure the lattice,which will cause a mixed arrangement of[BiCl_(6)]octahedra to improve the performance of the anode material.This new material can provide a feasible solution for solving the problem of low specific capacity anode materials caused by unstable crystal structures,and also indicates that such perovskites with unique crystal structures and lattice tunability have broad application prospects in lithium-ion batteries.展开更多
TiNb_(2)O_(7)represents an up-and-coming anode material for fast-charging lithium-ion batteries,but its practicalities are severely impeded by slow transfer rates of ionic and electronic especially at the low-temperat...TiNb_(2)O_(7)represents an up-and-coming anode material for fast-charging lithium-ion batteries,but its practicalities are severely impeded by slow transfer rates of ionic and electronic especially at the low-temperature conditions.Herein,we introduce crystallographic engineering to enhance structure stability and promote Li+diffusion kinetics of TiNb_(2)O_(7)(TNO).The density functional theory computation reveals that Ti^(4+)is replaced by Sb^(5+)and Nb^(5+)in crystal lattices,which can reduce the Li+diffusion impediment and improve electronic conductivity.Synchrotron radiation X-ray 3D nano-computed tomography and in situ X-ray diffraction measurement confirm the introduction of Sb/Nb alleviates volume expansion during lithiation and delithiation processes,contributing to enhancing structure stability.Extended X-ray absorption fine structure spectra results verify that crystallographic engineering also increases short Nb-O bond length in TNO-Sb/Nb.Accordingly,the TNO-Sb/Nb anode delivers an outstanding capacity retention rate of 89.8%at 10 C after 700 cycles and excellent rate performance(140.4 mAh g^(−1) at 20 C).Even at−30℃,TNO-Sb/Nb anode delivers a capacity of 102.6 mAh g^(−1) with little capacity degeneration for 500 cycles.This work provides guidance for the design of fast-charging batteries at low-temperature condition.展开更多
With the approaching of large-scale retirement of power lithium-ion batteries(LIBs),their urgent handling is required for environmental protection and resource reutilization.However,at present,substantial spent power ...With the approaching of large-scale retirement of power lithium-ion batteries(LIBs),their urgent handling is required for environmental protection and resource reutilization.However,at present,substantial spent power batteries,especially for those high recovery value cathode materials,have not been greenly,sustainably,and efficiently recycled.Compared to the traditional recovery method for cathode materials with high energy consumption and severe secondary pollution,the direct repair regeneration,as a new type of short-process and efficient treatment methods,has attracted widespread attention.However,it still faces challenges in homogenization repair,electrochemical performance decline,and scaling-up production.To promote the direct regeneration technology development of failed NCM materials,herein we deeply discuss the failure mechanism of nickel-cobalt-manganese(NCM)ternary cathode materials,including element loss,Li/Ni mixing,phase transformation,structural defects,oxygen release,and surface degradation and reconstruction.Based on this,the detailed analysis and summary of the direct regeneration method embracing solid-phase sintering,eutectic salt assistance,solvothermal synthesis,sol-gel process,spray drying,and redox mediation are provided.Further,the upcycling strategy for regeneration materials,such as single-crystallization and high-nickelization,structural regulation,ion doping,and surface engineering,are discussed in deep.Finally,the challenges faced by the direct regeneration and corresponding countermeasures are pointed out.Undoubtedly,this review provides valuable guidance for the efficient and high-value recovery of failed cathode materials.展开更多
Lithium-ion batteries(LIBs)play a critical role in reducing carbon emissions in the automotive industry.However,they face challenges related to safety and performance failures.Smart technologies offer a promising solu...Lithium-ion batteries(LIBs)play a critical role in reducing carbon emissions in the automotive industry.However,they face challenges related to safety and performance failures.Smart technologies offer a promising solution to address these issues.Bioinspired microcapsules are a common approach to enhancing the performance and safety of smart LIBs.However,despite their potential,this area has not been thoroughly explored.This review provides an overview of the preparation methods for microcapsules,including physical,chemical,and physicochemical techniques.These microcapsules are categorized based on their mechanisms into electrode self-healing burst microcapsules,interphase-forming sustained-release microcapsules,live-lithium sustained-release microcapsules,and flame-retardant burst microcapsules.A comprehensive analysis of their bioinspired design concepts,mechanisms,and performance is presented,along with the design criteria for microcapsules suitable for LIBs.Finally,the review explores the potential applications of microcapsule technologies in LIBs and their future trends,such as enhancing existing technologies for novel applications like solid-state batteries and developing new types of microcapsules.This review aims to provide a foundation for the implementation of microcapsule technologies in LIBs and to highlight the latest advancements in smart batteries.展开更多
The development of lithium-ion batteries with high-energy densities is substantially hampered by the graphite anode's low theoretical capacity(372 mAh g^(-1)).There is an urgent need to explore novel anode materia...The development of lithium-ion batteries with high-energy densities is substantially hampered by the graphite anode's low theoretical capacity(372 mAh g^(-1)).There is an urgent need to explore novel anode materials for lithium-ion batteries.Silicon(Si),the second-largest element outside of Earth,has an exceptionally high specific capacity(3579 mAh g^(-1)),regarded as an excellent choice for the anode material in high-capacity lithium-ion batteries.However,it is low intrinsic conductivity and volume amplification during service status,prevented it from developing further.These difficulties can be successfully overcome by incorporating carbon into pure Si systems to form a composite anode and constructing a buffer structure.This review looks at the diffusion mechanism,various silicon-based anode material configurations(including sandwich,core-shell,yolk-shell,and other 3D mesh/porous structures),as well as the appropriate binders and electrolytes.Finally,a summary and viewpoints are offered on the characteristics and structural layout of various structures,metal/non-metal doping,and the compatibility and application of various binders and electrolytes for silicon-based anodes.This review aims to provide valuable insights into the research and development of silicon-based carbon anodes for high-performance lithium-ion batteries,as well as their integration with binders and electrolyte.展开更多
To accelerate the development of lithium-ion batteries(LIBs),researchers should urgently exploit next-generation electrodes with high specific capacity,long cycle stability,and excellent rate performance,such as TMOs,...To accelerate the development of lithium-ion batteries(LIBs),researchers should urgently exploit next-generation electrodes with high specific capacity,long cycle stability,and excellent rate performance,such as TMOs,silicon-based materials,and alloys.Among all the modification measures,hierarchical micro-nano structure and yolk–shell structure are considered suitable and effective ways to improve the electrochemical performance of those novel materials.Herein,a facile glucose-assisted solvothermal method combined with heat treatment was implemented to synthesize hierarchical micro-nano yolk–shell V_(2)O_(3).The special-structured material exhibited higher specific capacity,better structure stability,and faster electrochemical kinetics compared with nanosheet-structured and micro-nano-cluster-structured V_(2)O_(3).When used as an anode for LIB,mnYS-V_(2)O_(3)delivered high specific capacity of 650.1 mA h g^(-1)after over 500 cycles at a current density of 100 mA g^(-1),with a retention of 93.4%.Moreover,the morphology evolution mechanism of micro-nano structure and yolk–shell structure was investigated in this work,which is beneficial to the design of other mnYS-structured TMOs.展开更多
The cobalt-free Mn-based Li-rich layered oxide material has the advantages of low cost,high energy density,and good performance at low temperatures,and is the promising choice for energy storage batteries.However,the ...The cobalt-free Mn-based Li-rich layered oxide material has the advantages of low cost,high energy density,and good performance at low temperatures,and is the promising choice for energy storage batteries.However,the long-cycling stability of batteries needs to be improved.Herein,the Mn-based Li-rich cathode materials with small amounts of Li2 MnO3 crystal domains and gradient doping of Al and Ti elements from the surface to the bulk have been developed to improve the structure and interface stability.Then the batteries with a high energy density of 600 Wh kg^(-1),excellent capacity retention of 99.7%with low voltage decay of 0.03 mV cycle^(-1) after 800 cycles,and good rates performances can be achieved.Therefore,the structure and cycling stability of low voltage Mn-based Li-rich cathode materials can be significantly improved by the bulk structure design and interface regulation,and this work has paved the way for developing low-cost and high-energy Mn-based energy storage batteries with long lifetime.展开更多
Exploring electrode materials with larger capacity,higher power density and longer cycle life was critical for developing advanced flexible lithium-ion batteries(LIBs).Herein,we used a controlled two-step method inclu...Exploring electrode materials with larger capacity,higher power density and longer cycle life was critical for developing advanced flexible lithium-ion batteries(LIBs).Herein,we used a controlled two-step method including electrospraying followed with calcination treatment by CVD furnace to design novel electrodes of Si/Si_(x)/C and Sn/C microrods array consisting of nanospheres on flexible carbon cloth substrate(denoted as Si/Si_(x)/C@CC,Sn/C@CC).Microrods composed of cumulated nanospheres(the diameter was approximately 120 nm)had a mean diameter of approximately 1.5μm and a length of around 4.0μm,distributing uniformly along the entire woven carbon fibers.Both of Si/Si/Si_(x)/C@CC and Sn/C@CC products were synthesized as binder-free anodes for Li-ion battery with the features of high reversible capacity and excellent cycling.Especially Si/Six/C electrode exhibited high specific capacity of about 1750 mA∙h∙g^(−1)at 0.5 A∙g^(−1)and excellent cycling ability even after 1050 cycles with a capacity of 1388 mA∙h∙g^(−1).Highly flexible Si/Si_(x)/C@CC//LiCoO_(2)batteries based on liquid and solid electrolytes were also fabricated,exhibiting high flexibility,excellent electrical stability and potential applications in flexible wearable electronics.展开更多
Micro-silicon(Si)anode that features high theoretical capacity and fine tap density is ideal for energy-dense lithiumion batteries.However,the substantial localized mechanical strain caused by the large volume expansi...Micro-silicon(Si)anode that features high theoretical capacity and fine tap density is ideal for energy-dense lithiumion batteries.However,the substantial localized mechanical strain caused by the large volume expansion often results in electrode disintegration and capacity loss.Herein,a microporous Si anode with the SiO_(x)/C layer functionalized all-surface and high tap density(~0.65 g cm^(-3))is developed by the hydrolysis-driven strategy that avoids the common use of corrosive etchants and toxic siloxane reagents.The functionalized inner pore with superior structural stability can effectively alleviate the volume change and enhance the electrolyte contact.Simultaneously,the outer particle surface forms a continuous network that prevents electrolyte parasitic decomposition,disperses the interface stress of Si matrix and facilitates electron/ion transport.As a result,the micron-sized Si anode shows only~9.94 GPa average stress at full lithiation state and delivers an impressive capacity of 901.1 mAh g^(-1)after 500 cycles at 1 A g^(-1).It also performs excellent rate performance of 1123.0 mAh g^(-1)at 5 A g^(-1)and 850.4 at 8 A g^(-1),far exceeding most of reported literatures.Furthermore,when paired with a commercial LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2),the pouch cell demonstrates high capacity and desirable cyclic performance.展开更多
The implementation of ultrahigh-Ni cathodes in high-energy lithium-ion batteries(LIBs)is constrained by significant structural and interfacial degradation during cycling.In this study,doping-induced surface restructur...The implementation of ultrahigh-Ni cathodes in high-energy lithium-ion batteries(LIBs)is constrained by significant structural and interfacial degradation during cycling.In this study,doping-induced surface restructuring in ultrahigh-nickel cathode materials is rapidly facilitated through an ultrafast Joule heating method.Density functional theory(DFT)calculations,synchrotron X-ray absorption spectroscopy(XAS),and single-particle force test confirmed the establishment of a stable crystal framework and lattice oxygen,which mitigated H2-H3 phase transitions and improved structural reversibility.Additionally,the Sc doping process exhibits a pinning effect on the grain boundaries,as shown by scanning transmission electron microscopy(STEM),enhancing Li~+diffusion kinetics and decreasing mechanical strain during cycling.The in situ development of a cation-mixing layer at grain boundaries also creates a robust cathode/electrolyte interphase,effectively reducing interfacial parasitic reactions and transition metal dissolution,as validated by STEM and time-of-flight secondary ion mass spectrometry(TOF-SIMS).These synergistic modifications reduce particle cracking and surface/interface degradation,leading to enhanced rate capability,structural integrity,and thermal stability.Consequently,the optimized Sc-modified ultrahigh-Ni cathode(Sc-1)exhibits 93.99%capacity retention after 100 cycles at 1 C(25℃)and87.06%capacity retention after 100 cycles at 1 C(50℃),indicating excellent cycling and thermal stability.By presenting a one-step multifunctional modification approach,this research delivers an extensive analysis of the mechanisms governing the structure,microstructure,and interface properties of nickel-rich layered cathode materials(NCMs).These results underscore the potential of ultrahigh-Ni cathodes as viable candidates for advanced lithium-ion batteries(LIBs)in next-generation electric vehicles(EVs).展开更多
Lithium-ion batteries(LIBs)are an electrochemical energy storage technology that has been widely used for portable electrical devices,electric vehicles,and grid storage,etc.To satisfy the demand for user convenience e...Lithium-ion batteries(LIBs)are an electrochemical energy storage technology that has been widely used for portable electrical devices,electric vehicles,and grid storage,etc.To satisfy the demand for user convenience especially for electric vehicles,the development of a fast-charging technology for LIBs has become a critical focus.In commercial LIBs,the slow kinetics of Li+intercalation into the graphite anode from the electrolyte solution is known as the main restriction for fast-charging.We summarize the recent advances in obtaining fast-charging graphite-based anodes,mainly involving modifications of the electrolyte solution and graphite anode.Specifically,strategies for increasing the ionic conductivity and regulating the Li+solvation/desolvation state in the electrolyte solution,as well as optimizing the fabrication and the intrinsic activity of graphite-based anodes are discussed in detail.This review considers practical ways to obtain fast Li+intercalation kinetics into a graphite anode from the electrolyte as well as analysing progress in the commercialization of fast-charging LIBs.展开更多
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.2022M3H4A6A0103720142)the National Research Council of Science&Technology(NST)grant by the Korea government(MSIT)(No.GTL24011-000)+1 种基金the Technology Innovation Program(RS-2024-00404165)through the Korea Planning&Evaluation Institute of Industrial Technology(KEIT)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea)supported by the Samsung SDI Co.Ltd.and the Korea Institute of Science and Technology(KIST)institutional program(2E33942,2E3394B)。
文摘Strategies for achieving high-energy-density lithium-ion batteries include using high-capacity materials such as high-nickel NCM,increasing the active material content in the electrode by utilizing high-conductivity carbon nanotubes(CNT)conductive materials,and electrode thickening.However,these methods are still limited due to the limitation in the capacity of high-nickel NCM,aggregation of CNT conductive materials,and nonuniform material distribution of thick-film electrodes,which ultimately damage the mechanical and electrical integrity of the electrode,leading to a decrease in electrochemical performance.Here,we present an integrated binder-CNT composite dispersion solution to realize a high-solids-content(>77 wt%)slurry for high-mass-loading electrodes and to mitigate the migration of binder and conductive additives.Indeed,the approach reduces solvent usage by approximately 30%and ensures uniform conductive additive-binder domain distribution during electrode manufacturing,resulting in improved coating quality and adhesive strength for high-mass-loading electrodes(>12 mAh cm^(−2)).In terms of various electrode properties,the presented electrode showed low resistance and excellent electrochemical properties despite the low CNT contents of 0.6 wt%compared to the pristine-applied electrode with 0.85 wt%CNT contents.Moreover,our strategy enables faster drying,which increases the coating speed,thereby offering potential energy savings and supporting carbon neutrality in wet-based electrode manufacturing processes.
基金the financial support from the Key Project of Shaanxi Provincial Natural Science Foundation-Key Project of Laboratory(2025SYS-SYSZD-117)the Natural Science Basic Research Program of Shaanxi(2025JCYBQN-125)+8 种基金Young Talent Fund of Xi'an Association for Science and Technology(0959202513002)the Key Industrial Chain Technology Research Program of Xi'an(24ZDCYJSGG0048)the Key Research and Development Program of Xianyang(L2023-ZDYF-SF-077)Postdoctoral Fellowship Program of CPSF(GZC20241442)Shaanxi Postdoctoral Science Foundation(2024BSHSDZZ070)Research Funds for the Interdisciplinary Projects,CHU(300104240913)the Fundamental Research Funds for the Central Universities,CHU(300102385739,300102384201,300102384103)the Scientific Innovation Practice Project of Postgraduate of Chang'an University(300103725063)the financial support from the Australian Research Council。
文摘Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temperature(LT)operation.Therefore,a more comprehensive and systematic understanding of LIB behavior at LT is urgently required.This review article comprehensively reviews recent advancements in electrolyte engineering strategies aimed at improving the low-temperature operational capabilities of LIBs.The study methodically examines critical performance-limiting mechanisms through fundamental analysis of four primary challenges:insufficient ionic conductivity under cryogenic conditions,kinetically hindered charge transfer processes,Li+transport limitations across the solidelectrolyte interphase(SEI),and uncontrolled lithium dendrite growth.The work elaborates on innovative optimization approaches encompassing lithium salt molecular design with tailored dissociation characteristics,solvent matrix optimization through dielectric constant and viscosity regulation,interfacial engineering additives for constructing low-impedance SEI layers,and gel-polymer composite electrolyte systems.Notably,particular emphasis is placed on emerging machine learning-guided electrolyte formulation strategies that enable high-throughput virtual screening of constituent combinations and prediction of structure-property relationships.These artificial intelligence-assisted rational design frameworks demonstrate significant potential for accelerating the development of next-generation LT electrolytes by establishing quantitative composition-performance correlations through advanced data-driven methodologies.
基金supported by the project of the National Natural Science Foundation of China(NSFC,Nos.5216040127,52164048 and U1802256)Central Guidance for Local Science and Technology Development Funds(No.202107AB110011)the Analysis and Test Funds of Kunming University of Science and Technology(No.2021M0202230188).
文摘As one of the alloy-type lithium-ion electrodes,Bi has outstanding application prospects for large volume capacity(3800 mAh·cm^(-3))and high electronic conductivity(1.4×10^(7)S·m^(-1)).However,the fast-charging performance is hindered by significant volume expansion(>218%)and a low rate of phase diffusion.To overcome these two problems,an N-doped carbon nanoflower coating layer was elaborately in-situ reconstructed on a multiple-wall Bi microsphere by hydrothermal methods and subsequent calcination in this study.The carbon nanoflowers greatly increase specific surface area(40.0 m^(2)·g^(-1))and alleviate the volume expansion(130%).In addition,the incorporation of N-doped carbon nanoflowers leads to a gradual enhancement in the Li adsorption energy of Bi during the process of lithium insertion and improves the electrical conductivity.Therefore,the contribution rate of pseudo-capacitance reached 87.5%at the scan rate of 0.8 mV·s^(-1),and the Li-ion diffusion coefficient(D_(Li^(+)))was calculated in the range of 10^(-10)to 10^(-12)cm^(2)·s^(-1).The Bi@CNFs anode provided a high specific volumetric capacity of 2117.0 mAh·cm^(-3)at 5C and a high capacity retention ratio of 93.2%after 800 cycles.The Bi@CNFs//LiFePO_(4)full cell also displayed a stable capacity of 113.9 mAh·g^(-1)and energy density of 296.1 Wh·kg^(-1)after 100 cycles with a Coulombic efficiency of 97.6%.The mechanism of fast-charging lithium storage was verified by distribution of relaxation time analysis and density functional theory calculation.This paper provides a new strategy to increase the pseudo-capacitance and reduce the volume expansion for the preparation of alloy-type fast-charging electrodes.
基金National Natural Science Foundation of China(No.61376017)。
文摘SnO_(2)-based anodes for lithium-ion batteries(LIBs)experience volume expansion,leading to rapid capacity decay and low conductivity.To address this problem,a composite consists of C/SnO_(2) with a core-shell structure and a carbonized nitrogen-doped Co-metal organic framework(Co-MOF)(NC)supported on carbon cloth(CC)was designed and prepared,which was denoted as C/SnO_(2)@NC@CC.C/SnO_(2)@NC@CC could be used directly as a flexible anode for LIBs.The combination of core-shell structure centered on carbon spheres,carbonized nitrogen-doped Co-MOF,and CC not only restricts the volume expansion but also functions as conductive networks to improve the electrical conductivity.C/SnO_(2)@NC@CC exhibits excellent electrochemical performance with charge and discharge specific capacities of 2066.0 and 2077.1 mAh/g,respectively,after 120 cycles at a current density of 0.5 A/g.
基金supported by the National Natural Science Foundation of China(NSFC,No.62303031)the Fundamental Research Funds for the Central Universities。
文摘When estimating the capacity of lithium-ion batteries offline or online,it is essential to extract a health feature(HF)that can effectively characterize capacity degradation under both conventional ideal and complex dynamic operating conditions.However,the extraction of most HFs relies on complete charge-discharge cycle data,making them less adaptable to complex dynamic operating conditions.Existing mechanism HFs,while capable of characterizing capacity degradation from a mechanism perspective,suffer from limitations such as insufficient physical model expressiveness,high dimension,and redundancy of the mechanism HF.These issues increase the complexity of subsequent modeling of the relationship between HFs and capacity,thereby restricting their promotion in engineering practice.To meet this gap,this paper proposes a novel mechanism-based HF.Firstly,a multi-physical fields coupling model is developed to describe the interactions between electrochemical,thermal,and aging behaviors of the battery.Secondly,based on the aging mechanism,the accumulated charge of lithium lost during the formation of the solid electrolyte interphase(SEI)film is extracted as HF to provide a more intuitive representation of capacity degradation.Then,to reduce estimation errors caused by considering only a single aging mechanism,multiple representative regression models are employed to establish the mapping relationship between the mechanism HF and capacity,further enhancing the accuracy of final results.Finally,the proposed method is implemented and validated using real battery data under three different types of operating conditions.Experimental results demonstrate that,compared to other commonly used HFs,the proposed HF exhibits significant competitive advantages in handling incomplete cycle data,unknown operating conditions,and capacity estimation models.The minimum estimation error under ideal conditions is 0.0074,and the minimum estimation error under complex dynamic conditions is 0.0268.
基金financially supported by the National Natural Science Foundation of China(No.51962027,and 52262039)the Major Science and Technology Project of Inner Mongolia Autonomous Region(2021ZD0016)+3 种基金the National Key R&D Program of China(2020YFC1909105)the Fundamental Research Funds for Inner Mongolia University of Science&Technology(NO.2024QNJS071,2023QNJS052 and 2024QNJS064)the Program for Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region(No.NJYT24002)the Central Guidance Fund for Local Scientific and Technological Development(2024ZY0012)。
文摘C/SiO_(x)anode with higher capacity and lower lithiation potential has been recognized as a nextgeneration alternative to graphite for high-energy-density lithium-ion batteries.However,C/SiO_(x)suffers from low initial Coulombic efficiency(ICE),which significantly hinders its practical application.Herein,we reported a straightforward iodine redox chemistry strategy to realize highly reversible Li storage behavior and remarkably enhanced ICE of high-capacity C/SiO_(x)anode toward long-life lithium-ion batteries.Specifically,I2is introduced into porous C/SiO_(x)via simple fumigation to synthesize their composite(C/SiO_(x)@I),in which I_(2)can effectively inhibit the irreversible lithiation reactions of SiO_(x)through redox reaction.Further,redox reaction intermediates of LiI_(3)and LiIO_(3)can inhibit the decomposition of electrolyte and LiPF6,thereby reducing the thickness of the solid-electrolyte interphase film.Consequently,the obtained C/SiO_(x)@I exhibits a considerable capacity of 1241 mAh g^(-1)with an improved ICE of 88.5%at 0.1 A g^(-1)and impressive cyclability,showing capacity retention of 95%after 700 cycles at5.0 A g^(-1).Besides,the C/SiO_(x)@I with a 12%addition ratio can greatly enhance the capacity of graphite from 352 to 454 mAh g^(-1),with negligible impact on its ICE.When the addition ratio is 9%,the energy density of the 18,650 cylindrical battery composed of graphite and Li[Ni_(0.8)Co_(0.1)Mn_(0.1)]O_(2)can be enhanced by approximately 25 Wh kg^(-1).This study opens a new avenue for developing high ICE in SiO_(x)-based anodes for high-energy-density lithium-ion batteries.
基金supported by the National Natural Science Foundation of China(NSFC)under Grant(No.51677058).
文摘Precisely estimating the state of health(SOH)of lithium-ion batteries is essential for battery management systems(BMS),as it plays a key role in ensuring the safe and reliable operation of battery systems.However,current SOH estimation methods often overlook the valuable temperature information that can effectively characterize battery aging during capacity degradation.Additionally,the Elman neural network,which is commonly employed for SOH estimation,exhibits several drawbacks,including slow training speed,a tendency to become trapped in local minima,and the initialization of weights and thresholds using pseudo-random numbers,leading to unstable model performance.To address these issues,this study addresses the challenge of precise and effective SOH detection by proposing a method for estimating the SOH of lithium-ion batteries based on differential thermal voltammetry(DTV)and an SSA-Elman neural network.Firstly,two health features(HFs)considering temperature factors and battery voltage are extracted fromthe differential thermal voltammetry curves and incremental capacity curves.Next,the Sparrow Search Algorithm(SSA)is employed to optimize the initial weights and thresholds of the Elman neural network,forming the SSA-Elman neural network model.To validate the performance,various neural networks,including the proposed SSA-Elman network,are tested using the Oxford battery aging dataset.The experimental results demonstrate that the method developed in this study achieves superior accuracy and robustness,with a mean absolute error(MAE)of less than 0.9%and a rootmean square error(RMSE)below 1.4%.
文摘Electrospinning technology has emerged as a promising method for fabricating flexible lithium-ion batter-ies(FLIBs)due to its ability to create materials with desir-able properties for energy storage applications.FLIBs,which are foldable and have high energy densities,are be-coming increasingly important as power sources for wear-able devices,flexible electronics,and mobile energy applica-tions.Carbon materials,especially carbon nanofibers,are pivotal in improving the performance of FLIBs by increas-ing electrical conductivity,chemical stability,and surface area,as well as reducing costs.These materials also play a significant role in establishing conducting networks and im-proving structural integrity,which are essential for extend-ing the cycle life and enhancing the safety of the batteries.This review considers the role of electrospinning in the fabrication of critical FLIB components,with a particular emphasis on the integration of carbon materials.It explores strategies to optimize FLIB performance by fine-tuning the electrospinning para-meters,such as electric field strength,spinning rate,solution concentration,and carbonization process.Precise control over fiber properties is crucial for enhancing battery reliability and stability during folding and bending.It also highlights the latest research findings in carbon-based electrode materials,high-performance electrolytes,and separator structures,discussing the practical challenges and opportunities these materials present.It underscores the significant impact of carbon materials on the evolution of FLIBs and their potential to shape future energy storage technologies.
基金the National Key R&D Plan of the Ministry of Science and Technology of China(2022YFE0122400)National Natural Science Foundation of China(52002238,22102207)+1 种基金Science and Technology Commission of Shanghai Municipality(22ZR1423800,21ZR1465200,23ZR1423600)Shanghai Municipal Education Commission and the NSRF via the Program Management Unit for Human Resources&Institutional Development,Research and Innovation(B49G680115).
文摘Silicon stands as a key anode material in lithium-ion battery ascribing to its high energy density.Nevertheless,the poor rate performance and limited cycling life remain unresolved through conventional approaches that involve carbon composites or nanostructures,primarily due to the un-controllable effects arising from the substantial formation of a solid electrolyte interphase(SEI)during the cycling.Here,an ultra-thin and homogeneous Ti doping alumina oxide catalytic interface is meticulously applied on the porous Si through a synergistic etching and hydrolysis process.This defect-rich oxide interface promotes a selective adsorption of fluoroethylene carbonate,leading to a catalytic reaction that can be aptly described as“molecular concentration-in situ conversion”.The resultant inorganic-rich SEI layer is electrochemical stable and favors ion-transport,particularly at high-rate cycling and high temperature.The robustly shielded porous Si,with a large surface area,achieves a high initial Coulombic efficiency of 84.7%and delivers exceptional high-rate performance at 25 A g^(−1)(692 mAh g^(−1))and a high Coulombic efficiency of 99.7%over 1000 cycles.The robust SEI constructed through a precious catalytic layer promises significant advantages for the fast development of silicon-based anode in fast-charging batteries.
基金supported by the Foundation of Yunnan Province(Nos.202301AU070021,202201BE070001-027)the Test Foundation of KUST(No.2022T20210208).
文摘Halide perovskite materials have received considerable attention for solar cells,LEDs,lasers etc.owing to their controllable physicochemical properties and structural advantages.However,little research has focused on energy storage and conversion applications,such as use as anodes in lithium-ion batteries.In this paper,all-inorganic lead-free halide perovskite Cs_(3)Bi_(2)Cl_(9)powders were synthesized by the grinding method,and the lattice was successfully adjusted via introducing Mn^(2+).The characterization results show that Mn-ion substitution can cause local lattice distortion to restructure the lattice,which will cause a mixed arrangement of[BiCl_(6)]octahedra to improve the performance of the anode material.This new material can provide a feasible solution for solving the problem of low specific capacity anode materials caused by unstable crystal structures,and also indicates that such perovskites with unique crystal structures and lattice tunability have broad application prospects in lithium-ion batteries.
基金supported by the National Natural Science Foundation of China(22279026,2247090373)the Natural Science Foundation of Chongqing(CSTB2022NSCQ-MSX1401)+2 种基金the China Postdoctoral Science Foundation(2024M764198)the National Natural Science Foundation of China(22509044)the Fundamental Research Funds for the Central Universities(grant no.HIT.OCEF.2022017).
文摘TiNb_(2)O_(7)represents an up-and-coming anode material for fast-charging lithium-ion batteries,but its practicalities are severely impeded by slow transfer rates of ionic and electronic especially at the low-temperature conditions.Herein,we introduce crystallographic engineering to enhance structure stability and promote Li+diffusion kinetics of TiNb_(2)O_(7)(TNO).The density functional theory computation reveals that Ti^(4+)is replaced by Sb^(5+)and Nb^(5+)in crystal lattices,which can reduce the Li+diffusion impediment and improve electronic conductivity.Synchrotron radiation X-ray 3D nano-computed tomography and in situ X-ray diffraction measurement confirm the introduction of Sb/Nb alleviates volume expansion during lithiation and delithiation processes,contributing to enhancing structure stability.Extended X-ray absorption fine structure spectra results verify that crystallographic engineering also increases short Nb-O bond length in TNO-Sb/Nb.Accordingly,the TNO-Sb/Nb anode delivers an outstanding capacity retention rate of 89.8%at 10 C after 700 cycles and excellent rate performance(140.4 mAh g^(−1) at 20 C).Even at−30℃,TNO-Sb/Nb anode delivers a capacity of 102.6 mAh g^(−1) with little capacity degeneration for 500 cycles.This work provides guidance for the design of fast-charging batteries at low-temperature condition.
基金financially supported by the National Key Research and Development Program of China(2023YFB3809300)。
文摘With the approaching of large-scale retirement of power lithium-ion batteries(LIBs),their urgent handling is required for environmental protection and resource reutilization.However,at present,substantial spent power batteries,especially for those high recovery value cathode materials,have not been greenly,sustainably,and efficiently recycled.Compared to the traditional recovery method for cathode materials with high energy consumption and severe secondary pollution,the direct repair regeneration,as a new type of short-process and efficient treatment methods,has attracted widespread attention.However,it still faces challenges in homogenization repair,electrochemical performance decline,and scaling-up production.To promote the direct regeneration technology development of failed NCM materials,herein we deeply discuss the failure mechanism of nickel-cobalt-manganese(NCM)ternary cathode materials,including element loss,Li/Ni mixing,phase transformation,structural defects,oxygen release,and surface degradation and reconstruction.Based on this,the detailed analysis and summary of the direct regeneration method embracing solid-phase sintering,eutectic salt assistance,solvothermal synthesis,sol-gel process,spray drying,and redox mediation are provided.Further,the upcycling strategy for regeneration materials,such as single-crystallization and high-nickelization,structural regulation,ion doping,and surface engineering,are discussed in deep.Finally,the challenges faced by the direct regeneration and corresponding countermeasures are pointed out.Undoubtedly,this review provides valuable guidance for the efficient and high-value recovery of failed cathode materials.
基金supported by the Jilin Provincial Science and Technology Development Plan Project(No.20220508003RC)the National Natural Science Foundation of China(52202440,52003012)。
文摘Lithium-ion batteries(LIBs)play a critical role in reducing carbon emissions in the automotive industry.However,they face challenges related to safety and performance failures.Smart technologies offer a promising solution to address these issues.Bioinspired microcapsules are a common approach to enhancing the performance and safety of smart LIBs.However,despite their potential,this area has not been thoroughly explored.This review provides an overview of the preparation methods for microcapsules,including physical,chemical,and physicochemical techniques.These microcapsules are categorized based on their mechanisms into electrode self-healing burst microcapsules,interphase-forming sustained-release microcapsules,live-lithium sustained-release microcapsules,and flame-retardant burst microcapsules.A comprehensive analysis of their bioinspired design concepts,mechanisms,and performance is presented,along with the design criteria for microcapsules suitable for LIBs.Finally,the review explores the potential applications of microcapsule technologies in LIBs and their future trends,such as enhancing existing technologies for novel applications like solid-state batteries and developing new types of microcapsules.This review aims to provide a foundation for the implementation of microcapsule technologies in LIBs and to highlight the latest advancements in smart batteries.
基金supported by National Natural Science Foundation of China(No.22205182)National Science Fund for Distinguished Young Scholars(No.52025034)+2 种基金China Postdoctoral Science Foundation(Nos.2022M722594/2024T171170)Guangdong Basic and Applied Basic Research Foundation(No.2024A1515011516)financially supported by Innovation Team of Shaanxi Sanqin Scholars。
文摘The development of lithium-ion batteries with high-energy densities is substantially hampered by the graphite anode's low theoretical capacity(372 mAh g^(-1)).There is an urgent need to explore novel anode materials for lithium-ion batteries.Silicon(Si),the second-largest element outside of Earth,has an exceptionally high specific capacity(3579 mAh g^(-1)),regarded as an excellent choice for the anode material in high-capacity lithium-ion batteries.However,it is low intrinsic conductivity and volume amplification during service status,prevented it from developing further.These difficulties can be successfully overcome by incorporating carbon into pure Si systems to form a composite anode and constructing a buffer structure.This review looks at the diffusion mechanism,various silicon-based anode material configurations(including sandwich,core-shell,yolk-shell,and other 3D mesh/porous structures),as well as the appropriate binders and electrolytes.Finally,a summary and viewpoints are offered on the characteristics and structural layout of various structures,metal/non-metal doping,and the compatibility and application of various binders and electrolytes for silicon-based anodes.This review aims to provide valuable insights into the research and development of silicon-based carbon anodes for high-performance lithium-ion batteries,as well as their integration with binders and electrolyte.
基金supported by the National Natural Science Foundation of China(NSFC No.52372200)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX23_0360).
文摘To accelerate the development of lithium-ion batteries(LIBs),researchers should urgently exploit next-generation electrodes with high specific capacity,long cycle stability,and excellent rate performance,such as TMOs,silicon-based materials,and alloys.Among all the modification measures,hierarchical micro-nano structure and yolk–shell structure are considered suitable and effective ways to improve the electrochemical performance of those novel materials.Herein,a facile glucose-assisted solvothermal method combined with heat treatment was implemented to synthesize hierarchical micro-nano yolk–shell V_(2)O_(3).The special-structured material exhibited higher specific capacity,better structure stability,and faster electrochemical kinetics compared with nanosheet-structured and micro-nano-cluster-structured V_(2)O_(3).When used as an anode for LIB,mnYS-V_(2)O_(3)delivered high specific capacity of 650.1 mA h g^(-1)after over 500 cycles at a current density of 100 mA g^(-1),with a retention of 93.4%.Moreover,the morphology evolution mechanism of micro-nano structure and yolk–shell structure was investigated in this work,which is beneficial to the design of other mnYS-structured TMOs.
基金supported by the National Key R&D Program of China(No.2022YFB2404400)the National Natural Science Foundation of China(Nos.U23A20577,52372168,92263206 and 21975006)+1 种基金the“The Youth Beijing Scholars program”(No.PXM2021_014204_000023)the Beijing Natural Science Foundation(Nos.2222001 and KM202110005009).
文摘The cobalt-free Mn-based Li-rich layered oxide material has the advantages of low cost,high energy density,and good performance at low temperatures,and is the promising choice for energy storage batteries.However,the long-cycling stability of batteries needs to be improved.Herein,the Mn-based Li-rich cathode materials with small amounts of Li2 MnO3 crystal domains and gradient doping of Al and Ti elements from the surface to the bulk have been developed to improve the structure and interface stability.Then the batteries with a high energy density of 600 Wh kg^(-1),excellent capacity retention of 99.7%with low voltage decay of 0.03 mV cycle^(-1) after 800 cycles,and good rates performances can be achieved.Therefore,the structure and cycling stability of low voltage Mn-based Li-rich cathode materials can be significantly improved by the bulk structure design and interface regulation,and this work has paved the way for developing low-cost and high-energy Mn-based energy storage batteries with long lifetime.
基金support from the National Nature Science Foundation of China(Grant No.52273256).
文摘Exploring electrode materials with larger capacity,higher power density and longer cycle life was critical for developing advanced flexible lithium-ion batteries(LIBs).Herein,we used a controlled two-step method including electrospraying followed with calcination treatment by CVD furnace to design novel electrodes of Si/Si_(x)/C and Sn/C microrods array consisting of nanospheres on flexible carbon cloth substrate(denoted as Si/Si_(x)/C@CC,Sn/C@CC).Microrods composed of cumulated nanospheres(the diameter was approximately 120 nm)had a mean diameter of approximately 1.5μm and a length of around 4.0μm,distributing uniformly along the entire woven carbon fibers.Both of Si/Si/Si_(x)/C@CC and Sn/C@CC products were synthesized as binder-free anodes for Li-ion battery with the features of high reversible capacity and excellent cycling.Especially Si/Six/C electrode exhibited high specific capacity of about 1750 mA∙h∙g^(−1)at 0.5 A∙g^(−1)and excellent cycling ability even after 1050 cycles with a capacity of 1388 mA∙h∙g^(−1).Highly flexible Si/Si_(x)/C@CC//LiCoO_(2)batteries based on liquid and solid electrolytes were also fabricated,exhibiting high flexibility,excellent electrical stability and potential applications in flexible wearable electronics.
基金supported by the National Natural Science Foundation of China Projects(Nos.52271213,52202299).
文摘Micro-silicon(Si)anode that features high theoretical capacity and fine tap density is ideal for energy-dense lithiumion batteries.However,the substantial localized mechanical strain caused by the large volume expansion often results in electrode disintegration and capacity loss.Herein,a microporous Si anode with the SiO_(x)/C layer functionalized all-surface and high tap density(~0.65 g cm^(-3))is developed by the hydrolysis-driven strategy that avoids the common use of corrosive etchants and toxic siloxane reagents.The functionalized inner pore with superior structural stability can effectively alleviate the volume change and enhance the electrolyte contact.Simultaneously,the outer particle surface forms a continuous network that prevents electrolyte parasitic decomposition,disperses the interface stress of Si matrix and facilitates electron/ion transport.As a result,the micron-sized Si anode shows only~9.94 GPa average stress at full lithiation state and delivers an impressive capacity of 901.1 mAh g^(-1)after 500 cycles at 1 A g^(-1).It also performs excellent rate performance of 1123.0 mAh g^(-1)at 5 A g^(-1)and 850.4 at 8 A g^(-1),far exceeding most of reported literatures.Furthermore,when paired with a commercial LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2),the pouch cell demonstrates high capacity and desirable cyclic performance.
基金supported by the National Key R&D Program of China(2022YFB3803501)the National Natural Science Foundation of China(22179008,22209156)+5 种基金support from the Beijing Nova Program(20230484241)support from the China Postdoctoral Science Foundation(2024M754084)the Postdoctoral Fellowship Program of CPSF(GZB20230931)support from beamline BL08U1A of Shanghai Synchrotron Radiation Facility(2024-SSRF-PT-506950)beamline 1W1B of the Beijing Synchrotron Radiation Facility(2021-BEPC-PT-006276)support from Initial Energy Science&Technology Co.,Ltd(IEST)。
文摘The implementation of ultrahigh-Ni cathodes in high-energy lithium-ion batteries(LIBs)is constrained by significant structural and interfacial degradation during cycling.In this study,doping-induced surface restructuring in ultrahigh-nickel cathode materials is rapidly facilitated through an ultrafast Joule heating method.Density functional theory(DFT)calculations,synchrotron X-ray absorption spectroscopy(XAS),and single-particle force test confirmed the establishment of a stable crystal framework and lattice oxygen,which mitigated H2-H3 phase transitions and improved structural reversibility.Additionally,the Sc doping process exhibits a pinning effect on the grain boundaries,as shown by scanning transmission electron microscopy(STEM),enhancing Li~+diffusion kinetics and decreasing mechanical strain during cycling.The in situ development of a cation-mixing layer at grain boundaries also creates a robust cathode/electrolyte interphase,effectively reducing interfacial parasitic reactions and transition metal dissolution,as validated by STEM and time-of-flight secondary ion mass spectrometry(TOF-SIMS).These synergistic modifications reduce particle cracking and surface/interface degradation,leading to enhanced rate capability,structural integrity,and thermal stability.Consequently,the optimized Sc-modified ultrahigh-Ni cathode(Sc-1)exhibits 93.99%capacity retention after 100 cycles at 1 C(25℃)and87.06%capacity retention after 100 cycles at 1 C(50℃),indicating excellent cycling and thermal stability.By presenting a one-step multifunctional modification approach,this research delivers an extensive analysis of the mechanisms governing the structure,microstructure,and interface properties of nickel-rich layered cathode materials(NCMs).These results underscore the potential of ultrahigh-Ni cathodes as viable candidates for advanced lithium-ion batteries(LIBs)in next-generation electric vehicles(EVs).
文摘Lithium-ion batteries(LIBs)are an electrochemical energy storage technology that has been widely used for portable electrical devices,electric vehicles,and grid storage,etc.To satisfy the demand for user convenience especially for electric vehicles,the development of a fast-charging technology for LIBs has become a critical focus.In commercial LIBs,the slow kinetics of Li+intercalation into the graphite anode from the electrolyte solution is known as the main restriction for fast-charging.We summarize the recent advances in obtaining fast-charging graphite-based anodes,mainly involving modifications of the electrolyte solution and graphite anode.Specifically,strategies for increasing the ionic conductivity and regulating the Li+solvation/desolvation state in the electrolyte solution,as well as optimizing the fabrication and the intrinsic activity of graphite-based anodes are discussed in detail.This review considers practical ways to obtain fast Li+intercalation kinetics into a graphite anode from the electrolyte as well as analysing progress in the commercialization of fast-charging LIBs.
