Thin polymer electrolyte with MXene functional layer for uniform Li^(+) deposition in all-solid-state lithium battery

Solid polymer electrolyte(SPE) shows great potential for all-solid-state batteries because of the inherent safety and flexibility;however, the unfavourable Li+deposition and large thickness hamper its development and application. Herein, a laminar MXene functional layer-thin SPE layer-cathode integration(MXene-PEO-LFP) is designed and fabricated. The MXene functional layer formed by stacking rigid MXene nanosheets imparts higher compressive strength relative to PEO electrolyte layer. And the abundant negatively-charged groups on MXene functional layer effectively repel anions and attract cations to adjust the charge distribution behavior at electrolyte–anode interface. Furthermore,the functional layer with rich lithiophilic groups and outstanding electronic conductivity results in low Li nucleation overpotential and nucleation energy barrier. In consequence, the cell assembled with MXene-PEO-LFP, where the PEO electrolyte layer is only 12 μm, much thinner than most solid electrolytes, exhibits uniform, dendrite-free Li+deposition and excellent cycling stability. High capacity(142.8 mAh g-1), stable operation of 140 cycles(capacity decay per cycle, 0.065%), and low polarization potential(0.5 C) are obtained in this Li|MXene-PEO-LFP cell,which is superior to most PEO-based electrolytes under identical condition. This integrated design may provide a strategy for the large-scale application of thin polymer electrolytes in all-solid-state battery.

Thermal safety boundary of lithium-ion battery at different state of charge

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.

In Situ Polymer Gel Electrolyte in Boosting Scalable Fibre Lithium Battery Applications

The poor interfacial stability not only deteriorates fibre lithium-ion batteries(FLBs)performance but also impacts their scalable applications.To efficiently address these challenges,Prof.Huisheng Peng team proposed a generalized channel structures strategy with optimized in situ polymerization technology in their recent study.The resultant FLBs can be woven into different-sized powering textiles,providing a high energy density output of 128 Wh kg^(-1) and simultaneously demonstrating good durability even under harsh conditions.Such a promising strategy expands the horizon in developing FLB with particular polymer gel electrolytes,and significantly ever-deepening understanding of the scaled wearable energy textile system toward a sustainable future.

Review on current development of polybenzimidazole membrane for lithium battery

With the rapid development of portable technology,lithium batteries have emerged as potential candidates for high-performance energy storage systems owing to their high energy density and cycling stability.Among the key components of a lithium battery system,the separator plays a critical role as it directly influences the battery performance benchmark(cycling performance and safety).However,traditional polyolefin separators(polypropylene/polyethylene)are unable to meet the demands of highperformance and safer battery systems due to their poor electrolyte compatibility,thermal runaways,and ultimate growth of dendrites.In contrast,membranes fabricated using polybenzimidazole(PBI)exhibit excellent electrolyte wettability and outstanding thermal dimensional stability,thus holding great potential as separators for high-performance and high-safety batteries.In this paper,we present a comprehensive review of the general requirements for separators,synthesis technology for separators,and research trends focusing PBI membranes in lithium batteries to alleviate the current commercial challenges faced by conventional polyolefin separators.In addition,we discuss the future development direction for PBI battery separators by considering various factors such as production cost,ecological footprint,preparation technology,and battery component compatibility.By exploring these perspectives,we aim to promote the continued application and exploration of PBI-based materials to advance lithium battery technology.

Lithium Salt Combining Fluoroethylene Carbonate Initiates Methyl Methacrylate Polymerization Enabling Dendrite-Free Solid-State Lithium Metal Battery

This work demonstrates a novel polymerization-derived polymer electrolyte consisting of methyl methacrylate,lithium bis(trifluoromethanesulfonyl)imide and fluoroethylene carbonate.The polymerization of MMA was initiated by the amino compounds following an anionic catalytic mechanism.LiTFSI plays both roles including the initiator and Li ion source in the polymer electrolyte.Normally,lithium bis(trifluoromethanesulfonyl)imide has difficulty in initiating the polymerization reaction of methyl methacrylate monomer,a very high concentration of lithium bis(trifluoromethanesulfonyl)imide is needed for initiating the polymerization.However,the fluoroethylene carbonate additive can work as a supporter to facilitate the degree of dissociation of lithium bis(trifluoromethanesulfonyl)imide and increase its initiator capacity due to the high dielectric constant.The as-prepared poly-methyl methacrylate-based polymer electrolyte has a high ionic conductivity(1.19×10^(−3)S cm^(−1)),a wide electrochemical stability window(5 V vs Li^(+)/Li),and a high Li ion transference number(t_(Li^(+)))of 0.74 at room temperature(RT).Moreover,this polymerization-derived polymer electrolyte can effectively work as an artificial protective layer on Li metal anode,which enabled the Li symmetric cell to achieve a long-term cycling performance at 0.2 mAh cm^(−2)for 2800 h.The LiFePO_(4)battery with polymerization-derived polymer electrolyte-modified Li metal anode shows a capacity retention of 91.17%after 800 cycles at 0.5 C.This work provides a facile and accessible approach to manufacturing poly-methyl methacrylate-based polymerization-derived polymer electrolyte and shows great potential as an interphase in Li metal batteries.

Viability of all-solid-state lithium metal battery coupled with oxide solid-state electrolyte and high-capacity cathode

Owing to the utilization of lithium metal as anode with the ultrahigh theoretical capacity density of 3860 mA h g^(-1)and oxide-based ceramic solid-state electrolytes(SE),e.g.,garnet-type Li7La_(3)Zr_(2)O_(12)(LLZO),all-state-state lithium metal batteries(ASLMBs)have been widely accepted as the promising alternatives for providing the satisfactory energy density and safety.However,its applications are still challenged by plenty of technical and scientific issues.In this contribution,the co-sintering temperature at 500℃is proved as a compromise method to fabricate the composite cathode with structural integrity and declined capacity fading of LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2)(NCM).On the other hand,it tends to form weaker grain boundary(GB)inside polycrystalline LLZO at inadequate sintering temperature for LLZO,which can induce the intergranular failure of SE during the growth of Li filament inside the unavoidable defect on the interface of SE.Therefore,increasing the strength of GB,refining the grain to 0.4μm,and precluding the interfacial defect are suggested to postpone the electro-chemo-mechanical failure of SE with weak GB.Moreover,the advanced sintering techniques to lower the co-sintering temperature for both NCM-LLZO composite cathode and LLZO SE can be posted out to realize the viability of state-of-the-art ASLMBs with higher energy density as well as the guaranteed safety.

Tuning the solubility of polysulfides for constructing practical lithium-sulfur battery

Li-S batteries are regarded as one of the most promising candidates for next-generation battery systems with high energy density and low cost.However,the dissolution-precipitation reaction mechanism of the sulfur(S)cathode enhances the kinetics of the redox processes of the insulating sulfu r,which also arouses the notorious shuttle effect,leading to serious loss of S species and corrosion of Li anode.To get a balance between the shuttle restraining and the kinetic property,a combined strategy of electrolyte regulation and cathode modification is proposed via introducing 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoroprpyl ether(HFE)instead of 1,2-dimethoxyethane(DME),and SeS_(7)instead of S_8.The introduction of HFE tunes the solvation structure of the LiTFSI and the dissolution of intermediate polysulfides with Se doping(LiPSSes),and optimize the interface stability of the Li anode simultaneously.The minor Se substitution compensates the decrease in kinetic due to the decreased solubility of LiPSs.In this way,the Li-SeS_(7)batteries deliver a reversible capacity of 1062 and 1037 mAh g^(-1)with 2.0 and 5.5 mg SeS_(7)cm^(-2)loading condition,respectively.Besides,an electrolyte-electrode loading model is established to explain the relationship between the optimal electrolyte and cathode loading.It makes more sense to guide the electrolyte design for practical Li-S batteries.

Lithium-Metal Free Sulfur Battery Based on Waste Biomass Anode and Nano-Sized Li_(2)S Cathode

The realization of a stable lithium-metal free(LiMF)sulfur battery based on amorphous carbon anode and lithium sulfide(Li_(2)S)cathode is here reported.In particular,a biomass waste originating full-cell combining a carbonized brewer's spent grain(CBSG)biochar anode with a Li_(2)S-graphene composite cathode(Li_(2)S70Gr30)is proposed.This design is particularly attractive for applying a cost-effective,high performance,environment friendly,and safe anode material,as an alternative to standard graphite and metallic lithium in emerging battery technologies.The anodic and cathodic materials are characterized in terms of structure,morphology and composition through X-ray diffraction,scanning and transmission electron microscopy,X-ray photoelectron and Raman spectroscopies.Furthermore,an electrochemical characterization comprising galvanostatic cycling,rate capability and cyclic voltammetry tests were carried out both in half-cell and full-cell configurations.The systematic investigation reveals that unlike graphite,the biochar electrode displays good compatibility with the electrolyte typically employed in sulfur batteries.The CBSG/Li_(2)S70Gr30 full-cell demonstrates an initial charge and discharge capacities of 726 and 537 mAh g^(-1),respectively,at 0.05C with a coulombic efficiency of 74%.Moreover,it discloses a reversible capacity of 330 mAh g^(-1)(0.1 C)after over 300 cycles.Based on these achievements,the CBSG/Li_(2)S70Gr30 battery system can be considered as a promising energy storage solution for electric vehicles(EVs),especially when taking into account its easy scalability to an industrial level.

Modification of Li Anode with Perfluorodecyltrimethoxysilane to Enhance the Performance of Lithium Metal Battery

The solid electrolyte interphase (SEI) on the surface of lithium metal anodes can dictate the electrochemical performance of lithium-metal-based batteries. Due to ineffective adhesion, the natural SEI layer may detach from the lithium negative electrode during interface fluctuations, thereby deteriorating the electrochemical performance of lithium-metal-based batteries. This work introduces perfluorosiloxane coupling agents as interfacial adhesion promoters, chemically bonding and physically entangling the lithium metal with the SEI via the formation of Li-O-Si bonds with the inorganic reactive groups anchoring to the Li substrate and the organic functional groups participating in the formation of the SEI layer, thus binding with its components. Lithium metal batteries modified with silane coupling agents exhibit superior electrochemical performance compared to unmodified lithium metal batteries. The modified lithium metal battery retains a specific capacity of 162 mAh/g after 200 cycles, while the unmodified lithium metal battery only retains 140 mAh/g.

Explainable Neural Network for Sensitivity Analysis of Lithium-ion Battery Smart Production

Battery production is crucial for determining the quality of electrode,which in turn affects the manufactured battery performance.As battery production is complicated with strongly coupled intermediate and control parameters,an efficient solution that can perform a reliable sensitivity analysis of the production terms of interest and forecast key battery properties in the early production phase is urgently required.This paper performs detailed sensitivity analysis of key production terms on determining the properties of manufactured battery electrode via advanced data-driven modelling.To be specific,an explainable neural network named generalized additive model with structured interaction(GAM-SI)is designed to predict two key battery properties,including electrode mass loading and porosity,while the effects of four early production terms on manufactured batteries are explained and analysed.The experimental results reveal that the proposed method is able to accurately predict battery electrode properties in the mixing and coating stages.In addition,the importance ratio ranking,global interpretation and local interpretation of both the main effects and pairwise interactions can be effectively visualized by the designed neural network.Due to the merits of interpretability,the proposed GAM-SI can help engineers gain important insights for understanding complicated production behavior,further benefitting smart battery production.

Correction:Direct Regeneration of Spent Lithium‑Ion Battery Cathodes:From Theoretical Study to Production Practice

The Highlights session of the article unfortunately was taken falsely from another manuscript.The correct Highlights session is now in place.The correct is:Analyze the primary causes of cathode failure in three representative batteries,illustrating their underlying regeneration mechanism.

Fluorine-Modulated MXene-Derived Catalysts for Multiphase Sulfur Conversion in Lithium-Sulfur Battery

Fluorine owing to its inherently high electronegativity exhibits charge delocalization and ion dissociation capabilities;as a result,there has been an influx of research studies focused on the utilization of fluorides to optimize solid electrolyte interfaces and provide dynamic protection of electrodes to regulate the reaction and function performance of batteries.Nonetheless,the shuttle effect and the sluggish redox reaction kinetics emphasize the potential bottlenecks of lithium-sulfur batteries.Whether fluorine modulation regulate the reaction process of Li-S chemistry?Here,the TiOF/Ti_(3)C_(2)MXene nanoribbons with a tailored F distribution were constructed via an NH4F fluorinated method.Relying on in situ characterizations and electrochemical analysis,the F activates the catalysis function of Ti metal atoms in the consecutive redox reaction.The positive charge of Ti metal sites is increased due to the formation of O-Ti-F bonds based on the Lewis acid-base mechanism,which contributes to the adsorption of polysulfides,provides more nucleation sites and promotes the cleavage of S-S bonds.This facilitates the deposition of Li_(2)S at lower overpotentials.Additionally,fluorine has the capacity to capture electrons originating from Li_(2)S dissolution due to charge compensation mechanisms.The fluorine modulation strategy holds the promise of guiding the construction of fluorine-based catalysts and facilitating the seamless integration of multiple consecutive heterogeneous catalytic processes.

Electric-controlled pressure relief valve for enhanced safety in liquid-cooled lithium-ion battery packs

The liquid-cooled battery energy sto rage system(LCBESS) has gained significant attention due to its superior thermal management capacity.However,liquid-cooled battery pack(LCBP) usually has a high sealing level above IP65,which can trap flammable and explosive gases from battery thermal runaway and cause explosions.This poses serious safety risks and challenges for LCBESS.In this study,we tested overcharged battery inside a commercial LCBP and found that the conventionally mechanical pressure relief valve(PRV) on the LCBP had a delayed response and low-pressure relief efficiency.A realistic 20-foot model of an energy storage cabin was constructed using the Flacs finite element simulation software.Comparative studies were conducted to evaluate the pressure relief efficiency and the influence on neighboring battery packs in case of internal explosions,considering different sizes and installation positions of the PRV.Here,a newly developed electric-controlled PRV integrated with battery fault detection is introduced,capable of starting within 50 ms of the battery safety valve opening.Furthermore,the PRV was integrated with the battery management system and changed the battery charging and discharging strategy after the PRV was opened.Experimental tests confirmed the efficacy of this method in preventing explosions.This paper addresses the safety concerns associated with LCBPs and proposes an effective solution for explosion relief.

Constructing Al@C-Sn pellet anode without passivation layer for lithium-ion battery

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.

Lithium-Ion Battery Pack Based on Fuzzy Logic Control Research on Multi-Layer Equilibrium Circuits

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.

Analysis of Differences in Electrochemical Performance Between Coin and Pouch Cells for Lithium-Ion Battery Applications

Small coin cell batteries are predominantly used for testing lithium-ion batteries(LIBs)in academia because they require small amounts of material and are easy to assemble.However,insufficient attention is given to difference in cell performance that arises from the differences in format between coin cells used by academic researchers and pouch or cylindrical cells which are used in industry.In this article,we compare coin cells and pouch cells of different size with exactly the same electrode materials,electrolyte,and electrochemical conditions.We show the battery impedance changes substantially depending on the cell format using techniques including Electrochemical Impedance Spectroscopy(EIS)and Galvanostatic Intermittent Titration Technique(GITT).Using full cell NCA-graphite LIBs,we demonstrate that this difference in impedance has important knock-on effects on the battery rate performance due to ohmic polarization and the battery life time due to Li metal plating on the anode.We hope this work will help researchers getting a better idea of how small coin cell formats impact the cell performance and help predicting improvements that can be achieved by implementing larger cell formats.

Solvent-Free Manufacturing of Lithium-Ion Battery Electrodes via Cold Plasma

Slurry casting has been used to fabricate lithium-ion battery electrodes for decades,which involves toxic and expensive organic solvents followed by high-cost vacuum drying and electrode calendering.This work presents a new manufacturing method using a nonthermal plasma to create inter-particle binding without using any polymeric binding materials,enabling solvent-free manufacturing electrodes with any electrochemistry of choice.The cold-plasma-coating technique enables fabricating electrodes with thickness(>200 pm),high mass loading(>30 mg cm^(-2)),high peel strength,and the ability to print lithium-ion batteries in an arbitrary geometry.This crosscutting,chemistry agnostic,platform technology would increase energy density,eliminate the use of solvents,vacuum drying,and calendering processes during production,and reduce manufacturing cost for current and future cell designs.Here,lithium iron phosphate and lithium cobalt oxide were used as examples to demonstrate the efficacy of the cold-plasma-coating technique.It is found that the mechanical peel strength of cold-plasma-coating-manufactured lithium iron phosphate is over an order of magnitude higher than that of slurry-casted lithium iron phosphate electrodes.Full cells assembled with a graphite anode and the cold-plasma-coating-lithium iron phosphate cathode offer highly reversible cycling performance with a capacity retention of 81.6%over 500 cycles.For the highly conductive cathode material lithium cobalt oxide,an areal capacity of 4.2 mAh cm^(-2)at 0.2 C is attained.We anticipate that this new,highly scalable manufacturing technique will redefine global lithium-ion battery manufacturing providing significantly reduced plant footprints and material costs.

Abnormal State Detection in Lithium-ion Battery Using Dynamic Frequency Memory and Correlation Attention LSTM Autoencoder

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.

Enhanced High-Temperature Cycling Stability of Garnet-Based All Solid-State Lithium Battery Using a Multi-Functional Catholyte Buffer Layer

The pursuit of safer and high-performance lithium-ion batteries(LIBs)has triggered extensive research activities on solid-state batteries,while challenges related to the unstable electrode-electrolyte interface hinder their practical implementation.Polymer has been used extensively to improve the cathode-electrolyte interface in garnet-based all-solid-state LIBs(ASSLBs),while it introduces new concerns about thermal stability.In this study,we propose the incorporation of a multi-functional flame-retardant triphenyl phos-phate additive into poly(ethylene oxide),acting as a thin buffer layer between LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cathode and garnet electro-lyte.Through electrochemical stability tests,cycling performance evaluations,interfacial thermal stability analysis and flammability tests,improved thermal stability(capacity retention of 98.5%after 100 cycles at 60℃,and 89.6%after 50 cycles at 80℃)and safety characteristics(safe and stable cycling up to 100℃)are demonstrated.Based on various materials characterizations,the mechanism for the improved thermal stability of the interface is proposed.The results highlight the potential of multi-functional flame-retardant additives to address the challenges associated with the electrode-electrolyte interface in ASSLBs at high temperature.Efficient thermal modification in ASSLBs operating at elevated temperatures is also essential for enabling large-scale energy storage with safety being the primary concern.

A New Equalization Method for Lithium-Ion Battery Packs Based on CUK

Aiming at the traditional CUK equalizer can only perform energy equalization between adjacent batteries,if the two single batteries that need to be equalized are far away from each other,there will be the problem of longer energy transmission path and lower equalization efficiency,this paper optimizes the CUK equalizer and optimizes its peripheral selection circuit,which can support the equalization of single batteries at any two positions.The control strategy adopts the open-circuit voltage(OVC)of the battery and the state of charge(SOC)of the battery as the equalization variables,and selects the corresponding equalization variables according to the energy conditions of the two batteries that need to be equalized,and generates the adaptive equalization current with an adaptive PID controller in order to improve the equalization efficiency.Simulation modeling is performed in Matlab/Simulink 2021b,and the experimental results show that the optimized CUK equalizer in this paper improves the equalization time by 25.58%compared with the traditional CUK equalizer.In addition,compared with the mean value difference(MVD)method,the adaptive PID method reduces the equalization time by about 30%in the static and charging and discharging experimental environments,which verifies the superiority of this equalization scheme.