Silicon(Si)anode has been considered a promising candidate due to its remarkable theoretical capacity but it was plagued by severe pulverization because of the inherent huge volume variation.Enhancing electrode stabil...Silicon(Si)anode has been considered a promising candidate due to its remarkable theoretical capacity but it was plagued by severe pulverization because of the inherent huge volume variation.Enhancing electrode stability is an effective approach to improve electrochemical performance.Herein,a stable Si anode was established by an innovative construction of the bonding between conductive agents and active materials/binders.As a result,the strong interaction of electrode components not only effectively alleviates the volume expansion of Si but also achieves a stable interface by generating the beneficial solid electrolyte interphase(SEI)composition.Attributed to the deliberate scheme of the electrode,the Si anode exhibits sterling electrochemical performance.Besides,the device of the electrode is not only effective for other binders but also for other anode materials with high volume variation,thus shedding light on the rational design of electrodes for high-energy-density lithium-ion batteries.展开更多
Silicon-based materials have demonstrated remarkable potential in high-energy-density batteries owing to their high theoretical capacity.However,the significant volume expansion of silicon seriously hinders its utiliz...Silicon-based materials have demonstrated remarkable potential in high-energy-density batteries owing to their high theoretical capacity.However,the significant volume expansion of silicon seriously hinders its utilization as a lithium-ion anode.Herein,a functionalized high-toughness polyimide(PDMI) is synthesized by copolymerizing the 4,4'-Oxydiphthalic anhydride(ODPA) with 4,4'-oxydianiline(ODA),2,3-diaminobenzoic acid(DABA),and 1,3-bis(3-aminopropyl)-tetramethyl disiloxane(DMS).The combination of rigid benzene rings and flexible oxygen groups(-O-) in the PDMI molecular chain via a rigidness/softness coupling mechanism contributes to high toughness.The plentiful polar carboxyl(-COOH) groups establish robust bonding strength.Rapid ionic transport is achieved by incorporating the flexible siloxane segment(Si-O-Si),which imparts high molecular chain motility and augments free volume holes to facilitate lithium-ion transport(9.8 × 10^(-10) cm^(2) s^(-1) vs.16 × 10^(-10) cm^(2) s~(-1)).As expected,the SiO_x@PDMI-1.5 electrode delivers brilliant long-term cycle performance with a remarkable capacity retention of 85% over 500 cycles at 1.3 A g^(-1).The well-designed functionalized polyimide also significantly enhances the electrochemical properties of Si nanoparticles electrode.Meanwhile,the assembled SiO_x@PDMI-1.5/NCM811 full cell delivers a high retention of 80% after 100 cycles.The perspective of the binder design strategy based on polyimide modification delivers a novel path toward high-capacity electrodes for high-energy-density batteries.展开更多
Silicon(Si)has emerged as a potent anode material for lithium-ion batteries(LIBs),but faces challenges like low electrical conductivity and significant volume changes during lithiation/delithiation,leading to material...Silicon(Si)has emerged as a potent anode material for lithium-ion batteries(LIBs),but faces challenges like low electrical conductivity and significant volume changes during lithiation/delithiation,leading to material pulverization and capacity degradation.Recent research on nanostructured Si aims to mitigate volume expansion and enhance electrochemical performance,yet still grapples with issues like pulverization,unstable solid electrolyte interface(SEI)growth,and interparticle resistance.This review delves into innovative strategies for optimizing Si anodes’electrochemical performance via structural engineering,focusing on the synthesis of Si/C composites,engineering multidimensional nanostructures,and applying non-carbonaceous coatings.Forming a stable SEI is vital to prevent electrolyte decomposition and enhance Li^(+)transport,thereby stabilizing the Si anode interface and boosting cycling Coulombic efficiency.We also examine groundbreaking advancements such as self-healing polymers and advanced prelithiation methods to improve initial Coulombic efficiency and combat capacity loss.Our review uniquely provides a detailed examination of these strategies in real-world applications,moving beyond theoretical discussions.It offers a critical analysis of these approaches in terms of performance enhancement,scalability,and commercial feasibility.In conclusion,this review presents a comprehensive view and a forward-looking perspective on designing robust,high-performance Si-based anodes the next generation of LIBs.展开更多
The demand for lithium-ion batteries(LIBs)is driven largely by their use in electric vehicles,which is projected to increase dramatically in the future.This great success,however,urgently calls for the efficient recyc...The demand for lithium-ion batteries(LIBs)is driven largely by their use in electric vehicles,which is projected to increase dramatically in the future.This great success,however,urgently calls for the efficient recycling of LIBs at the end of their life.Herein,we describe a froth flotation-based process to recycle graphite—the predominant active material for the negative electrode—from spent LIBs and investigate its reuse in newly assembled LIBs.It has been found that the structure and morphology of the recycled graphite are essentially unchanged compared to pristine commercial anode-grade graphite,and despite some minor impurities from the recycling process,the recycled graphite provides a remarkable reversible specific capacity of more than 350 mAh g^(−1).Even more importantly,newly assembled graphite‖NMC532 cells show excellent cycling stability with a capacity retention of 80%after 1000 cycles,that is,comparable to the performance of reference full cells comprising pristine commercial graphite.展开更多
Separators play a critical role in the safety and performance of lithium-ion batteries.However,commercial polyolefin separators are limited by their poor affinity with electrolytes and low melting points.In this work,...Separators play a critical role in the safety and performance of lithium-ion batteries.However,commercial polyolefin separators are limited by their poor affinity with electrolytes and low melting points.In this work,we constructed a reinforced-concrete-like structure by homogeneously dispersing nano-Al_(2)O_(3) and cellulose on the separators to improve their stability and performance.In this reinforcedconcrete-like structure,the cellulose is a reinforcing mesh,and the nano-Al_(2)O_(3) acts as concrete to support the separator.After constructing the reinforced-concrete-like structure,the separators exhibit good stability even at 200℃(thermal shrinkage of 0.3%),enhanced tensile strain(tensile stress of 133.4 MPa and tensile strains of 62%),and better electrolyte wettability(a contact angle of 6.5°).Combining these advantages,the cells with nano-Al_(2)O_(3)@cellulose-coated separators exhibit stable cycling performance and good rate performance.Therefore,the construction of the reinforced-concretelike structure is a promising technology to promote the application of lithium-ion batteries in extreme environments.展开更多
Metal-organic frameworks(MOFs)are among the most promising materials for lithium-ion batteries(LIBs)owing to their high surface area,periodic porosity,adjustable pore size,and controllable chemical composition.For ins...Metal-organic frameworks(MOFs)are among the most promising materials for lithium-ion batteries(LIBs)owing to their high surface area,periodic porosity,adjustable pore size,and controllable chemical composition.For instance,their unique porous structures promote electrolyte penetration,ions transport,and make them ideal for battery separators.Regulating the chemical composition of MOF can introduce more active sites for electrochemical reactions.Therefore,MOFs and their related composites have been extensively and thoroughly explored for LIBs.However,the reported reviews solely include the applications of MOFs in the electrode materials of LIBs and rarely involve other aspects.A systematic review of the application of MOFs in LIBs is essential for understanding the mechanism of MOFs and better designing related MOFs battery materials.This review systematically evaluates the latest developments in pristine MOFs and MOF composites for LIB applications,including MOFs as the main materials(anode,cathode,separators,and electrolytes)to auxiliary materials(coating layers and additives for electrodes).Furthermore,the synthesis,modification methods,challenges,and prospects for the application of MOFs in LIBs are discussed.展开更多
The global importance of lithium-ion batteries(LIBs)has been increasingly underscored with the advancement of high-performance energy storage technologies.However,the end-of-life of these batteries poses significant c...The global importance of lithium-ion batteries(LIBs)has been increasingly underscored with the advancement of high-performance energy storage technologies.However,the end-of-life of these batteries poses significant challenges from environmental,economic,and resource management perspectives.This review paper focuses on the pyrometallurgy-based recycling process of lithium-ion batteries,exploring the fundamental understanding of this process and the importance of its optimization.Centering on the high energy consumption and emission gas issues of the pyrometallurgical recycling process,we systematically analyzed the capital-intensive nature of this process and the resulting technological characteristics.Furthermore,we conducted an in-depth discussion on the future research directions to overcome the existing technological barriers and limitations.This review will provide valuable insights for researchers and industry stakeholders in the battery recycling field.展开更多
Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode ...Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.展开更多
Silicon(Si)is a promising anode material for lithium‐ion batteries(LIBs)owing to its tremendously high theoretical storage capacity(4200 mAh g−1),which has the potential to elevate the energy of LIBs.However,Si anode...Silicon(Si)is a promising anode material for lithium‐ion batteries(LIBs)owing to its tremendously high theoretical storage capacity(4200 mAh g−1),which has the potential to elevate the energy of LIBs.However,Si anodes exhibit severe volume change during lithiation/delithiation processes,resulting in anode pulverization and delamination with detrimental growth of solid electrolyte interface layers.As a result,the cycling stability of Si anodes is insufficient for commercialization in LIBs.Polymeric binders can play critical roles in Si anodes by affecting their cycling stability,although they occupy a small portion of the electrodes.This review introduces crucial factors influencing polymeric binders'properties and the electrochemical performance of Si anodes.In particular,we emphasize the structure–property relationships of binders in the context of molecular design strategy,functional groups,types of interactions,and functionalities of binders.Furthermore,binders with additional functionalities,such as electrical conductivity and self‐healability,are extensively discussed,with an emphasis on the binder design principle.展开更多
Lithium-ion batteries are widely recognized as a crucial enabling technology for the advancement of electric vehicles and energy storage systems in the grid.The design of battery state estimation and control algorithm...Lithium-ion batteries are widely recognized as a crucial enabling technology for the advancement of electric vehicles and energy storage systems in the grid.The design of battery state estimation and control algorithms in battery management systems is usually based on battery models,which interpret crucial battery dynamics through the utilization of mathematical functions.Therefore,the investigation of battery dynamics with the purpose of battery system identification has garnered considerable attention in the realm of battery research.Characterization methods in terms of linear and nonlinear response of lithium-ion batteries have emerged as a prominent area of study in this field.This review has undertaken an analysis and discussion of characterization methods,with a particular focus on the motivation of battery system identification.Specifically,this work encompasses the incorporation of frequency domain nonlinear characterization methods and dynamics-based battery electrical models.The aim of this study is to establish a connection between the characterization and identification of battery systems for researchers and engineers specialized in the field of batteries,with the intention of promoting the advancement of efficient battery technology for real-world applications.展开更多
Al is considered as a promising lithium-ion battery(LIBs)anode materials owing to its high theoretical capacity and appropri-ate lithation/de-lithation potential.Unfortunately,its inevitable volume expansion causes th...Al is considered as a promising lithium-ion battery(LIBs)anode materials owing to its high theoretical capacity and appropri-ate lithation/de-lithation potential.Unfortunately,its inevitable volume expansion causes the electrode structure instability,leading to poor cyclic stability.What’s worse,the natural Al2O3 layer on commercial Al pellets is always existed as a robust insulating barrier for elec-trons,which brings the voltage dip and results in low reversible capacity.Herein,this work synthesized core-shell Al@C-Sn pellets for LIBs by a plus-minus strategy.In this proposal,the natural Al2O3 passivation layer is eliminated when annealing the pre-introduced SnCl2,meanwhile,polydopamine-derived carbon is introduced as dual functional shell to liberate the fresh Al core from re-oxidization and alle-viate the volume swellings.Benefiting from the addition of C-Sn shell and the elimination of the Al2O3 passivation layer,the as-prepared Al@C-Sn pellet electrode exhibits little voltage dip and delivers a reversible capacity of 1018.7 mAh·g^(-1) at 0.1 A·g^(-1) and 295.0 mAh·g^(-1) at 2.0 A·g^(-1)(after 1000 cycles),respectively.Moreover,its diffusion-controlled capacity is muchly improved compared to those of its counterparts,confirming the well-designed nanostructure contributes to the rapid Li-ion diffusion and further enhances the lithium storage activity.展开更多
Traditional hydrometallurgical methods for recovering spent lithium-ion batteries(LIBs)involve acid leaching to simultaneously extract all valuable metals into the leachate.These methods usually are followed by a seri...Traditional hydrometallurgical methods for recovering spent lithium-ion batteries(LIBs)involve acid leaching to simultaneously extract all valuable metals into the leachate.These methods usually are followed by a series of separation steps such as precipitation,extraction,and stripping to separate the individual valuable metals.In this study,we present a process for selectively leaching lithium through the synergistic effect of sulfuric and oxalic acids.Under optimal leaching conditions(leaching time of 1.5 h,leaching temperature of 70°C,liquid-solid ratio of 4 mL/g,oxalic acid ratio of 1.3,and sulfuric acid ratio of 1.3),the lithium leaching efficiency reached89.6%,and the leaching efficiencies of Ni,Co,and Mn were 12.8%,6.5%,and 21.7%.X-ray diffraction(XRD)and inductively coupled plasma optical emission spectrometer(ICP-OES)analyses showed that most of the Ni,Co,and Mn in the raw material remained as solid residue oxides and oxalates.This study offers a new approach to enriching the relevant theory for selectively recovering lithium from spent LIBs.展开更多
This work extensively investigates the thermal characteristic evolution of lithium-ion batteries under different degradation paths,and the evolution mechanism through multi-angle characterization is revealed.Under dif...This work extensively investigates the thermal characteristic evolution of lithium-ion batteries under different degradation paths,and the evolution mechanism through multi-angle characterization is revealed.Under different degradation paths,the evolution trend of temperature rise rate remains unchanged with respect to depth of discharge during the adiabatic discharge process,albeit to varying degrees of alteration.The temperature rise rate changes significantly with aging during the adiabatic discharge process under low-temperature cycling and high-rate cycling paths.The total heat generation rate,irreversible heat generation rate,and reversible heat generation rate exhibit similar evolution behavior with aging under different degradation paths.The interval range of endothermic process of reversible electrochemical reactions increases and the contribution of irreversible heat to the total heat increases with aging.To further standardize the assessment of different degradation paths on the thermal characteristics,this work introduces the innovative concept of“Ampere-hour temperature rise”.In low-temperature cycling and high-rate cycling paths,the ampere-hour temperature rise increases significantly with aging,particularly accentuated with higher discharge rates.Conversely,in high-temperature cycling and high-temperature storage paths,the ampere-hour temperature rise remains relatively stable during the initial stages of aging,yet undergoes a notable increase in the later stages of aging.The multi-angle characterization reveals distinct thermal evolution behavior under different degradation paths primarily attributed to different behavior changes of severe side reactions,such as lithium plating.The findings provide crucial insights for the safe utilization and management of lithium–ion batteries throughout the whole lifecycle.展开更多
Lithium-ion thermoelectrochemical cell(LTEC), featuring simultaneous energy conversion and storage, has emerged as promising candidate for low-grade heat harvesting. However, relatively poor thermosensitivity and heat...Lithium-ion thermoelectrochemical cell(LTEC), featuring simultaneous energy conversion and storage, has emerged as promising candidate for low-grade heat harvesting. However, relatively poor thermosensitivity and heat-to-current behavior limit the application of LTECs using LiPF_6 electrolyte. Introducing additives into bulk electrolyte is a reasonable strategy to solve such problem by modifying the solvation structure of electrolyte ions. In this work, we develop a dual-salt electrolyte with fluorosurfactant(FS) additive to achieve high thermopower and durability of LTECs during the conversion of low-grade heat into electricity. The addition of FS induces a unique Li~+ solvation with the aggregated double anions through a crowded electrolyte environment,resulting in an enhanced mobility kinetics of Li~+ as well as boosted thermoelectrochemical performances. By coupling optimized electrolyte with graphite electrode, a high thermopower of 13.8 mV K^(-1) and a normalized output power density of 3.99 mW m^(–2) K^(–2) as well as an outstanding output energy density of 607.96 J m^(-2) can be obtained.These results demonstrate that the optimization of electrolyte by regulating solvation structure will inject new vitality into the construction of thermoelectrochemical devices with attractive properties.展开更多
Battery remaining charging time(RCT)prediction can facilitate charging management and alleviate mileage anxiety for electric vehicles(EVs).Also,it is of great significance to improve EV users’experience.However,the R...Battery remaining charging time(RCT)prediction can facilitate charging management and alleviate mileage anxiety for electric vehicles(EVs).Also,it is of great significance to improve EV users’experience.However,the RCT for a lithiumion battery pack in EVs changes with temperature and other battery parameters.This study proposes an electrothermal model-based method to accurately predict battery RCT.Firstly,a characteristic battery cell is adopted to represent the battery pack,thus an equivalent circuit model(ECM)of the characteristic battery cell is established to describe the electrical behaviors of a battery pack.Secondly,an equivalent thermal model(ETM)of the battery pack is developed by considering the influence of ambient temperature,thermal management,and battery connectors in the battery pack to calculate the temperature which is then fed back to the ECM to realize electrothermal coupling.Finally,the RCT prediction method is proposed based on the electrothermal model and validated in the wide temperature range from-20℃to 45℃.The experimental results show that the prediction error of the RCT in the whole temperature range is less than 1.5%.展开更多
3D hierarchical flowerlike WS_(2) microspheres were synthesized through a facile one-pot hydrothermal route.The as-synthesized samples were characterized by powder X-ray powder diffraction (XRD),energy-dispersive spec...3D hierarchical flowerlike WS_(2) microspheres were synthesized through a facile one-pot hydrothermal route.The as-synthesized samples were characterized by powder X-ray powder diffraction (XRD),energy-dispersive spectroscopy (EDS),scanning electron microscopy (SEM) and Raman.SEM images of the samples reveal that the hierarchical flowerlike WS_(2) microspheres with diameters of about 3-5μm are composed of a number of curled nanosheets.Electrochemical tests such as charge/discharge,cyclic voltammetry,cycle life and rate performance were carried out on the WS_(2) sample.As an anode material for lithium-ion batteries,hierarchical flowerlike WS_(2) microspheres show excellent electrochemical performance.At a current density of100 mA·g^(-1),a high specific capacity of 647.8 mA·h·g^(-1) was achieved after 120 discharge/charge cycles.The excellent electrochemical performance of WS_(2) as an anode material for lithium-ion batteries can be attributed to its special 3D hierarchical structure.展开更多
This paper addresses the challenge of identifying abnormal states in Lithium-ion Battery(LiB)time series data.As the energy sector increasingly focuses on integrating distributed energy resources,Virtual Power Plants(...This paper addresses the challenge of identifying abnormal states in Lithium-ion Battery(LiB)time series data.As the energy sector increasingly focuses on integrating distributed energy resources,Virtual Power Plants(VPP)have become a vital new framework for energy management.LiBs are key in this context,owing to their high-efficiency energy storage capabilities essential for VPP operations.However,LiBs are prone to various abnormal states like overcharging,over-discharging,and internal short circuits,which impede power transmission efficiency.Traditional methods for detecting such abnormalities in LiB are too broad and lack precision for the dynamic and irregular nature of LiB data.In response,we introduce an innovative method:a Long Short-Term Memory(LSTM)autoencoder based on Dynamic Frequency Memory and Correlation Attention(DFMCA-LSTM-AE).This unsupervised,end-to-end approach is specifically designed for dynamically monitoring abnormal states in LiB data.The method starts with a Dynamic Frequency Fourier Transform module,which dynamically captures the frequency characteristics of time series data across three scales,incorporating a memory mechanism to reduce overgeneralization of abnormal frequencies.This is followed by integrating LSTM into both the encoder and decoder,enabling the model to effectively encode and decode the temporal relationships in the time series.Empirical tests on a real-world LiB dataset demonstrate that DFMCA-LSTM-AE outperforms existing models,achieving an average Area Under the Curve(AUC)of 90.73%and an F1 score of 83.83%.These results mark significant improvements over existing models,ranging from 2.4%–45.3%for AUC and 1.6%–28.9%for F1 score,showcasing the model’s enhanced accuracy and reliability in detecting abnormal states in LiB data.展开更多
Silicon suboxide(SiO_(x),x≈1)is promising in serving as an anode material for lithium-ion batteries with high capacity,but it has a low initial Coulombic efficiency(ICE)due to the irreversible formation of lithium si...Silicon suboxide(SiO_(x),x≈1)is promising in serving as an anode material for lithium-ion batteries with high capacity,but it has a low initial Coulombic efficiency(ICE)due to the irreversible formation of lithium silicates during the first cycle.In this work,we modify SiO_(x) by solid-phase Mg doping reaction using low-cost Mg powder as a reducing agent.We show that Mg reduces SiO_(2) in SiO_(x) to Si and forms MgSiO_(3) or Mg_(2)SiO_(4).The MgSiO_(3) or Mg_(2)SiO_(4) are mainly distributed on the surface of SiO_(x),which suppresses the irreversible lithium-ion loss and enhances the ICE of SiO_(x).However,the formation of MgSiO_(3) or Mg_(2)SiO_(4) also sacrifices the capacity of SiO_(x).Therefore,by controlling the reaction process between Mg and SiO_(x),we can tune the phase composition,proportion,and morphology of the Mg-doped SiO_(x) and manipulate the performance.We obtain samples with a capacity of 1226 mAh g^(–1) and an ICE of 84.12%,which show significant improvement over carbon-coated SiO_(x) without Mg doping.By the synergistical modification of both Mg doping and prelithiation,the capacity of SiO_(x) is further increased to 1477 mAh g^(–1) with a minimal compromise in the ICE(83.77%).展开更多
In order to solve the problem of inconsistent energy in the charging and discharging cycles of lithium-ion battery packs,a new multilayer equilibrium topology is designed in this paper.The structure adopts a hierarchi...In order to solve the problem of inconsistent energy in the charging and discharging cycles of lithium-ion battery packs,a new multilayer equilibrium topology is designed in this paper.The structure adopts a hierarchical structure design,which includes intra-group equilibrium,primary inter-group equilibrium and secondary inter-group equilibrium.This structure greatly increases the number of equilibrium paths for lithium-ion batteries,thus shortening the time required for equilibrium,and improving the overall efficiency.In terms of control strategy,fuzzy logic control(FLC)is chosen to control the size of the equilibrium current during the equilibrium process.We performed rigorous modeling and simulation of the proposed system by MATLAB and Simulink software.Experiments show that the multilayer equilibrium circuit structure greatly exceeds the traditional single-layer equilibrium circuit in terms of efficacy,specifically,the Li-ion battery equilibrium speed is improved by 12.71%in static equilibrium,14.48%in charge equilibrium,and 11.19%in discharge equilibrium.In addition,compared with the maximum value algorithm,the use of the FLC algorithm reduces the equalization time by about 3.27%and improves the energy transfer efficiency by about 66.49%under the stationary condition,which verifies the feasibility of the equalization scheme.展开更多
基金the National Natural Science Foundation of China(51874108,52164036,52264046)the Guizhou High Level and Innovative Talents Projects([2022]009-1)+1 种基金the Guizhou Science and Technology Planning Project([2020]5021)the Natural Science Research Project of Guizhou Provincial Department of Education([2022]041)。
文摘Silicon(Si)anode has been considered a promising candidate due to its remarkable theoretical capacity but it was plagued by severe pulverization because of the inherent huge volume variation.Enhancing electrode stability is an effective approach to improve electrochemical performance.Herein,a stable Si anode was established by an innovative construction of the bonding between conductive agents and active materials/binders.As a result,the strong interaction of electrode components not only effectively alleviates the volume expansion of Si but also achieves a stable interface by generating the beneficial solid electrolyte interphase(SEI)composition.Attributed to the deliberate scheme of the electrode,the Si anode exhibits sterling electrochemical performance.Besides,the device of the electrode is not only effective for other binders but also for other anode materials with high volume variation,thus shedding light on the rational design of electrodes for high-energy-density lithium-ion batteries.
基金supported by the National Natural Science Foundation of China (51673017)the National Natural Science Foundation of China (21404005)+1 种基金the Fundamental Research Funds for the Central Universities (XK1802-2)the Natural Science Foundation of Jiangsu Province (BK20150273)。
文摘Silicon-based materials have demonstrated remarkable potential in high-energy-density batteries owing to their high theoretical capacity.However,the significant volume expansion of silicon seriously hinders its utilization as a lithium-ion anode.Herein,a functionalized high-toughness polyimide(PDMI) is synthesized by copolymerizing the 4,4'-Oxydiphthalic anhydride(ODPA) with 4,4'-oxydianiline(ODA),2,3-diaminobenzoic acid(DABA),and 1,3-bis(3-aminopropyl)-tetramethyl disiloxane(DMS).The combination of rigid benzene rings and flexible oxygen groups(-O-) in the PDMI molecular chain via a rigidness/softness coupling mechanism contributes to high toughness.The plentiful polar carboxyl(-COOH) groups establish robust bonding strength.Rapid ionic transport is achieved by incorporating the flexible siloxane segment(Si-O-Si),which imparts high molecular chain motility and augments free volume holes to facilitate lithium-ion transport(9.8 × 10^(-10) cm^(2) s^(-1) vs.16 × 10^(-10) cm^(2) s~(-1)).As expected,the SiO_x@PDMI-1.5 electrode delivers brilliant long-term cycle performance with a remarkable capacity retention of 85% over 500 cycles at 1.3 A g^(-1).The well-designed functionalized polyimide also significantly enhances the electrochemical properties of Si nanoparticles electrode.Meanwhile,the assembled SiO_x@PDMI-1.5/NCM811 full cell delivers a high retention of 80% after 100 cycles.The perspective of the binder design strategy based on polyimide modification delivers a novel path toward high-capacity electrodes for high-energy-density batteries.
基金financially supported by the Jiangsu Distinguished Professors Project(No.1711510024)the funding for Scientific Research Startup of Jiangsu University(Nos.4111510015,19JDG044)+3 种基金the Jiangsu Provincial Program for High-Level Innovative and Entrepreneurial Talents Introductionthe National Natural Science Foundation of China(No.22008091)Natural Science Foundation of Guangdong Province(2023A1515010894)the Open Project of Luzhou Key Laboratory of Fine Chemical Application Technology(HYJH-2302-A).
文摘Silicon(Si)has emerged as a potent anode material for lithium-ion batteries(LIBs),but faces challenges like low electrical conductivity and significant volume changes during lithiation/delithiation,leading to material pulverization and capacity degradation.Recent research on nanostructured Si aims to mitigate volume expansion and enhance electrochemical performance,yet still grapples with issues like pulverization,unstable solid electrolyte interface(SEI)growth,and interparticle resistance.This review delves into innovative strategies for optimizing Si anodes’electrochemical performance via structural engineering,focusing on the synthesis of Si/C composites,engineering multidimensional nanostructures,and applying non-carbonaceous coatings.Forming a stable SEI is vital to prevent electrolyte decomposition and enhance Li^(+)transport,thereby stabilizing the Si anode interface and boosting cycling Coulombic efficiency.We also examine groundbreaking advancements such as self-healing polymers and advanced prelithiation methods to improve initial Coulombic efficiency and combat capacity loss.Our review uniquely provides a detailed examination of these strategies in real-world applications,moving beyond theoretical discussions.It offers a critical analysis of these approaches in terms of performance enhancement,scalability,and commercial feasibility.In conclusion,this review presents a comprehensive view and a forward-looking perspective on designing robust,high-performance Si-based anodes the next generation of LIBs.
基金Bundesministerium für Bildung und Forschung,Grant/Award Numbers:03XP0138C,03XP0306C。
文摘The demand for lithium-ion batteries(LIBs)is driven largely by their use in electric vehicles,which is projected to increase dramatically in the future.This great success,however,urgently calls for the efficient recycling of LIBs at the end of their life.Herein,we describe a froth flotation-based process to recycle graphite—the predominant active material for the negative electrode—from spent LIBs and investigate its reuse in newly assembled LIBs.It has been found that the structure and morphology of the recycled graphite are essentially unchanged compared to pristine commercial anode-grade graphite,and despite some minor impurities from the recycling process,the recycled graphite provides a remarkable reversible specific capacity of more than 350 mAh g^(−1).Even more importantly,newly assembled graphite‖NMC532 cells show excellent cycling stability with a capacity retention of 80%after 1000 cycles,that is,comparable to the performance of reference full cells comprising pristine commercial graphite.
基金funding from the Natural Science Foundation of China(22278150,22075086,22138005,and 22141001)the Guangdong Basic and Applied Basic Research Foundation(2022A1515010980,2023A1515010046)the Fundamental Research Funds for the Central Universities(2022ZYGXZR101).
文摘Separators play a critical role in the safety and performance of lithium-ion batteries.However,commercial polyolefin separators are limited by their poor affinity with electrolytes and low melting points.In this work,we constructed a reinforced-concrete-like structure by homogeneously dispersing nano-Al_(2)O_(3) and cellulose on the separators to improve their stability and performance.In this reinforcedconcrete-like structure,the cellulose is a reinforcing mesh,and the nano-Al_(2)O_(3) acts as concrete to support the separator.After constructing the reinforced-concrete-like structure,the separators exhibit good stability even at 200℃(thermal shrinkage of 0.3%),enhanced tensile strain(tensile stress of 133.4 MPa and tensile strains of 62%),and better electrolyte wettability(a contact angle of 6.5°).Combining these advantages,the cells with nano-Al_(2)O_(3)@cellulose-coated separators exhibit stable cycling performance and good rate performance.Therefore,the construction of the reinforced-concretelike structure is a promising technology to promote the application of lithium-ion batteries in extreme environments.
基金supported by the National Natural Science Foundation of China(22179006)。
文摘Metal-organic frameworks(MOFs)are among the most promising materials for lithium-ion batteries(LIBs)owing to their high surface area,periodic porosity,adjustable pore size,and controllable chemical composition.For instance,their unique porous structures promote electrolyte penetration,ions transport,and make them ideal for battery separators.Regulating the chemical composition of MOF can introduce more active sites for electrochemical reactions.Therefore,MOFs and their related composites have been extensively and thoroughly explored for LIBs.However,the reported reviews solely include the applications of MOFs in the electrode materials of LIBs and rarely involve other aspects.A systematic review of the application of MOFs in LIBs is essential for understanding the mechanism of MOFs and better designing related MOFs battery materials.This review systematically evaluates the latest developments in pristine MOFs and MOF composites for LIB applications,including MOFs as the main materials(anode,cathode,separators,and electrolytes)to auxiliary materials(coating layers and additives for electrodes).Furthermore,the synthesis,modification methods,challenges,and prospects for the application of MOFs in LIBs are discussed.
基金the Technology Innovation Program(or Industrial Strategic Technology Development Program)and the Ministry of Trade,Industry&Energy(MOTIE)of the Republic of Korea(No.20022950)。
文摘The global importance of lithium-ion batteries(LIBs)has been increasingly underscored with the advancement of high-performance energy storage technologies.However,the end-of-life of these batteries poses significant challenges from environmental,economic,and resource management perspectives.This review paper focuses on the pyrometallurgy-based recycling process of lithium-ion batteries,exploring the fundamental understanding of this process and the importance of its optimization.Centering on the high energy consumption and emission gas issues of the pyrometallurgical recycling process,we systematically analyzed the capital-intensive nature of this process and the resulting technological characteristics.Furthermore,we conducted an in-depth discussion on the future research directions to overcome the existing technological barriers and limitations.This review will provide valuable insights for researchers and industry stakeholders in the battery recycling field.
基金the financial support by the National Science Foundation of China(51822706 and 52107234)Beijing Natural Science Foundation(JQ19012)+2 种基金the DNL Cooperation Fund,CAS(DNL201912 and DNL201915)Innovation Academy for Green Manufacture Fund(IAGM2020C02)Youth Innovation Promotion Association,CAS(Y2021052).
文摘Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.
基金National Research Foundation,Grant/Award Number:2022R1A2C1092273。
文摘Silicon(Si)is a promising anode material for lithium‐ion batteries(LIBs)owing to its tremendously high theoretical storage capacity(4200 mAh g−1),which has the potential to elevate the energy of LIBs.However,Si anodes exhibit severe volume change during lithiation/delithiation processes,resulting in anode pulverization and delamination with detrimental growth of solid electrolyte interface layers.As a result,the cycling stability of Si anodes is insufficient for commercialization in LIBs.Polymeric binders can play critical roles in Si anodes by affecting their cycling stability,although they occupy a small portion of the electrodes.This review introduces crucial factors influencing polymeric binders'properties and the electrochemical performance of Si anodes.In particular,we emphasize the structure–property relationships of binders in the context of molecular design strategy,functional groups,types of interactions,and functionalities of binders.Furthermore,binders with additional functionalities,such as electrical conductivity and self‐healability,are extensively discussed,with an emphasis on the binder design principle.
基金supported by the National Natural Science Foundation of China(Grant No.62373224)the Scientific Research Foundation of Nanjing Institute of Technology(Grant No.YKJ202212)+1 种基金the Nanjing Overseas Educated Personnel Science and Technology Innovation Projectthe Open Research Fund of Jiangsu Collaborative Innovation Center for Smart Distribution Network,Nanjing Institute of Technology(Grant No.XTCX202307)。
文摘Lithium-ion batteries are widely recognized as a crucial enabling technology for the advancement of electric vehicles and energy storage systems in the grid.The design of battery state estimation and control algorithms in battery management systems is usually based on battery models,which interpret crucial battery dynamics through the utilization of mathematical functions.Therefore,the investigation of battery dynamics with the purpose of battery system identification has garnered considerable attention in the realm of battery research.Characterization methods in terms of linear and nonlinear response of lithium-ion batteries have emerged as a prominent area of study in this field.This review has undertaken an analysis and discussion of characterization methods,with a particular focus on the motivation of battery system identification.Specifically,this work encompasses the incorporation of frequency domain nonlinear characterization methods and dynamics-based battery electrical models.The aim of this study is to establish a connection between the characterization and identification of battery systems for researchers and engineers specialized in the field of batteries,with the intention of promoting the advancement of efficient battery technology for real-world applications.
基金supported by the National Natural Science Foundation of China(No.62105277)the Natural Science Foundation of Henan Province(No.232300420139)the Internationalization Training of High-Level Talents of Henan Province,and Nanhu Scholars Program for Young Scholars of XYNU.
文摘Al is considered as a promising lithium-ion battery(LIBs)anode materials owing to its high theoretical capacity and appropri-ate lithation/de-lithation potential.Unfortunately,its inevitable volume expansion causes the electrode structure instability,leading to poor cyclic stability.What’s worse,the natural Al2O3 layer on commercial Al pellets is always existed as a robust insulating barrier for elec-trons,which brings the voltage dip and results in low reversible capacity.Herein,this work synthesized core-shell Al@C-Sn pellets for LIBs by a plus-minus strategy.In this proposal,the natural Al2O3 passivation layer is eliminated when annealing the pre-introduced SnCl2,meanwhile,polydopamine-derived carbon is introduced as dual functional shell to liberate the fresh Al core from re-oxidization and alle-viate the volume swellings.Benefiting from the addition of C-Sn shell and the elimination of the Al2O3 passivation layer,the as-prepared Al@C-Sn pellet electrode exhibits little voltage dip and delivers a reversible capacity of 1018.7 mAh·g^(-1) at 0.1 A·g^(-1) and 295.0 mAh·g^(-1) at 2.0 A·g^(-1)(after 1000 cycles),respectively.Moreover,its diffusion-controlled capacity is muchly improved compared to those of its counterparts,confirming the well-designed nanostructure contributes to the rapid Li-ion diffusion and further enhances the lithium storage activity.
基金financially supported by the Young Scientists Fund of the National Natural Science Foundation of China(Nos.52104395 and 52304365)the Science and Technology Planning Project of Guangzhou,China(Nos.202102021080 and 2024A04J10006)+1 种基金the National Key R&D Program of China(No.2021YFC2902605)the Natural Science Foundation of Guangdong Province,China(Nos.2023A1515030145 and 2023A1515011847)。
文摘Traditional hydrometallurgical methods for recovering spent lithium-ion batteries(LIBs)involve acid leaching to simultaneously extract all valuable metals into the leachate.These methods usually are followed by a series of separation steps such as precipitation,extraction,and stripping to separate the individual valuable metals.In this study,we present a process for selectively leaching lithium through the synergistic effect of sulfuric and oxalic acids.Under optimal leaching conditions(leaching time of 1.5 h,leaching temperature of 70°C,liquid-solid ratio of 4 mL/g,oxalic acid ratio of 1.3,and sulfuric acid ratio of 1.3),the lithium leaching efficiency reached89.6%,and the leaching efficiencies of Ni,Co,and Mn were 12.8%,6.5%,and 21.7%.X-ray diffraction(XRD)and inductively coupled plasma optical emission spectrometer(ICP-OES)analyses showed that most of the Ni,Co,and Mn in the raw material remained as solid residue oxides and oxalates.This study offers a new approach to enriching the relevant theory for selectively recovering lithium from spent LIBs.
基金This work is supported by the National Natural Science Foundation of China(NSFC,Nos.52176199,and U20A20310)supported by the Program of Shanghai Academic/Technology Research Leader(22XD1423800).
文摘This work extensively investigates the thermal characteristic evolution of lithium-ion batteries under different degradation paths,and the evolution mechanism through multi-angle characterization is revealed.Under different degradation paths,the evolution trend of temperature rise rate remains unchanged with respect to depth of discharge during the adiabatic discharge process,albeit to varying degrees of alteration.The temperature rise rate changes significantly with aging during the adiabatic discharge process under low-temperature cycling and high-rate cycling paths.The total heat generation rate,irreversible heat generation rate,and reversible heat generation rate exhibit similar evolution behavior with aging under different degradation paths.The interval range of endothermic process of reversible electrochemical reactions increases and the contribution of irreversible heat to the total heat increases with aging.To further standardize the assessment of different degradation paths on the thermal characteristics,this work introduces the innovative concept of“Ampere-hour temperature rise”.In low-temperature cycling and high-rate cycling paths,the ampere-hour temperature rise increases significantly with aging,particularly accentuated with higher discharge rates.Conversely,in high-temperature cycling and high-temperature storage paths,the ampere-hour temperature rise remains relatively stable during the initial stages of aging,yet undergoes a notable increase in the later stages of aging.The multi-angle characterization reveals distinct thermal evolution behavior under different degradation paths primarily attributed to different behavior changes of severe side reactions,such as lithium plating.The findings provide crucial insights for the safe utilization and management of lithium–ion batteries throughout the whole lifecycle.
基金supported by the Leading Edge Technology of Jiangsu Province (BK20220009, BK20202008)Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)。
文摘Lithium-ion thermoelectrochemical cell(LTEC), featuring simultaneous energy conversion and storage, has emerged as promising candidate for low-grade heat harvesting. However, relatively poor thermosensitivity and heat-to-current behavior limit the application of LTECs using LiPF_6 electrolyte. Introducing additives into bulk electrolyte is a reasonable strategy to solve such problem by modifying the solvation structure of electrolyte ions. In this work, we develop a dual-salt electrolyte with fluorosurfactant(FS) additive to achieve high thermopower and durability of LTECs during the conversion of low-grade heat into electricity. The addition of FS induces a unique Li~+ solvation with the aggregated double anions through a crowded electrolyte environment,resulting in an enhanced mobility kinetics of Li~+ as well as boosted thermoelectrochemical performances. By coupling optimized electrolyte with graphite electrode, a high thermopower of 13.8 mV K^(-1) and a normalized output power density of 3.99 mW m^(–2) K^(–2) as well as an outstanding output energy density of 607.96 J m^(-2) can be obtained.These results demonstrate that the optimization of electrolyte by regulating solvation structure will inject new vitality into the construction of thermoelectrochemical devices with attractive properties.
基金Supported by National Key R&D Program of China(Grant No.2021YFB2402002)Beijing Municipal Natural Science Foundation of China(Grant No.L223013).
文摘Battery remaining charging time(RCT)prediction can facilitate charging management and alleviate mileage anxiety for electric vehicles(EVs).Also,it is of great significance to improve EV users’experience.However,the RCT for a lithiumion battery pack in EVs changes with temperature and other battery parameters.This study proposes an electrothermal model-based method to accurately predict battery RCT.Firstly,a characteristic battery cell is adopted to represent the battery pack,thus an equivalent circuit model(ECM)of the characteristic battery cell is established to describe the electrical behaviors of a battery pack.Secondly,an equivalent thermal model(ETM)of the battery pack is developed by considering the influence of ambient temperature,thermal management,and battery connectors in the battery pack to calculate the temperature which is then fed back to the ECM to realize electrothermal coupling.Finally,the RCT prediction method is proposed based on the electrothermal model and validated in the wide temperature range from-20℃to 45℃.The experimental results show that the prediction error of the RCT in the whole temperature range is less than 1.5%.
基金Funded by the Jiangsu Province Industry-University-Research Cooperation Project (No.BY2018314)the Scientific Research Foundation of Jiangsu University of Technology (No.KYY18030)Jiangsu Overseas Visiting Scholar Program for University Prominent Young&Middle-aged Teachers and Presidents。
文摘3D hierarchical flowerlike WS_(2) microspheres were synthesized through a facile one-pot hydrothermal route.The as-synthesized samples were characterized by powder X-ray powder diffraction (XRD),energy-dispersive spectroscopy (EDS),scanning electron microscopy (SEM) and Raman.SEM images of the samples reveal that the hierarchical flowerlike WS_(2) microspheres with diameters of about 3-5μm are composed of a number of curled nanosheets.Electrochemical tests such as charge/discharge,cyclic voltammetry,cycle life and rate performance were carried out on the WS_(2) sample.As an anode material for lithium-ion batteries,hierarchical flowerlike WS_(2) microspheres show excellent electrochemical performance.At a current density of100 mA·g^(-1),a high specific capacity of 647.8 mA·h·g^(-1) was achieved after 120 discharge/charge cycles.The excellent electrochemical performance of WS_(2) as an anode material for lithium-ion batteries can be attributed to its special 3D hierarchical structure.
基金supported by“Regional Innovation Strategy(RIS)”through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(MOE)(2021RIS-002)the Technology Development Program(RS-2023-00278623)funded by the Ministry of SMEs and Startups(MSS,Korea).
文摘This paper addresses the challenge of identifying abnormal states in Lithium-ion Battery(LiB)time series data.As the energy sector increasingly focuses on integrating distributed energy resources,Virtual Power Plants(VPP)have become a vital new framework for energy management.LiBs are key in this context,owing to their high-efficiency energy storage capabilities essential for VPP operations.However,LiBs are prone to various abnormal states like overcharging,over-discharging,and internal short circuits,which impede power transmission efficiency.Traditional methods for detecting such abnormalities in LiB are too broad and lack precision for the dynamic and irregular nature of LiB data.In response,we introduce an innovative method:a Long Short-Term Memory(LSTM)autoencoder based on Dynamic Frequency Memory and Correlation Attention(DFMCA-LSTM-AE).This unsupervised,end-to-end approach is specifically designed for dynamically monitoring abnormal states in LiB data.The method starts with a Dynamic Frequency Fourier Transform module,which dynamically captures the frequency characteristics of time series data across three scales,incorporating a memory mechanism to reduce overgeneralization of abnormal frequencies.This is followed by integrating LSTM into both the encoder and decoder,enabling the model to effectively encode and decode the temporal relationships in the time series.Empirical tests on a real-world LiB dataset demonstrate that DFMCA-LSTM-AE outperforms existing models,achieving an average Area Under the Curve(AUC)of 90.73%and an F1 score of 83.83%.These results mark significant improvements over existing models,ranging from 2.4%–45.3%for AUC and 1.6%–28.9%for F1 score,showcasing the model’s enhanced accuracy and reliability in detecting abnormal states in LiB data.
基金supported by the National Natural Science Foundation(52232009)the National Natural Science Foundation for Distinguished Young Scholar(52125404)+1 种基金the National Youth Talent Support Program,“131”First Level Innovative Talents Training Project in Tianjinthe Tianjin Natural Science Foundation for Distinguished Young Scholar(18JCJQJC46500).
文摘Silicon suboxide(SiO_(x),x≈1)is promising in serving as an anode material for lithium-ion batteries with high capacity,but it has a low initial Coulombic efficiency(ICE)due to the irreversible formation of lithium silicates during the first cycle.In this work,we modify SiO_(x) by solid-phase Mg doping reaction using low-cost Mg powder as a reducing agent.We show that Mg reduces SiO_(2) in SiO_(x) to Si and forms MgSiO_(3) or Mg_(2)SiO_(4).The MgSiO_(3) or Mg_(2)SiO_(4) are mainly distributed on the surface of SiO_(x),which suppresses the irreversible lithium-ion loss and enhances the ICE of SiO_(x).However,the formation of MgSiO_(3) or Mg_(2)SiO_(4) also sacrifices the capacity of SiO_(x).Therefore,by controlling the reaction process between Mg and SiO_(x),we can tune the phase composition,proportion,and morphology of the Mg-doped SiO_(x) and manipulate the performance.We obtain samples with a capacity of 1226 mAh g^(–1) and an ICE of 84.12%,which show significant improvement over carbon-coated SiO_(x) without Mg doping.By the synergistical modification of both Mg doping and prelithiation,the capacity of SiO_(x) is further increased to 1477 mAh g^(–1) with a minimal compromise in the ICE(83.77%).
基金funded by the National Natural Science Foundation of China:Research on the Energy Management Strategy of Li-Ion Battery and Sc Hybrid Energy Storage System for Electric Vehicle(51677058).
文摘In order to solve the problem of inconsistent energy in the charging and discharging cycles of lithium-ion battery packs,a new multilayer equilibrium topology is designed in this paper.The structure adopts a hierarchical structure design,which includes intra-group equilibrium,primary inter-group equilibrium and secondary inter-group equilibrium.This structure greatly increases the number of equilibrium paths for lithium-ion batteries,thus shortening the time required for equilibrium,and improving the overall efficiency.In terms of control strategy,fuzzy logic control(FLC)is chosen to control the size of the equilibrium current during the equilibrium process.We performed rigorous modeling and simulation of the proposed system by MATLAB and Simulink software.Experiments show that the multilayer equilibrium circuit structure greatly exceeds the traditional single-layer equilibrium circuit in terms of efficacy,specifically,the Li-ion battery equilibrium speed is improved by 12.71%in static equilibrium,14.48%in charge equilibrium,and 11.19%in discharge equilibrium.In addition,compared with the maximum value algorithm,the use of the FLC algorithm reduces the equalization time by about 3.27%and improves the energy transfer efficiency by about 66.49%under the stationary condition,which verifies the feasibility of the equalization scheme.