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
Thermal runaway(TR)is a critical issue hindering the large-scale application of lithium-ion batteries(LIBs).Understanding the thermal safety behavior of LIBs at the cell and module level under different state of charg...Thermal runaway(TR)is a critical issue hindering the large-scale application of lithium-ion batteries(LIBs).Understanding the thermal safety behavior of LIBs at the cell and module level under different state of charges(SOCs)has significant implications for reinforcing the thermal safety design of the lithium-ion battery module.This study first investigates the thermal safety boundary(TSB)correspondence at the cells and modules level under the guidance of a newly proposed concept,safe electric quantity boundary(SEQB).A reasonable thermal runaway propagation(TRP)judgment indicator,peak heat transfer power(PHTP),is proposed to predict whether TRP occurs.Moreover,a validated 3D model is used to quantitatively clarify the TSB at different SOCs from the perspective of PHTP,TR trigger temperature,SOC,and the full cycle life.Besides,three different TRP transfer modes are discovered.The interconversion relationship of three different TRP modes is investigated from the perspective of PHTP.This paper explores the TSB of LIBs under different SOCs at both cell and module levels for the first time,which has great significance in guiding the thermal safety design of battery systems.展开更多
To effectively separate and recover Co(Ⅱ) from the leachate of spent lithium-ion battery cathodes,we investigated solvent extraction with quaternary ammonium salt N263 in the sodium nitrite system.NO_(2)^(-)combines ...To effectively separate and recover Co(Ⅱ) from the leachate of spent lithium-ion battery cathodes,we investigated solvent extraction with quaternary ammonium salt N263 in the sodium nitrite system.NO_(2)^(-)combines with Co(Ⅱ) to form an anion [Co(NO_(2))_(3)]^(-),and it is then extracted by N263.The extraction of Co(Ⅱ) is related to the concentration of NO_(2)^(-).The extraction efficiency of Co(Ⅱ) reaches the maximum of99.16%,while the extraction efficiencies of Ni(Ⅱ),Mn(Ⅱ),and Li(Ⅰ) are 9.27%-9.80% under the following conditions:30vol% of N263 and15vol% of iso-propyl alcohol in sulfonated kerosene,the volume ratio of the aqueous-to-organic phase is 2:1,the extraction time is 30 min,and1 M sodium nitrite in 0.1 MHNO_(3).The theoretical stages require for the Co(Ⅱ) extraction are performed in the McCabe–Thiele diagram,and the extraction efficiency of Co(Ⅱ) reaches more than 99.00% after three-stage counter-current extraction with Co(Ⅱ) concentration of 2544mg/L.When the HCl concentration is 1.5 M,the volume ratio of the aqueous-to-organic phase is 1:1,the back-extraction efficiency of Co(Ⅱ)achieves 91.41%.After five extraction and back-extraction cycles,the Co(Ⅱ) extraction efficiency can still reach 93.89%.The Co(Ⅱ) extraction efficiency in the actual leaching solution reaches 100%.展开更多
Green energy storage devices play vital roles in reducing fossil fuel emissions and achieving carbon neutrality by 2050.Growing markets for portable electronics and electric vehicles create tremendous demand for advan...Green energy storage devices play vital roles in reducing fossil fuel emissions and achieving carbon neutrality by 2050.Growing markets for portable electronics and electric vehicles create tremendous demand for advanced lithium-ion batteries(LIBs)with high power and energy density,and novel electrode material with high capacity and energy density is one of the keys to next-generation LIBs.Silicon-based materials,with high specific capacity,abundant natural resources,high-level safety and environmental friendliness,are quite promising alternative anode materials.However,significant volume expansion and redundant side reactions with electrolytes lead to active lithium loss and decreased coulombic efficiency(CE)of silicon-based material,which hinders the commercial application of silicon-based anode.Prelithiation,preembedding extra lithium ions in the electrodes,is a promising approach to replenish the lithium loss during cycling.Recent progress on prelithiation strategies for silicon-based anode,including electrochemical method,chemical method,direct contact method,and active material method,and their practical potentials are reviewed and prospected here.The development of advanced Si-based material and prelithiation technologies is expected to provide promising approaches for the large-scale application of silicon-based materials.展开更多
The state of charge(SOC)estimation of lithium-ion battery is an important function in the battery management system(BMS)of electric vehicles.The long short term memory(LSTM)model can be employed for SOC estimation,whi...The state of charge(SOC)estimation of lithium-ion battery is an important function in the battery management system(BMS)of electric vehicles.The long short term memory(LSTM)model can be employed for SOC estimation,which is capable of estimating the future changing states of a nonlinear system.Since the BMS usually works under complicated operating conditions,i.e the real measurement data used for model training may be corrupted by non-Gaussian noise,and thus the performance of the original LSTM with the mean square error(MSE)loss may deteriorate.Therefore,a novel LSTM with mixture kernel mean p-power error(MKMPE)loss,called MKMPE-LSTM,is developed by using the MKMPE loss to replace the MSE as the learning criterion in LSTM framework,which can achieve robust SOC estimation under the measurement data contaminated with non-Gaussian noises(or outliers)because of the MKMPE containing the p-order moments of the error distribution.In addition,a meta-heuristic algorithm,called heap-based-optimizer(HBO),is employed to optimize the hyper-parameters(mainly including learning rate,number of hidden layer neuron and value of p in MKMPE)of the proposed MKMPE-LSTM model to further improve its flexibility and generalization performance,and a novel hybrid model(HBO-MKMPE-LSTM)is established for SOC estimation under non-Gaussian noise cases.Finally,several tests are performed under various cases through a benchmark to evaluate the performance of the proposed HBO-MKMPE-LSTM model,and the results demonstrate that the proposed hybrid method can provide a good robustness and accuracy under different non-Gaussian measurement noises,and the SOC estimation results in terms of mean square error(MSE),root MSE(RMSE),mean absolute relative error(MARE),and determination coefficient R2are less than 0.05%,3%,3%,and above 99.8%at 25℃,respectively.展开更多
As the energy density of battery increases rapidly,lithium-ion batteries(LIBs)are facing serious safety issue with thermal runaway,which largely limits the large-scale applications of high-energy-density LIBs.It is ge...As the energy density of battery increases rapidly,lithium-ion batteries(LIBs)are facing serious safety issue with thermal runaway,which largely limits the large-scale applications of high-energy-density LIBs.It is generally agreed that the chemical crosstalk between the cathode and anode leads to thermal runaway of LIBs.Herein,a multifunctional high safety electrolyte is designed with synergistic construction of cathode electrolyte interphase and capture of reactive free radicals to limit the intrinsic pathway of thermal runaway.The cathode electrolyte interphase not only resists the gas attack from the anode but suppresses the parasitic side reactions induced by electrolyte.And the function of free radical capture has the ability of reducing heat release from thermal runaway of battery.The dual strategy improves the intrinsic safety of battery prominently that the triggering temperature of thermal runaway is increased by 24.4℃and the maximum temperature is reduced by 177.7℃.Simultaneously,the thermal runaway propagation in module can be self-quenched.Moreover,the electrolyte design balances the trade-off of electrochemical and safety performance of high-energy batteries.The capacity retention of LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)|graphite pouch cell has been significantly increased from 53.85%to 97.05%with higher coulombic efficiency of 99.94%at operating voltage extended up to 4.5 V for 200 cycles.Therefore,this work suggests a feasible strategy to mitigate the safety risk of high-energy-density LIBs without sacrificing electrochemical performances.展开更多
Knowing the long-term degradation trajectory of Lithium-ion(Li-ion) battery in its early usage stage is critical for the maintenance of the battery energy storage system(BESS) in reality. Previous battery health diagn...Knowing the long-term degradation trajectory of Lithium-ion(Li-ion) battery in its early usage stage is critical for the maintenance of the battery energy storage system(BESS) in reality. Previous battery health diagnosis methods focus on capacity and state of health(SOH) estimation which can receive only the short-term health status of the cell. This paper proposes a novel degradation trajectory prediction method with synthetic dataset and deep learning, which enables to grasp the characterization of the cell's health at a very early stage of Li-ion battery usage. A transferred convolutional neural network(CNN) is chosen to finalize the early prediction target, and the polynomial function based synthetic dataset generation strategy is designed to reduce the costly data collection procedure in real application. In this thread, the proposed method needs one full lifespan data to predict the overall degradation trajectories of other cells. With only the full lifespan cycling data from 4 cells and 100 cycling data from each cell in experimental validation, the proposed method shows a good prediction accuracy on a dataset with more than 100 commercial Li-ion batteries.展开更多
The electrode material is regarded as one of the key factors that determine the performance of lithium-ion batteries(LIBs).However,it is still a challenge to search for an anode material with large capacity,low diffus...The electrode material is regarded as one of the key factors that determine the performance of lithium-ion batteries(LIBs).However,it is still a challenge to search for an anode material with large capacity,low diffusion barrier,and good stability.In the present work,two new CrP_(2) monolayers(Pmmn-CrP_(2) and Pmma-CrP_(2)) are predicted by means of first principles swarm structure search.Our study shows that both the two CrP_(2) monolayers have high dynamical and thermal stability,as well as excellent electron conductivity.Additionally,Pmmn-CrP_(2) exhibits a remarkably high storage capacity of 705 mA·h·g^(-1) for Li,meanwhile the diffusion energy barrier of Li on the surface of this monolayer is 0.21 eV,ensuring it as a high-performance anode material for LIBs.We hope that our study will inspire researchers to search for new-type two-dimensional(2D) transition metal phosphides for the electrode materials of LIB s.展开更多
Accurate insight into the heat generation rate(HGR) of lithium-ion batteries(LIBs) is one of key issues for battery management systems to formulate thermal safety warning strategies in advance.For this reason,this pap...Accurate insight into the heat generation rate(HGR) of lithium-ion batteries(LIBs) is one of key issues for battery management systems to formulate thermal safety warning strategies in advance.For this reason,this paper proposes a novel physics-informed neural network(PINN) approach for HGR estimation of LIBs under various driving conditions.Specifically,a single particle model with thermodynamics(SPMT) is first constructed for extracting the critical physical knowledge related with battery HGR.Subsequently,the surface concentrations of positive and negative electrodes in battery SPMT model are integrated into the bidirectional long short-term memory(BiLSTM) networks as physical information.And combined with other feature variables,a novel PINN approach to achieve HGR estimation of LIBs with higher accuracy is constituted.Additionally,some critical hyperparameters of BiLSTM used in PINN approach are determined through Bayesian optimization algorithm(BOA) and the results of BOA-based BiLSTM are compared with other traditional BiLSTM/LSTM networks.Eventually,combined with the HGR data generated from the validated virtual battery,it is proved that the proposed approach can well predict the battery HGR under the dynamic stress test(DST) and worldwide light vehicles test procedure(WLTP),the mean absolute error under DST is 0.542 kW/m^(3),and the root mean square error under WLTP is1.428 kW/m^(3)at 25℃.Lastly,the investigation results of this paper also show a new perspective in the application of the PINN approach in battery HGR estimation.展开更多
High-voltage lithium-ion batteries(HVLIBs) are considered as promising devices of energy storage for electric vehicle, hybrid electric vehicle, and other high-power equipment. HVLIBs require their own platform voltage...High-voltage lithium-ion batteries(HVLIBs) are considered as promising devices of energy storage for electric vehicle, hybrid electric vehicle, and other high-power equipment. HVLIBs require their own platform voltages to be higher than 4.5 V on charge. Lithium nickel manganese spinel LiNi_(0.5)Mn_(1.5)O_4(LNMO) cathode is the most promising candidate among the 5 V cathode materials for HVLIBs due to its flat plateau at 4.7 V. However, the degradation of cyclic performance is very serious when LNMO cathode operates over 4.2 V. In this review, we summarize some methods for enhancing the cycling stability of LNMO cathodes in lithium-ion batteries, including doping, cathode surface coating,electrolyte modifying, and other methods. We also discuss the advantages and disadvantages of different methods.展开更多
In this paper, a state of charge(SOC) estimation approach for lithium-ion battery based on equivalent circuit model and the input-to-state stability(ISS) theory has been proposed. According to the electrochemical perf...In this paper, a state of charge(SOC) estimation approach for lithium-ion battery based on equivalent circuit model and the input-to-state stability(ISS) theory has been proposed. According to the electrochemical performance of lithiumion battery, the equivalent circuit model with two RC networks is established, which includes hysteresis characteristic in inner electrochemical response process. The nonlinear relation between open circuit voltage(OCV) and SOC is obtained from a rapid test. Exponential fitting method is used to identify the parameters of the model. A novel state observer based on ISS theory is designed for lithium-ion battery SOC estimation. The designed observer is tested on AMESim and Simulink co-simulation. The simulation results show that the proposed method has a high SOC estimation accuracy with an error of about 2 percent.展开更多
Lithium-ion batteries(LIBs), as the first choice for green batteries, have been widely used in energy storage, electric vehicles, 3C devices, and other related fields, and will have greater application prospects in th...Lithium-ion batteries(LIBs), as the first choice for green batteries, have been widely used in energy storage, electric vehicles, 3C devices, and other related fields, and will have greater application prospects in the future. However, one of the obstacles hindering the future development of battery technology is how to accurately evaluate and monitor battery health, which affects the entire lifespan of battery use. It is not enough to assess battery health comprehensively through the state of health(SoH) alone, especially when nonlinear aging occurs in onboard applications. Here, for the first time, we propose a brand-new health evaluation indicator—state of nonlinear aging(SoNA) to explain the nonlinear aging phenomenon that occurs during the battery use, and also design a knee-point identification method and two SoNA quantitative methods. We apply our health evaluation indicator to build a complete LIB full-lifespan grading evaluation system and a ground-to-cloud service framework, which integrates multi-scenario data collection, multi-dimensional data-based grading evaluation, and cloud management functions. Our works fill the gap in the LIBs’ health evaluation of nonlinear aging, which is of great significance for the health and safety evaluation of LIBs in the field of echelon utilization such as vehicles and energy storage. In addition, this comprehensive evaluation system and service framework are expected to be extended to other battery material systems other than LIBs, yet guiding the design of new energy ecosystem.展开更多
Thermal runaway caused by overcharging results in catastrophic disasters. The influences of charging rate, ambient temperature and aging on thermal runaway caused by overcharging are studied qualitatively and quantita...Thermal runaway caused by overcharging results in catastrophic disasters. The influences of charging rate, ambient temperature and aging on thermal runaway caused by overcharging are studied qualitatively and quantitatively in this manuscript. The results of overcharging tests indicate that high charging rate and ambient temperature increase thermal runaway risk. Aging in 40 ℃ decreases thermal runaway risk. The risk increase of battery with high overcharging rate and in high ambient temperature is due to fast lithium plating reaction and accelerated SEI decomposition, respectively. The risk decrease of aged battery is due to the occurrence of SEI before overcharging tests. SEI suppresses the side reactions between lithium plating and electrolyte. The results of orthogonal tests indicate that the rank of effect is: discharging rate > ambient temperature > aging. The heat generation is calculated based on the results of overcharging tests. The calculation results indicate that heat generated by side reactions contributes more to the total heat generation. Although thermal runaway does not occur during overcharging with low current, the heat dissipation of the lithium-ion battery is the most and deserves focus. The results are important to the design of battery management system and thermal management system to prevent thermal runaway induced by overcharging in total lifespan of battery.展开更多
The technology deployed for lithium-ion battery state of charge(SOC)estimation is an important part of the design of electric vehicle battery management systems.Accurate SOC estimation can forestall excessive charging...The technology deployed for lithium-ion battery state of charge(SOC)estimation is an important part of the design of electric vehicle battery management systems.Accurate SOC estimation can forestall excessive charging and discharging of lithium-ion batteries,thereby improving discharge efficiency and extending cycle life.In this study,the key lithium-ion battery SOC estimation technologies are summarized.First,the research status of lithium-ion battery modeling is introduced.Second,the main technologies and difficulties in model parameter identification for lithium-ion batteries are discussed.Third,the development status and advantages and disadvantages of SOC estimation methods are summarized.Finally,the current research problems and prospects for development trends are summarized.展开更多
Aging diagnosis of batteries is essential to ensure that the energy storage systems operate within a safe region.This paper proposes a novel cell to pack health and lifetime prognostics method based on the combination...Aging diagnosis of batteries is essential to ensure that the energy storage systems operate within a safe region.This paper proposes a novel cell to pack health and lifetime prognostics method based on the combination of transferred deep learning and Gaussian process regression.General health indicators are extracted from the partial discharge process.The sequential degradation model of the health indicator is developed based on a deep learning framework and is migrated for the battery pack degradation prediction.The future degraded capacities of both battery pack and each battery cell are probabilistically predicted to provide a comprehensive lifetime prognostic.Besides,only a few separate battery cells in the source domain and early data of battery packs in the target domain are needed for model construction.Experimental results show that the lifetime prediction errors are less than 25 cycles for the battery pack,even with only 50 cycles for model fine-tuning,which can save about 90%time for the aging experiment.Thus,it largely reduces the time and labor for battery pack investigation.The predicted capacity trends of the battery cells connected in the battery pack accurately reflect the actual degradation of each battery cell,which can reveal the weakest cell for maintenance in advance.展开更多
As a promising alternative anode material,silicon(Si)presents a larger capacity than the commercial anode to achieve large capacity lithium-ion batteries.However,the application of pure Si as anode is hampered by limi...As a promising alternative anode material,silicon(Si)presents a larger capacity than the commercial anode to achieve large capacity lithium-ion batteries.However,the application of pure Si as anode is hampered by limitations such as volume expansion,low conductivity and unstable solid electrolyte interphase.To break through these limitations,the core-shell Si@Li4Ti5O12nanocomposite,which was prepared via in-situ self-assembly reaction and decompressive boiling fast concentration method,was proposed in this work.This anode combines the advantages of nano-sized Si particle and pure Li4Ti5O12(LTO)coating layer,improving the performance of the lithium-ion batteries.The Si@Li4Ti5O12 anode displays a high initial discharge/charge specific capacity of 1756/1383 m Ahg^-1 at 500 mAg^-1(representing high initial coulombic efficiency of 78.8%),a large rate capability(specific capacity of 620 mAhg^-1 at4000 mAg^-1),an outstanding cycling stability(reversible specific capacity of 883 mAhg^-1 after 150 cycles)and a low volume expansion rate(only 3.3% after 150 cycles).Moreover,the synthesis process shows the merits of efficiency,simplicity,and economy,providing a reliable method to fabricate large capacity Si@Li4Ti5O12nanocomposite anode materials for practical lithium-ion batteries.展开更多
Conventional charging methods for lithium-ion battery(LIB)are challenged with vital problems at low temperatures:risk of lithium(Li)plating and low charging speed.This study proposes a fast-charging strategy without L...Conventional charging methods for lithium-ion battery(LIB)are challenged with vital problems at low temperatures:risk of lithium(Li)plating and low charging speed.This study proposes a fast-charging strategy without Li plating to achieve high-rate charging at low temperatures with bidirectional chargers.The strategy combines the pulsed-heating method and the optimal charging method via precise control of the battery states.A thermo-electric coupled model is developed based on the pseudo-twodimensional(P2D)electrochemical model to derive charging performances.Two current maps of pulsed heating and charging are generated to realize real-time control.Therefore,our proposed strategy achieves a 3 C equivalent rate at 0℃ and 1.5 C at-10℃ without Li plating,which is 10–30 times faster than the traditional methods.The entropy method is employed to balance the charging speed and the energy efficiency,and the charging performance is further enhanced.For practical application,the power limitation of the charger is considered,and a 2.4 C equivalent rate is achieved at 0℃ with a 250 kW maximum power output.This novel strategy significantly expands LIB usage boundary,and increases charging speed and battery safety.展开更多
Silicon(Si)is widely considered to be the most attractive candidate anode material for use in next-generation high-energy-density lithium(Li)-ion batteries(LIBs)because it has a high theoretical gravimetric Li storage...Silicon(Si)is widely considered to be the most attractive candidate anode material for use in next-generation high-energy-density lithium(Li)-ion batteries(LIBs)because it has a high theoretical gravimetric Li storage capacity,relatively low lithiation voltage,and abundant resources.Consequently,massive efforts have been exerted to improve its electrochemical performance.While some progress in this field has been achieved,a number of severe challenges,such as the element’s large volume change during cycling,low intrinsic electronic conductivity,and poor rate capacity,have yet to be solved.Methods to solve these problems have been attempted via the development of nanosized Si materials.Unfortunately,reviews summarizing the work on Si-based alloys are scarce.Herein,the recent progress related to Si-based alloy anode materials is reviewed.The problems associated with Si anodes and the corresponding strategies used to address these problems are first described.Then,the available Si-based alloys are divided into Si/Li-active and inactive systems,and the characteristics of these systems are discussed.Other special systems are also introduced.Finally,perspectives and future outlooks are provided to enable the wider application of Si-alloy anodes to commercial LIBs.展开更多
This mini-review highlights selectively the recent research progress in the composites of Li Fe PO4 and graphene. In particularly, the different fabrication protocols, and the electrochemical performance of the compos...This mini-review highlights selectively the recent research progress in the composites of Li Fe PO4 and graphene. In particularly, the different fabrication protocols, and the electrochemical performance of the composites are summarized in detail. The structural and morphology characters of graphene sheets that may affect the property of the composites are discussed briefly. The possible ongoing researches in area are speculated upon.展开更多
Prelithiation technology is widely considered a feasible route to raise the energy density and elongate the cycle life of lithium-ion batteries.The principle of prelithiation is to introduce extra active Li ions in th...Prelithiation technology is widely considered a feasible route to raise the energy density and elongate the cycle life of lithium-ion batteries.The principle of prelithiation is to introduce extra active Li ions in the battery so that the lithium loss during the first charge and long-term cycling can be compensated.Such an effect does not need to change the major electrode material or battery structure and is compatible with the majority of current lithium-ion battery production lines.At this stage,various prelithiation methods have been reported,some of which are already in the pilot-scale production stage.But there is still no definitive development roadmap for prelithiation.In this review,we first introduce the influence of prelithiation on electrochemical performance from a theoretical point of view and then compare the pros and cons of different prelithiation methods in different battery manufacturing stages.Finally,we discuss the challenges and future development trends of prelithiation.We aim to build up a bridge between academic research and industrial application.Some engineering problems in the promotion of prelithiation technique are extensively discussed,including not only the implementation of prelithiation but also some collateral issues on battery designing and management.展开更多
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supported by the National Natural Science Foundation of China(No.U20A20310 and No.52176199)sponsored by the Program of Shanghai Academic/Technology Research Leader(No.22XD1423800)。
文摘Thermal runaway(TR)is a critical issue hindering the large-scale application of lithium-ion batteries(LIBs).Understanding the thermal safety behavior of LIBs at the cell and module level under different state of charges(SOCs)has significant implications for reinforcing the thermal safety design of the lithium-ion battery module.This study first investigates the thermal safety boundary(TSB)correspondence at the cells and modules level under the guidance of a newly proposed concept,safe electric quantity boundary(SEQB).A reasonable thermal runaway propagation(TRP)judgment indicator,peak heat transfer power(PHTP),is proposed to predict whether TRP occurs.Moreover,a validated 3D model is used to quantitatively clarify the TSB at different SOCs from the perspective of PHTP,TR trigger temperature,SOC,and the full cycle life.Besides,three different TRP transfer modes are discovered.The interconversion relationship of three different TRP modes is investigated from the perspective of PHTP.This paper explores the TSB of LIBs under different SOCs at both cell and module levels for the first time,which has great significance in guiding the thermal safety design of battery systems.
基金financially supported by the National Natural Science Foundation of China(No.51804084)the Natural Science Foundation of Guangxi Province,China(No.2021GXNSFAA220096)the Science and Technology Major Project of Guangxi Province,China(No.AA17204100)。
文摘To effectively separate and recover Co(Ⅱ) from the leachate of spent lithium-ion battery cathodes,we investigated solvent extraction with quaternary ammonium salt N263 in the sodium nitrite system.NO_(2)^(-)combines with Co(Ⅱ) to form an anion [Co(NO_(2))_(3)]^(-),and it is then extracted by N263.The extraction of Co(Ⅱ) is related to the concentration of NO_(2)^(-).The extraction efficiency of Co(Ⅱ) reaches the maximum of99.16%,while the extraction efficiencies of Ni(Ⅱ),Mn(Ⅱ),and Li(Ⅰ) are 9.27%-9.80% under the following conditions:30vol% of N263 and15vol% of iso-propyl alcohol in sulfonated kerosene,the volume ratio of the aqueous-to-organic phase is 2:1,the extraction time is 30 min,and1 M sodium nitrite in 0.1 MHNO_(3).The theoretical stages require for the Co(Ⅱ) extraction are performed in the McCabe–Thiele diagram,and the extraction efficiency of Co(Ⅱ) reaches more than 99.00% after three-stage counter-current extraction with Co(Ⅱ) concentration of 2544mg/L.When the HCl concentration is 1.5 M,the volume ratio of the aqueous-to-organic phase is 1:1,the back-extraction efficiency of Co(Ⅱ)achieves 91.41%.After five extraction and back-extraction cycles,the Co(Ⅱ) extraction efficiency can still reach 93.89%.The Co(Ⅱ) extraction efficiency in the actual leaching solution reaches 100%.
基金This work was supported by Guangdong Basic and Applied Basic Research Foundation(2019A1515110530,2022A1515010486)Shenzhen Science and Technology Program(JCYJ20210324140804013)Tsinghua Shenzhen International Graduate School(QD2021005N,JC2021007).
文摘Green energy storage devices play vital roles in reducing fossil fuel emissions and achieving carbon neutrality by 2050.Growing markets for portable electronics and electric vehicles create tremendous demand for advanced lithium-ion batteries(LIBs)with high power and energy density,and novel electrode material with high capacity and energy density is one of the keys to next-generation LIBs.Silicon-based materials,with high specific capacity,abundant natural resources,high-level safety and environmental friendliness,are quite promising alternative anode materials.However,significant volume expansion and redundant side reactions with electrolytes lead to active lithium loss and decreased coulombic efficiency(CE)of silicon-based material,which hinders the commercial application of silicon-based anode.Prelithiation,preembedding extra lithium ions in the electrodes,is a promising approach to replenish the lithium loss during cycling.Recent progress on prelithiation strategies for silicon-based anode,including electrochemical method,chemical method,direct contact method,and active material method,and their practical potentials are reviewed and prospected here.The development of advanced Si-based material and prelithiation technologies is expected to provide promising approaches for the large-scale application of silicon-based materials.
基金supported by the National Key R.D Program of China(2021YFB2401904)the Joint Fund project of the National Natural Science Foundation of China(U21A20485)+1 种基金the National Natural Science Foundation of China(61976175)the Key Laboratory Project of Shaanxi Provincial Education Department Scientific Research Projects(20JS109)。
文摘The state of charge(SOC)estimation of lithium-ion battery is an important function in the battery management system(BMS)of electric vehicles.The long short term memory(LSTM)model can be employed for SOC estimation,which is capable of estimating the future changing states of a nonlinear system.Since the BMS usually works under complicated operating conditions,i.e the real measurement data used for model training may be corrupted by non-Gaussian noise,and thus the performance of the original LSTM with the mean square error(MSE)loss may deteriorate.Therefore,a novel LSTM with mixture kernel mean p-power error(MKMPE)loss,called MKMPE-LSTM,is developed by using the MKMPE loss to replace the MSE as the learning criterion in LSTM framework,which can achieve robust SOC estimation under the measurement data contaminated with non-Gaussian noises(or outliers)because of the MKMPE containing the p-order moments of the error distribution.In addition,a meta-heuristic algorithm,called heap-based-optimizer(HBO),is employed to optimize the hyper-parameters(mainly including learning rate,number of hidden layer neuron and value of p in MKMPE)of the proposed MKMPE-LSTM model to further improve its flexibility and generalization performance,and a novel hybrid model(HBO-MKMPE-LSTM)is established for SOC estimation under non-Gaussian noise cases.Finally,several tests are performed under various cases through a benchmark to evaluate the performance of the proposed HBO-MKMPE-LSTM model,and the results demonstrate that the proposed hybrid method can provide a good robustness and accuracy under different non-Gaussian measurement noises,and the SOC estimation results in terms of mean square error(MSE),root MSE(RMSE),mean absolute relative error(MARE),and determination coefficient R2are less than 0.05%,3%,3%,and above 99.8%at 25℃,respectively.
基金supported by the National Key R&D ProgramStrategic Scientific and Technological Innovation Cooperation(2022YFB3803500)the National Key Research and Development Program of China(2019YFA0705700)+1 种基金the National Natural Science Foundation of China(52076121,51904016,and 52004138)the Fundamental Research Funds for the Central Universities。
文摘As the energy density of battery increases rapidly,lithium-ion batteries(LIBs)are facing serious safety issue with thermal runaway,which largely limits the large-scale applications of high-energy-density LIBs.It is generally agreed that the chemical crosstalk between the cathode and anode leads to thermal runaway of LIBs.Herein,a multifunctional high safety electrolyte is designed with synergistic construction of cathode electrolyte interphase and capture of reactive free radicals to limit the intrinsic pathway of thermal runaway.The cathode electrolyte interphase not only resists the gas attack from the anode but suppresses the parasitic side reactions induced by electrolyte.And the function of free radical capture has the ability of reducing heat release from thermal runaway of battery.The dual strategy improves the intrinsic safety of battery prominently that the triggering temperature of thermal runaway is increased by 24.4℃and the maximum temperature is reduced by 177.7℃.Simultaneously,the thermal runaway propagation in module can be self-quenched.Moreover,the electrolyte design balances the trade-off of electrochemical and safety performance of high-energy batteries.The capacity retention of LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)|graphite pouch cell has been significantly increased from 53.85%to 97.05%with higher coulombic efficiency of 99.94%at operating voltage extended up to 4.5 V for 200 cycles.Therefore,this work suggests a feasible strategy to mitigate the safety risk of high-energy-density LIBs without sacrificing electrochemical performances.
基金supported in part by the National Natural Science Foundation of China (52107229, 62203423, and 61903114)in part by the Fujian Provincial Natural Science Foundation (2022J01504)。
文摘Knowing the long-term degradation trajectory of Lithium-ion(Li-ion) battery in its early usage stage is critical for the maintenance of the battery energy storage system(BESS) in reality. Previous battery health diagnosis methods focus on capacity and state of health(SOH) estimation which can receive only the short-term health status of the cell. This paper proposes a novel degradation trajectory prediction method with synthetic dataset and deep learning, which enables to grasp the characterization of the cell's health at a very early stage of Li-ion battery usage. A transferred convolutional neural network(CNN) is chosen to finalize the early prediction target, and the polynomial function based synthetic dataset generation strategy is designed to reduce the costly data collection procedure in real application. In this thread, the proposed method needs one full lifespan data to predict the overall degradation trajectories of other cells. With only the full lifespan cycling data from 4 cells and 100 cycling data from each cell in experimental validation, the proposed method shows a good prediction accuracy on a dataset with more than 100 commercial Li-ion batteries.
基金Project supported by the National Natural Science Foundation of China(Grant No.11964006)the Science and Technology Foundation of Kaili University(Grant No.2022ZD06)the Specialized Research Fund for the Doctoral Program of Kaili University(Grant Nos.BS201601 and BS201702)。
文摘The electrode material is regarded as one of the key factors that determine the performance of lithium-ion batteries(LIBs).However,it is still a challenge to search for an anode material with large capacity,low diffusion barrier,and good stability.In the present work,two new CrP_(2) monolayers(Pmmn-CrP_(2) and Pmma-CrP_(2)) are predicted by means of first principles swarm structure search.Our study shows that both the two CrP_(2) monolayers have high dynamical and thermal stability,as well as excellent electron conductivity.Additionally,Pmmn-CrP_(2) exhibits a remarkably high storage capacity of 705 mA·h·g^(-1) for Li,meanwhile the diffusion energy barrier of Li on the surface of this monolayer is 0.21 eV,ensuring it as a high-performance anode material for LIBs.We hope that our study will inspire researchers to search for new-type two-dimensional(2D) transition metal phosphides for the electrode materials of LIB s.
基金funded by the Artificial Intelligence Technology Project of Xi’an Science and Technology Bureau in China(No.21RGZN0014)。
文摘Accurate insight into the heat generation rate(HGR) of lithium-ion batteries(LIBs) is one of key issues for battery management systems to formulate thermal safety warning strategies in advance.For this reason,this paper proposes a novel physics-informed neural network(PINN) approach for HGR estimation of LIBs under various driving conditions.Specifically,a single particle model with thermodynamics(SPMT) is first constructed for extracting the critical physical knowledge related with battery HGR.Subsequently,the surface concentrations of positive and negative electrodes in battery SPMT model are integrated into the bidirectional long short-term memory(BiLSTM) networks as physical information.And combined with other feature variables,a novel PINN approach to achieve HGR estimation of LIBs with higher accuracy is constituted.Additionally,some critical hyperparameters of BiLSTM used in PINN approach are determined through Bayesian optimization algorithm(BOA) and the results of BOA-based BiLSTM are compared with other traditional BiLSTM/LSTM networks.Eventually,combined with the HGR data generated from the validated virtual battery,it is proved that the proposed approach can well predict the battery HGR under the dynamic stress test(DST) and worldwide light vehicles test procedure(WLTP),the mean absolute error under DST is 0.542 kW/m^(3),and the root mean square error under WLTP is1.428 kW/m^(3)at 25℃.Lastly,the investigation results of this paper also show a new perspective in the application of the PINN approach in battery HGR estimation.
基金supported by the foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions and Science and Technology Foundation(ykj-2016-00161)partly supported by International Research Promotion Program(IRPR)of Osaka University
文摘High-voltage lithium-ion batteries(HVLIBs) are considered as promising devices of energy storage for electric vehicle, hybrid electric vehicle, and other high-power equipment. HVLIBs require their own platform voltages to be higher than 4.5 V on charge. Lithium nickel manganese spinel LiNi_(0.5)Mn_(1.5)O_4(LNMO) cathode is the most promising candidate among the 5 V cathode materials for HVLIBs due to its flat plateau at 4.7 V. However, the degradation of cyclic performance is very serious when LNMO cathode operates over 4.2 V. In this review, we summarize some methods for enhancing the cycling stability of LNMO cathodes in lithium-ion batteries, including doping, cathode surface coating,electrolyte modifying, and other methods. We also discuss the advantages and disadvantages of different methods.
基金supported by the High Technology Research and Development Program of Jilin(20130204021GX)the Specialized Research Fund for Graduate Course Identification System Program(Jilin University)of China(450060523183)+2 种基金the National Natural Science Foundation of China(61520106008,U1564207,61503149)the Education Department of Jilin Province of China(2016430)the Graduate Innovation Fund of Jilin University(2016030)
文摘In this paper, a state of charge(SOC) estimation approach for lithium-ion battery based on equivalent circuit model and the input-to-state stability(ISS) theory has been proposed. According to the electrochemical performance of lithiumion battery, the equivalent circuit model with two RC networks is established, which includes hysteresis characteristic in inner electrochemical response process. The nonlinear relation between open circuit voltage(OCV) and SOC is obtained from a rapid test. Exponential fitting method is used to identify the parameters of the model. A novel state observer based on ISS theory is designed for lithium-ion battery SOC estimation. The designed observer is tested on AMESim and Simulink co-simulation. The simulation results show that the proposed method has a high SOC estimation accuracy with an error of about 2 percent.
基金financially supported by the National Natural Science Foundation of China(NSFC,U20A20310,52107230,52176199,52102470)the support of the research project Model2Life(03XP0334),funded by the German Federal Ministry of Education and Research(BMBF)。
文摘Lithium-ion batteries(LIBs), as the first choice for green batteries, have been widely used in energy storage, electric vehicles, 3C devices, and other related fields, and will have greater application prospects in the future. However, one of the obstacles hindering the future development of battery technology is how to accurately evaluate and monitor battery health, which affects the entire lifespan of battery use. It is not enough to assess battery health comprehensively through the state of health(SoH) alone, especially when nonlinear aging occurs in onboard applications. Here, for the first time, we propose a brand-new health evaluation indicator—state of nonlinear aging(SoNA) to explain the nonlinear aging phenomenon that occurs during the battery use, and also design a knee-point identification method and two SoNA quantitative methods. We apply our health evaluation indicator to build a complete LIB full-lifespan grading evaluation system and a ground-to-cloud service framework, which integrates multi-scenario data collection, multi-dimensional data-based grading evaluation, and cloud management functions. Our works fill the gap in the LIBs’ health evaluation of nonlinear aging, which is of great significance for the health and safety evaluation of LIBs in the field of echelon utilization such as vehicles and energy storage. In addition, this comprehensive evaluation system and service framework are expected to be extended to other battery material systems other than LIBs, yet guiding the design of new energy ecosystem.
基金the support given by National Natural Science Foundation of China(51874184)the Key Natural Science Foundation in Jiangsu Province(18KJA620003)Jiangsu Project Plan for Outstanding Talents Team in Six Research Fields(TD-XNYQC-002)。
文摘Thermal runaway caused by overcharging results in catastrophic disasters. The influences of charging rate, ambient temperature and aging on thermal runaway caused by overcharging are studied qualitatively and quantitatively in this manuscript. The results of overcharging tests indicate that high charging rate and ambient temperature increase thermal runaway risk. Aging in 40 ℃ decreases thermal runaway risk. The risk increase of battery with high overcharging rate and in high ambient temperature is due to fast lithium plating reaction and accelerated SEI decomposition, respectively. The risk decrease of aged battery is due to the occurrence of SEI before overcharging tests. SEI suppresses the side reactions between lithium plating and electrolyte. The results of orthogonal tests indicate that the rank of effect is: discharging rate > ambient temperature > aging. The heat generation is calculated based on the results of overcharging tests. The calculation results indicate that heat generated by side reactions contributes more to the total heat generation. Although thermal runaway does not occur during overcharging with low current, the heat dissipation of the lithium-ion battery is the most and deserves focus. The results are important to the design of battery management system and thermal management system to prevent thermal runaway induced by overcharging in total lifespan of battery.
基金supported by research on value model and technology application of patent operation of science and technology project(52094020000U)National Natural Science Foundation of China(52177193).
文摘The technology deployed for lithium-ion battery state of charge(SOC)estimation is an important part of the design of electric vehicle battery management systems.Accurate SOC estimation can forestall excessive charging and discharging of lithium-ion batteries,thereby improving discharge efficiency and extending cycle life.In this study,the key lithium-ion battery SOC estimation technologies are summarized.First,the research status of lithium-ion battery modeling is introduced.Second,the main technologies and difficulties in model parameter identification for lithium-ion batteries are discussed.Third,the development status and advantages and disadvantages of SOC estimation methods are summarized.Finally,the current research problems and prospects for development trends are summarized.
基金Supported by National Natural Science Foundation of China(Grant Nos.51875054,U1864212)Graduate Research and Innovation Foundation of Chongqing+2 种基金China(Grant No.CYS20018)Chongqing Municipal Natural Science Foundation for Distinguished Young Scholars of China(Grant No.cstc2019jcyjjq X0016)Chongqing Science and Technology Bureau of China。
文摘Aging diagnosis of batteries is essential to ensure that the energy storage systems operate within a safe region.This paper proposes a novel cell to pack health and lifetime prognostics method based on the combination of transferred deep learning and Gaussian process regression.General health indicators are extracted from the partial discharge process.The sequential degradation model of the health indicator is developed based on a deep learning framework and is migrated for the battery pack degradation prediction.The future degraded capacities of both battery pack and each battery cell are probabilistically predicted to provide a comprehensive lifetime prognostic.Besides,only a few separate battery cells in the source domain and early data of battery packs in the target domain are needed for model construction.Experimental results show that the lifetime prediction errors are less than 25 cycles for the battery pack,even with only 50 cycles for model fine-tuning,which can save about 90%time for the aging experiment.Thus,it largely reduces the time and labor for battery pack investigation.The predicted capacity trends of the battery cells connected in the battery pack accurately reflect the actual degradation of each battery cell,which can reveal the weakest cell for maintenance in advance.
基金the financial support from the National Natural Science Foundation of China (51876052, 51676128)
文摘As a promising alternative anode material,silicon(Si)presents a larger capacity than the commercial anode to achieve large capacity lithium-ion batteries.However,the application of pure Si as anode is hampered by limitations such as volume expansion,low conductivity and unstable solid electrolyte interphase.To break through these limitations,the core-shell Si@Li4Ti5O12nanocomposite,which was prepared via in-situ self-assembly reaction and decompressive boiling fast concentration method,was proposed in this work.This anode combines the advantages of nano-sized Si particle and pure Li4Ti5O12(LTO)coating layer,improving the performance of the lithium-ion batteries.The Si@Li4Ti5O12 anode displays a high initial discharge/charge specific capacity of 1756/1383 m Ahg^-1 at 500 mAg^-1(representing high initial coulombic efficiency of 78.8%),a large rate capability(specific capacity of 620 mAhg^-1 at4000 mAg^-1),an outstanding cycling stability(reversible specific capacity of 883 mAhg^-1 after 150 cycles)and a low volume expansion rate(only 3.3% after 150 cycles).Moreover,the synthesis process shows the merits of efficiency,simplicity,and economy,providing a reliable method to fabricate large capacity Si@Li4Ti5O12nanocomposite anode materials for practical lithium-ion batteries.
基金supported by the National Natural Science Foundation of China(52177217 and 52037006)the Beijing Natural Science Foundation(3212031)。
文摘Conventional charging methods for lithium-ion battery(LIB)are challenged with vital problems at low temperatures:risk of lithium(Li)plating and low charging speed.This study proposes a fast-charging strategy without Li plating to achieve high-rate charging at low temperatures with bidirectional chargers.The strategy combines the pulsed-heating method and the optimal charging method via precise control of the battery states.A thermo-electric coupled model is developed based on the pseudo-twodimensional(P2D)electrochemical model to derive charging performances.Two current maps of pulsed heating and charging are generated to realize real-time control.Therefore,our proposed strategy achieves a 3 C equivalent rate at 0℃ and 1.5 C at-10℃ without Li plating,which is 10–30 times faster than the traditional methods.The entropy method is employed to balance the charging speed and the energy efficiency,and the charging performance is further enhanced.For practical application,the power limitation of the charger is considered,and a 2.4 C equivalent rate is achieved at 0℃ with a 250 kW maximum power output.This novel strategy significantly expands LIB usage boundary,and increases charging speed and battery safety.
基金financially supported by the National Natural Science Foundation of China(No.52074360)the Natural Science Foundation for Distinguished Young Scholars of Hunan Province(No.2020JJ2047)+1 种基金the Program of Huxiang Young Talents(No.2019RS2002)the Innovation-Driven Project of Central South University(No.2020CX027).
文摘Silicon(Si)is widely considered to be the most attractive candidate anode material for use in next-generation high-energy-density lithium(Li)-ion batteries(LIBs)because it has a high theoretical gravimetric Li storage capacity,relatively low lithiation voltage,and abundant resources.Consequently,massive efforts have been exerted to improve its electrochemical performance.While some progress in this field has been achieved,a number of severe challenges,such as the element’s large volume change during cycling,low intrinsic electronic conductivity,and poor rate capacity,have yet to be solved.Methods to solve these problems have been attempted via the development of nanosized Si materials.Unfortunately,reviews summarizing the work on Si-based alloys are scarce.Herein,the recent progress related to Si-based alloy anode materials is reviewed.The problems associated with Si anodes and the corresponding strategies used to address these problems are first described.Then,the available Si-based alloys are divided into Si/Li-active and inactive systems,and the characteristics of these systems are discussed.Other special systems are also introduced.Finally,perspectives and future outlooks are provided to enable the wider application of Si-alloy anodes to commercial LIBs.
基金the Science and Technology Commission of Shanghai Municipality (No. 12nm0503500)the National Science Foundation of China (Nos. 21376148, 11374205)
文摘This mini-review highlights selectively the recent research progress in the composites of Li Fe PO4 and graphene. In particularly, the different fabrication protocols, and the electrochemical performance of the composites are summarized in detail. The structural and morphology characters of graphene sheets that may affect the property of the composites are discussed briefly. The possible ongoing researches in area are speculated upon.
基金National Natural Science Foundation of China,Grant/Award Numbers:22179045,5202780089。
文摘Prelithiation technology is widely considered a feasible route to raise the energy density and elongate the cycle life of lithium-ion batteries.The principle of prelithiation is to introduce extra active Li ions in the battery so that the lithium loss during the first charge and long-term cycling can be compensated.Such an effect does not need to change the major electrode material or battery structure and is compatible with the majority of current lithium-ion battery production lines.At this stage,various prelithiation methods have been reported,some of which are already in the pilot-scale production stage.But there is still no definitive development roadmap for prelithiation.In this review,we first introduce the influence of prelithiation on electrochemical performance from a theoretical point of view and then compare the pros and cons of different prelithiation methods in different battery manufacturing stages.Finally,we discuss the challenges and future development trends of prelithiation.We aim to build up a bridge between academic research and industrial application.Some engineering problems in the promotion of prelithiation technique are extensively discussed,including not only the implementation of prelithiation but also some collateral issues on battery designing and management.
