With the widespread use of lithium-ion batteries in electric vehicles,energy storage,and mobile terminals,there is an urgent need to develop cathode materials with specific properties.However,existing material control...With the widespread use of lithium-ion batteries in electric vehicles,energy storage,and mobile terminals,there is an urgent need to develop cathode materials with specific properties.However,existing material control synthesis routes based on repetitive experiments are often costly and inefficient,which is unsuitable for the broader application of novel materials.The development of machine learning and its combination with materials design offers a potential pathway for optimizing materials.Here,we present a design synthesis paradigm for developing high energy Ni-rich cathodes with thermal/kinetic simulation and propose a coupled image-morphology machine learning model.The paradigm can accurately predict the reaction conditions required for synthesizing cathode precursors with specific morphologies,helping to shorten the experimental duration and costs.After the model-guided design synthesis,cathode materials with different morphological characteristics can be obtained,and the best shows a high discharge capacity of 206 mAh g^(−1)at 0.1C and 83%capacity retention after 200 cycles.This work provides guidance for designing cathode materials for lithium-ion batteries,which may point the way to a fast and cost-effective direction for controlling the morphology of all types of particles.展开更多
The accurate representation of lithium plating and aging phenomena has posed a persistent challenge within the battery research community.Empirical evidence underscores the pivotal role of cell structure in influencin...The accurate representation of lithium plating and aging phenomena has posed a persistent challenge within the battery research community.Empirical evidence underscores the pivotal role of cell structure in influencing aging behaviors and lithium plating within lithium-ion batteries(LIBs).Available lithium-ion plating models often falter in detailed description when integrating the structural intricacies.To address this challenge,this study proposes an innovative hierarchical model that intricately incorporates the layered rolling structure in cells.Notably,our model demonstrates a remarkable capacity to predict the non-uniform distribution of current density and overpotential along the rolling direction of LIBs.Subsequently,we delve into an insightful exploration of the structural factors that influence lithium plating behavior,leveraging the foundation laid by our established model.Furthermore,we easily update the hierarchical model by considering aging factors.This aging model effectively anticipates capacity fatigue and lithium plating tendencies across individual layers of LIBs,all while maintaining computational efficiency.In light of our findings,this model yields novel perspectives on capacity fatigue dynamics and local lithium plating behaviors,offering a substantial advancement compared to existing models.This research paves the way for more efficient and tailored LIB design and operation,with broad implications for energy storage technologies.展开更多
Iron oxide(Fe_(2)O_(3))emerges as a highly attractive anode candidate among rapidly expanding energy storage market.Nonethe-less,its considerable volume changes during cycling as an electrode material result in a vast...Iron oxide(Fe_(2)O_(3))emerges as a highly attractive anode candidate among rapidly expanding energy storage market.Nonethe-less,its considerable volume changes during cycling as an electrode material result in a vast reduced battery cycle life.In this work,an ap-proach is pioneered for preparing high-performance Fe_(2)O_(3)anode materials,by innovatively synthesizing a triple-layer yolk-shell Fe_(2)O_(3)uniformly coated with a conductive polypyrrole(Ppy)layer(Fe_(2)O_(3)@Ppy-TLY).The uniform polypyrrole coating introduces more reac-tion sites and adsorption sites,and maintains structure stability through charge-discharge process.In the uses as lithium-ion battery elec-trodes,Fe_(2)O_(3)@Ppy-TLY demonstrates high reversible specific capacity(maintaining a discharge capacity of 1375.11 mAh·g^(−1)after 500 cycles at 1 C),exceptional cycling stability(retaining the steady charge-discharge performance at 544.33 mAh·g^(−1)after 6000 ultrafast charge-discharge cycles at a 10 C current density),and outstanding high current charge-discharge performance(retaining a reversible ca-pacity of 156.75 mAh·g^(−1)after 10000 cycles at 15 C),thereby exhibiting superior lithium storage performance.This work introduces in-novative advancements for Fe_(2)O_(3)anode design,aiming to enhance its performance in energy storage fields.展开更多
Lithium-ion batteries(LIBs)and lithium-sulfur(Li–S)batteries are two types of energy storage systems with significance in both scientific research and commercialization.Nevertheless,the rational design of electrode m...Lithium-ion batteries(LIBs)and lithium-sulfur(Li–S)batteries are two types of energy storage systems with significance in both scientific research and commercialization.Nevertheless,the rational design of electrode materials for overcoming the bottlenecks of LIBs and Li–S batteries(such as low diffusion rates in LIBs and low sulfur utilization in Li–S batteries)remain the greatest challenge,while two-dimensional(2D)electrodes materials provide a solution because of their unique structural and electrochemical properties.In this article,from the perspective of ab-initio simulations,we review the design of 2D electrode materials for LIBs and Li–S batteries.We first propose the theoretical design principles for 2D electrodes,including stability,electronic properties,capacity,and ion diffusion descriptors.Next,classified examples of promising 2D electrodes designed by theoretical simulations are given,covering graphene,phosphorene,MXene,transition metal sulfides,and so on.Finally,common challenges and a future perspective are provided.This review paves the way for rational design of 2D electrode materials for LIBs and Li–S battery applications and may provide a guide for future experiments.展开更多
Although the lithium-ion batteries(LIBs) have been increasingly applied in consumer electronics, electric vehicles,and smart grid, they still face great challenges from the continuously improving requirements of energ...Although the lithium-ion batteries(LIBs) have been increasingly applied in consumer electronics, electric vehicles,and smart grid, they still face great challenges from the continuously improving requirements of energy density, power density, service life, and safety. To solve these issues, various studies have been conducted surrounding the battery design and management methods in recent decades. In the hope of providing some inspirations to the research in this field, the state of the art of design and management methods for LIBs are reviewed here from the perspective of process systems engineering. First, different types of battery models are summarized extensively, including electrical model and multi-physics coupled model, and the parameter identification methods are introduced correspondingly. Next, the model based battery design methods are reviewed briefly on three different scales, namely, electrode scale, cell scale, and pack scale. Then, the battery model based battery management methods, especially the state estimation methods with different model types are thoroughly compared. The key science and technology challenges for the development of battery systems engineering are clarified finally.展开更多
The interfacial debonding between the active layer and the current collector has been recognized as a critical mechanism for battery fading,and thus has attracted great efforts focused on the related analyses.However,...The interfacial debonding between the active layer and the current collector has been recognized as a critical mechanism for battery fading,and thus has attracted great efforts focused on the related analyses.However,much still remains to be studied regarding practical methods for suppressing electrode debonding,especially from the perspective of mechanics.In this paper,a pre-strain strategy of current collectors to alleviate electrode debonding is proposed.An analytical model for a symmetric electrode with a deformable and limited-thickness current collector is developed to analyze the debonding behavior involving both a pre-strain of the current collector and an eigen-strain of the active layers.The results reveal that the well-designed pre-strain can significantly delay the debonding onset(by up to 100%)and considerably reduce the debonding size.The critical values of the pre-strain are identified,and the pre-strain design principles are also provided.Based on these findings,this work sheds light on the mechanical design to suppress electrode degradation.展开更多
Direct recycling is a novel approach to overcoming the drawbacks of conventional lithium-ion battery(LIB)recycling processes and has gained considerable attention from the academic and industrial sectors in recent yea...Direct recycling is a novel approach to overcoming the drawbacks of conventional lithium-ion battery(LIB)recycling processes and has gained considerable attention from the academic and industrial sectors in recent years.The primary objective of directly recycling LIBs is to efficiently recover and restore the active electrode materials and other components in the solid phase while retaining electrochemical performance.This technology's advantages over traditional pyrometallurgy and hydrometallurgy are costeffectiveness,energy efficiency,and sustainability,and it preserves the material structure and morphology and can shorten the overall recycling path.This review extensively discusses the advancements in the direct recycling of LIBs,including battery sorting,pretreatment processes,separation of cathode and anode materials,and regeneration and quality enhancement of electrode materials.It encompasses various approaches to successfully regenerate high-value electrode materials and streamlining the recovery process without compromising their electrochemical properties.Furthermore,we highlight key challenges in direct recycling when scaled from lab to industries in four perspectives:(1)battery design,(2)disassembling,(3)electrode delamination,and(4)commercialization and sustainability.Based on these challenges and changing market trends,a few strategies are discussed to aid direct recycling efforts,such as binders,electrolyte selection,and alternative battery designs;and recent transitions and technological advancements in the battery industry are presented.展开更多
Li-rich layered oxide(LRLO)cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density,which combines cationic and anionic redox activities.H...Li-rich layered oxide(LRLO)cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density,which combines cationic and anionic redox activities.However,continuous voltage decay during cycling remains the primary obstacle for practical applications,which has yet to be fundamentally addressed.It is widely acknowledged that voltage decay originates from the irreversible migration of transition metal ions,which usually further exacerbates structural evolution and aggravates the irreversible oxygen redox reactions.Recently,constructing O2-type structure has been considered one of the most promising approaches for inhibiting voltage decay.In this review,the relationship between voltage decay and structural evolution is systematically elucidated.Strategies to suppress voltage decay are systematically summarized.Additionally,the design of O2-type structure and the corresponding mechanism of suppressing voltage decay are comprehensively discussed.Unfortunately,the reported O2-type LRLO cathodes still exhibit partially disordered structure with extended cycles.Herein,the factors that may cause the irreversible transition metal migrations in O2-type LRLO materials are also explored,while the perspectives and challenges for designing high-performance O2-type LRLO cathodes without voltage decay are proposed.展开更多
Flexible lithium-ion batteries(FLBs)are of critical importance to the seamless power supply of flexible and wearable electronic devices.However,the simultaneous acquirements of mechanical deformability and high energy...Flexible lithium-ion batteries(FLBs)are of critical importance to the seamless power supply of flexible and wearable electronic devices.However,the simultaneous acquirements of mechanical deformability and high energy density remain a major challenge for FLBs.Through billions of years of evolutions,many plants and animals have developed unique compositional and structural characteristics,which enable them to have both high mechanical deformability and robustness to cope with the complex and stressful environment.Inspired by nature,many new materials and designs emerge recently to achieve mechanically flexible and high storage capacity of lithiumion batteries at the same time.Here,we summarize these novel FLBs inspired by natural and biological materials and designs.We first give a brief introduction to the fundamentals and challenges of FLBs.Then,we highlight the latest achievements based on nature inspiration,including fiber-shaped FLBs,origami and kirigami-derived FLBs,and the nature-inspired structural designs in FLBs.Finally,we discuss the current status,remaining challenges,and future opportunities for the development of FLBs.This concise yet focused review highlights current inspirations in FLBs and wishes to broaden our view of FLB materials and designs,which can be directly“borrowed”from nature.展开更多
Based upon advances in theoretical algorithms, modeling and simulations, and computer technologies, the rational design of materials, cells, devices, and packs in the field of lithium-ion batteries is being realized i...Based upon advances in theoretical algorithms, modeling and simulations, and computer technologies, the rational design of materials, cells, devices, and packs in the field of lithium-ion batteries is being realized incrementally and will at some point trigger a paradigm revolution by combining calculations and experiments linked by a big shared database, enabling accelerated development of the whole industrial chain. Theory and multi-scale modeling and simulation, as supplements to experimental efforts, can help greatly to close some of the current experimental and technological gaps, as well as predict path-independent properties and help to fundamentally understand path-independent performance in multiple spatial and temporal scales.展开更多
With the advent of flexible/wearable electronic devices,flexible lithium-ion batteries(LIBs)have attracted significant attention as optimal power source candidates.Flexible LIBs with good flexibility,mechanical stabil...With the advent of flexible/wearable electronic devices,flexible lithium-ion batteries(LIBs)have attracted significant attention as optimal power source candidates.Flexible LIBs with good flexibility,mechanical stability,and high energy density are still an enormous challenge.In recent years,many complex and diverse design methods for flexible LIBs have been reported.The design and evaluation of ideal flexible LIBs must take into consideration both mechanical and electrochemical factors.In this review,the recent progress and challenges of flexible LIBs are reviewed from a mechano-electrochemical perspective.The recent progress in flexible LIB design is addressed concerning flexible material and configuration design.The mechanical and electrochemical evaluations of flexible LIBs are also summarized.Furthermore,mechano-electrochemical perspectives for the future direction of flexible LIBs are also discussed.Finally,the relationship between mechanical loading and the electrode process is analyzed from a mechano-electrochemical perspective.The evaluation of flexible LIBs should be based on mechano-electrochemical processes.Reviews and perspectives are of great significance to the design and practicality of flexible LIBs,which is contributed to bridging the gap between laboratory exploration and practical applications.展开更多
Various nanostructured architectures have been demonstrated to be effective to address the issues of high capacity Si anodes. However, the scale-up of these nano-Si materials is still a critical obstacle for commercia...Various nanostructured architectures have been demonstrated to be effective to address the issues of high capacity Si anodes. However, the scale-up of these nano-Si materials is still a critical obstacle for commercialization. Herein, we use industrial ferrosilicon as low-cost Si source and introduce a facile and scalable method to fabricate a micrometer-sized ferrosilicon/C composite anode, in which ferrosilicon microparticles are wrapped with multi-layered carbon nanosheets. The multi-layered carbon nanosheets could effectively buffer the volume variation of Si as well as create an abundant and reliable conductivity framework, ensuring fast transport of electrons. As a result, the micrometer-sized ferrosilicon/C anode achieves a stable cycling with 805.9 m Ah g-1 over 200 cycles at 500 mA g-1 and a good rate capability of455.6 mAh g-1 at 10 A g-1. Therefore, our approach based on ferrosilicon provides a new opportunity in fabricating cost-effective, pollution-free, and large-scale Si electrode materials for high energy lithium-ion batteries.展开更多
Lithium-ion(Li-ion) battery and lithium-sulfur(Li-S) battery have attracted significant attention as promising components for large-scale energy storage because of high theoretical capacity of Li,excellent energy dens...Lithium-ion(Li-ion) battery and lithium-sulfur(Li-S) battery have attracted significant attention as promising components for large-scale energy storage because of high theoretical capacity of Li,excellent energy density or environmental friendness for two kinds of batteries.However,there still exist some respective obstacles for commercial applications,such as limited theoretical capacity,high cost and low conductivity of Li-ion cells or shuttle effect of lithium polysulfides of Li-S cells.As typical twodimensional materials,layered double hydroxides(LDHs) exhibit excellent potential in the field of energy storage due to facile tunability of composition,structure and morphology as well as convenient composite and strong catalytic properties.Consequently,various LDHs toward novel separators or interlayers,cathodes,anodes,and interesting catalytic templates are researched to resolve these challenges.In this review,the recent progress for LDHs applied in Li-ion batteries and Li-S batteries including the synthesis methods,designs and applications is presented and reviewed.Meanwhile,the existing challenges and future perspectives associated with material designs and practical applications of LDHs for these two classes of cells are discussed.WeWe hope that the review can attract more attention and inspire more profound researches toward the LDH-based electrochemical materials for energy storage.展开更多
For several years now, electric vehicles (EVs) have been expected to become widely available in the micro-mobility field. However, the insufficiency of such vehicles’ battery-charging and discharging performance has ...For several years now, electric vehicles (EVs) have been expected to become widely available in the micro-mobility field. However, the insufficiency of such vehicles’ battery-charging and discharging performance has limited their practical use. A hybrid energy storage system, which comprises a capacitor and battery, is a promising solution to this problem;however, to apply model-based designs, which are indispensable to embedded systems, such as the electronic control units used in EVs, a simple and accurate capacitor model is required. Within this framework, a lithium-ion capacitor (LIC) model is proposed, and its charging and discharging performances are evaluated against an actual LIC. The model corresponds accurately to the actual LIC, and the results indicate that the proposed LIC model will work well when used with Model-Based Design (MBD).展开更多
Separators are indispensable components of modern electrochemical energy storage devices such as lithium-ion batteries(LIBs).They perform the critical function of physically separating the electrodes to prevent short-...Separators are indispensable components of modern electrochemical energy storage devices such as lithium-ion batteries(LIBs).They perform the critical function of physically separating the electrodes to prevent short-circuits while permitting the ions to pass through.While conventional separators using polypropylene(PP) and polyethylene(PE) are prone to shrinkage and melting at relatively high temperatures(150℃ or above) causing short circuits and thermal runaway,separators made of thermally stable polyimides(PIs) are electrochemically stable and resistant to high temperatures,and possess good mechanical strength-making them a promising solution to the safety concerns of LIBs.In this review,the research progress on PI separators for use in LIBs is summarized with a special focus on molecular design and microstructural control.In view of the significant progress in advanced chemistries beyond LIBs,recent advances in PI-based membranes for applications in lithium-sulfur,lithium-metal,and solid-state batteries are also reviewed.Finally,practical issues are also discussed along with their prospects.展开更多
Developing high-performance lithium-ion batteries (LIBs) with high energy density, rate capability and long cycle life are essential for the ever-growing practical application. Among all battery components, the binder...Developing high-performance lithium-ion batteries (LIBs) with high energy density, rate capability and long cycle life are essential for the ever-growing practical application. Among all battery components, the binder plays a key role in determining the preparation of electrodes and the improvement of battery performance, in spite of a low usage amount. The main function of binder is to bond the active material, conductive additive and current collector together and provide electron and ion channels to improve the kinetics of electrochemical reaction. With the ever-increasing requirement of high energy density by LIBs, technical challenges such as volume expansion and active material dissolution are attracting worldwide attentions, where binder is thought to provide a new solution.There are two main categories (organic solvent soluble binder and water-soluble binder) and abundant polar functional groups providing adhesion ability. It is of great significance to timely summarize the latest progress in battery binders and present the principles for designing novel binders with both robust binding interaction and outstanding electrode stabilization function. This review begins with an introduction of the binding mechanism and the related binding forces, including mechanical interlocking forces and interfacial forces. Then, we discussed four different strategies (the enhancement of binding force,the formation of three-dimensional (3D) network, the enhancement of conductivity and binders with special functions) for constructing ideal binder system in order to satisfy the specific demands of different batteries, such as LIBs and lithium–sulfur (Li–S) batteries. Finally, some prospective and promising directions of binder design are proposed based on the existing and emerging binders and guide the development of the next-generation LIBs.展开更多
Lithium-ion batteries,first commercialized in 1991,have been thriving for the past 30 years and become an important basis for portable electronics and electric vehicles.However,this first generation of lithium-ion bat...Lithium-ion batteries,first commercialized in 1991,have been thriving for the past 30 years and become an important basis for portable electronics and electric vehicles.However,this first generation of lithium-ion batteries built on the intercalation materials has limited energy density and can not meet the increased demand of various applications.Thus,a transition from intercalation to alloying chemistry for anodes is on call.Silicon,as the most attractive alloying anode material,has been on the research focus for next-generation highenergy density battery.Alloying mechanism benefits silicon a large capacity while brings silicon the challenge of volume expansion.This article discusses the structure design strategies to address the issues of large volume change and interface instability.展开更多
Electric vehicles(EVs)are globally undergoing rapid developments,and have great potentials to replace the traditional vehicles based on fossil fuels.Power-type lithium-ion batteries(LIBs)have been widely used for EVs,...Electric vehicles(EVs)are globally undergoing rapid developments,and have great potentials to replace the traditional vehicles based on fossil fuels.Power-type lithium-ion batteries(LIBs)have been widely used for EVs,owing to high power densities,good charge/discharge stability,and long cycle life.The driving ranges and acceleration performances are gaining increasing concerns from customers,which depend highly on the power level of LIBs.With the increase in power outputs,rising heat generation significantly affects the battery performances,and in particular operation safety.Meanwhile,the cold-start performance is still an intractable problem under extreme conditions.These challenges put forward higher requirements for a dedicated battery thermal management system(BTMS).Compared to traditional BTMSs in EVs,the heat pipe-based BTMS has great application prospects owing to its compact structure,flexibility,low cost,and especially high thermal conductivity.Encompassing this topic,this review first introduces heat generation phenomena and temperature characteristics of LIBs.Multiple abuse conditions and thermal runaway issues are described afterward.Typical cooling and preheating methods for designing a BTMS are also discussed.More emphasis on this review is put on the use of various heat pipes for BTMSs to enhance the thermal performances of LIBs.For lack of wide application in actual EVs,more efforts should be made to extend the use of heat pipes for constructing an energy-efficient,cost-effective,and reliable BTMS to improve the performances and safety of EVs.展开更多
基金supported by the National Natural Science Foundation of China(52072036)the Key Research and Development Program of Henan province,China(231111242500).
文摘With the widespread use of lithium-ion batteries in electric vehicles,energy storage,and mobile terminals,there is an urgent need to develop cathode materials with specific properties.However,existing material control synthesis routes based on repetitive experiments are often costly and inefficient,which is unsuitable for the broader application of novel materials.The development of machine learning and its combination with materials design offers a potential pathway for optimizing materials.Here,we present a design synthesis paradigm for developing high energy Ni-rich cathodes with thermal/kinetic simulation and propose a coupled image-morphology machine learning model.The paradigm can accurately predict the reaction conditions required for synthesizing cathode precursors with specific morphologies,helping to shorten the experimental duration and costs.After the model-guided design synthesis,cathode materials with different morphological characteristics can be obtained,and the best shows a high discharge capacity of 206 mAh g^(−1)at 0.1C and 83%capacity retention after 200 cycles.This work provides guidance for designing cathode materials for lithium-ion batteries,which may point the way to a fast and cost-effective direction for controlling the morphology of all types of particles.
基金the financial support from The National Key Research and Development Program of China(2022YFB3305402)The National Natural Science Foundation of China(12272072)+1 种基金The Key Project of Chongqing Technology Innovation and Application Development(CSTB2022TIAD-KPX0037)Research Project of the State Key Laboratory of Intel igent Vehicle Safety Technology(NVHSKL-202207)
文摘The accurate representation of lithium plating and aging phenomena has posed a persistent challenge within the battery research community.Empirical evidence underscores the pivotal role of cell structure in influencing aging behaviors and lithium plating within lithium-ion batteries(LIBs).Available lithium-ion plating models often falter in detailed description when integrating the structural intricacies.To address this challenge,this study proposes an innovative hierarchical model that intricately incorporates the layered rolling structure in cells.Notably,our model demonstrates a remarkable capacity to predict the non-uniform distribution of current density and overpotential along the rolling direction of LIBs.Subsequently,we delve into an insightful exploration of the structural factors that influence lithium plating behavior,leveraging the foundation laid by our established model.Furthermore,we easily update the hierarchical model by considering aging factors.This aging model effectively anticipates capacity fatigue and lithium plating tendencies across individual layers of LIBs,all while maintaining computational efficiency.In light of our findings,this model yields novel perspectives on capacity fatigue dynamics and local lithium plating behaviors,offering a substantial advancement compared to existing models.This research paves the way for more efficient and tailored LIB design and operation,with broad implications for energy storage technologies.
基金supported by the Natural Science Foundation of Jiangsu Province of China(No.BK20201008).
文摘Iron oxide(Fe_(2)O_(3))emerges as a highly attractive anode candidate among rapidly expanding energy storage market.Nonethe-less,its considerable volume changes during cycling as an electrode material result in a vast reduced battery cycle life.In this work,an ap-proach is pioneered for preparing high-performance Fe_(2)O_(3)anode materials,by innovatively synthesizing a triple-layer yolk-shell Fe_(2)O_(3)uniformly coated with a conductive polypyrrole(Ppy)layer(Fe_(2)O_(3)@Ppy-TLY).The uniform polypyrrole coating introduces more reac-tion sites and adsorption sites,and maintains structure stability through charge-discharge process.In the uses as lithium-ion battery elec-trodes,Fe_(2)O_(3)@Ppy-TLY demonstrates high reversible specific capacity(maintaining a discharge capacity of 1375.11 mAh·g^(−1)after 500 cycles at 1 C),exceptional cycling stability(retaining the steady charge-discharge performance at 544.33 mAh·g^(−1)after 6000 ultrafast charge-discharge cycles at a 10 C current density),and outstanding high current charge-discharge performance(retaining a reversible ca-pacity of 156.75 mAh·g^(−1)after 10000 cycles at 15 C),thereby exhibiting superior lithium storage performance.This work introduces in-novative advancements for Fe_(2)O_(3)anode design,aiming to enhance its performance in energy storage fields.
基金supported by the Research Grants Council of the Hong Kong Special Administrative Region,China(PolyU152178/20 E)the Hong Kong Polytechnic University(1-W19S)Science and Technology Program of Guangdong Province of China(2020A0505090001).
文摘Lithium-ion batteries(LIBs)and lithium-sulfur(Li–S)batteries are two types of energy storage systems with significance in both scientific research and commercialization.Nevertheless,the rational design of electrode materials for overcoming the bottlenecks of LIBs and Li–S batteries(such as low diffusion rates in LIBs and low sulfur utilization in Li–S batteries)remain the greatest challenge,while two-dimensional(2D)electrodes materials provide a solution because of their unique structural and electrochemical properties.In this article,from the perspective of ab-initio simulations,we review the design of 2D electrode materials for LIBs and Li–S batteries.We first propose the theoretical design principles for 2D electrodes,including stability,electronic properties,capacity,and ion diffusion descriptors.Next,classified examples of promising 2D electrodes designed by theoretical simulations are given,covering graphene,phosphorene,MXene,transition metal sulfides,and so on.Finally,common challenges and a future perspective are provided.This review paves the way for rational design of 2D electrode materials for LIBs and Li–S battery applications and may provide a guide for future experiments.
基金National Key R&D Program of China(Grant No.2018YFB0905000)the National Natural Science Foundation of China(Grant No.21978166).
文摘Although the lithium-ion batteries(LIBs) have been increasingly applied in consumer electronics, electric vehicles,and smart grid, they still face great challenges from the continuously improving requirements of energy density, power density, service life, and safety. To solve these issues, various studies have been conducted surrounding the battery design and management methods in recent decades. In the hope of providing some inspirations to the research in this field, the state of the art of design and management methods for LIBs are reviewed here from the perspective of process systems engineering. First, different types of battery models are summarized extensively, including electrical model and multi-physics coupled model, and the parameter identification methods are introduced correspondingly. Next, the model based battery design methods are reviewed briefly on three different scales, namely, electrode scale, cell scale, and pack scale. Then, the battery model based battery management methods, especially the state estimation methods with different model types are thoroughly compared. The key science and technology challenges for the development of battery systems engineering are clarified finally.
基金Project supported by the National Natural Science Foundation of China(Nos.12072183,11872236,12172205)the Key Research Project of Zhejiang Laboratory of China(No.2021PE0AC02)。
文摘The interfacial debonding between the active layer and the current collector has been recognized as a critical mechanism for battery fading,and thus has attracted great efforts focused on the related analyses.However,much still remains to be studied regarding practical methods for suppressing electrode debonding,especially from the perspective of mechanics.In this paper,a pre-strain strategy of current collectors to alleviate electrode debonding is proposed.An analytical model for a symmetric electrode with a deformable and limited-thickness current collector is developed to analyze the debonding behavior involving both a pre-strain of the current collector and an eigen-strain of the active layers.The results reveal that the well-designed pre-strain can significantly delay the debonding onset(by up to 100%)and considerably reduce the debonding size.The critical values of the pre-strain are identified,and the pre-strain design principles are also provided.Based on these findings,this work sheds light on the mechanical design to suppress electrode degradation.
基金National Research Foundation Singapore and National Environment Agency Singapore,Grant/Award Number:CTRL-2023-1D-01。
文摘Direct recycling is a novel approach to overcoming the drawbacks of conventional lithium-ion battery(LIB)recycling processes and has gained considerable attention from the academic and industrial sectors in recent years.The primary objective of directly recycling LIBs is to efficiently recover and restore the active electrode materials and other components in the solid phase while retaining electrochemical performance.This technology's advantages over traditional pyrometallurgy and hydrometallurgy are costeffectiveness,energy efficiency,and sustainability,and it preserves the material structure and morphology and can shorten the overall recycling path.This review extensively discusses the advancements in the direct recycling of LIBs,including battery sorting,pretreatment processes,separation of cathode and anode materials,and regeneration and quality enhancement of electrode materials.It encompasses various approaches to successfully regenerate high-value electrode materials and streamlining the recovery process without compromising their electrochemical properties.Furthermore,we highlight key challenges in direct recycling when scaled from lab to industries in four perspectives:(1)battery design,(2)disassembling,(3)electrode delamination,and(4)commercialization and sustainability.Based on these challenges and changing market trends,a few strategies are discussed to aid direct recycling efforts,such as binders,electrolyte selection,and alternative battery designs;and recent transitions and technological advancements in the battery industry are presented.
基金funded by the National Natural Science Foundation of China(Grant Nos.22279092 and 5202780089).
文摘Li-rich layered oxide(LRLO)cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density,which combines cationic and anionic redox activities.However,continuous voltage decay during cycling remains the primary obstacle for practical applications,which has yet to be fundamentally addressed.It is widely acknowledged that voltage decay originates from the irreversible migration of transition metal ions,which usually further exacerbates structural evolution and aggravates the irreversible oxygen redox reactions.Recently,constructing O2-type structure has been considered one of the most promising approaches for inhibiting voltage decay.In this review,the relationship between voltage decay and structural evolution is systematically elucidated.Strategies to suppress voltage decay are systematically summarized.Additionally,the design of O2-type structure and the corresponding mechanism of suppressing voltage decay are comprehensively discussed.Unfortunately,the reported O2-type LRLO cathodes still exhibit partially disordered structure with extended cycles.Herein,the factors that may cause the irreversible transition metal migrations in O2-type LRLO materials are also explored,while the perspectives and challenges for designing high-performance O2-type LRLO cathodes without voltage decay are proposed.
基金National Nature Science Foundation of China,Grant/Award Numbers:21875040,21905051Macao Science and Technology Development Fund,Grant/Award Numbers:FDCT-0035/2019/AMJ,FDCT-0057/2019/A1,FDCT-0092/2019/A2pt>。
文摘Flexible lithium-ion batteries(FLBs)are of critical importance to the seamless power supply of flexible and wearable electronic devices.However,the simultaneous acquirements of mechanical deformability and high energy density remain a major challenge for FLBs.Through billions of years of evolutions,many plants and animals have developed unique compositional and structural characteristics,which enable them to have both high mechanical deformability and robustness to cope with the complex and stressful environment.Inspired by nature,many new materials and designs emerge recently to achieve mechanically flexible and high storage capacity of lithiumion batteries at the same time.Here,we summarize these novel FLBs inspired by natural and biological materials and designs.We first give a brief introduction to the fundamentals and challenges of FLBs.Then,we highlight the latest achievements based on nature inspiration,including fiber-shaped FLBs,origami and kirigami-derived FLBs,and the nature-inspired structural designs in FLBs.Finally,we discuss the current status,remaining challenges,and future opportunities for the development of FLBs.This concise yet focused review highlights current inspirations in FLBs and wishes to broaden our view of FLB materials and designs,which can be directly“borrowed”from nature.
基金supported by the National Natural Science Foundation of China(Grant Nos.51372228 and 11234013)the National High Technology Research and Development Program of China(Grant No.2015AA034201)Shanghai Pujiang Program,China(Grant No.14PJ1403900)
文摘Based upon advances in theoretical algorithms, modeling and simulations, and computer technologies, the rational design of materials, cells, devices, and packs in the field of lithium-ion batteries is being realized incrementally and will at some point trigger a paradigm revolution by combining calculations and experiments linked by a big shared database, enabling accelerated development of the whole industrial chain. Theory and multi-scale modeling and simulation, as supplements to experimental efforts, can help greatly to close some of the current experimental and technological gaps, as well as predict path-independent properties and help to fundamentally understand path-independent performance in multiple spatial and temporal scales.
基金supported by National Natural Science Foundation of China(No.52074036)Technology Innovation Program of Beijing Institute of Technology(No.2019CX01021)BIT Teli Young Fellow。
文摘With the advent of flexible/wearable electronic devices,flexible lithium-ion batteries(LIBs)have attracted significant attention as optimal power source candidates.Flexible LIBs with good flexibility,mechanical stability,and high energy density are still an enormous challenge.In recent years,many complex and diverse design methods for flexible LIBs have been reported.The design and evaluation of ideal flexible LIBs must take into consideration both mechanical and electrochemical factors.In this review,the recent progress and challenges of flexible LIBs are reviewed from a mechano-electrochemical perspective.The recent progress in flexible LIB design is addressed concerning flexible material and configuration design.The mechanical and electrochemical evaluations of flexible LIBs are also summarized.Furthermore,mechano-electrochemical perspectives for the future direction of flexible LIBs are also discussed.Finally,the relationship between mechanical loading and the electrode process is analyzed from a mechano-electrochemical perspective.The evaluation of flexible LIBs should be based on mechano-electrochemical processes.Reviews and perspectives are of great significance to the design and practicality of flexible LIBs,which is contributed to bridging the gap between laboratory exploration and practical applications.
基金the National Natural Science Foundation of China(No:21703285)。
文摘Various nanostructured architectures have been demonstrated to be effective to address the issues of high capacity Si anodes. However, the scale-up of these nano-Si materials is still a critical obstacle for commercialization. Herein, we use industrial ferrosilicon as low-cost Si source and introduce a facile and scalable method to fabricate a micrometer-sized ferrosilicon/C composite anode, in which ferrosilicon microparticles are wrapped with multi-layered carbon nanosheets. The multi-layered carbon nanosheets could effectively buffer the volume variation of Si as well as create an abundant and reliable conductivity framework, ensuring fast transport of electrons. As a result, the micrometer-sized ferrosilicon/C anode achieves a stable cycling with 805.9 m Ah g-1 over 200 cycles at 500 mA g-1 and a good rate capability of455.6 mAh g-1 at 10 A g-1. Therefore, our approach based on ferrosilicon provides a new opportunity in fabricating cost-effective, pollution-free, and large-scale Si electrode materials for high energy lithium-ion batteries.
基金the National Natural Science Foundation of China(51973157,51673148 and 51678411)the Special Grade of the Financial Support from the China Postdoctoral Science Foundation(2020 T130469)+1 种基金the China Postdoctoral Science Foundation Grant(2019 M651047)the Science and Technology Plans of Tianjin(No.17PTSYJC00040 and18PTSYJC00180)for their financial support。
文摘Lithium-ion(Li-ion) battery and lithium-sulfur(Li-S) battery have attracted significant attention as promising components for large-scale energy storage because of high theoretical capacity of Li,excellent energy density or environmental friendness for two kinds of batteries.However,there still exist some respective obstacles for commercial applications,such as limited theoretical capacity,high cost and low conductivity of Li-ion cells or shuttle effect of lithium polysulfides of Li-S cells.As typical twodimensional materials,layered double hydroxides(LDHs) exhibit excellent potential in the field of energy storage due to facile tunability of composition,structure and morphology as well as convenient composite and strong catalytic properties.Consequently,various LDHs toward novel separators or interlayers,cathodes,anodes,and interesting catalytic templates are researched to resolve these challenges.In this review,the recent progress for LDHs applied in Li-ion batteries and Li-S batteries including the synthesis methods,designs and applications is presented and reviewed.Meanwhile,the existing challenges and future perspectives associated with material designs and practical applications of LDHs for these two classes of cells are discussed.WeWe hope that the review can attract more attention and inspire more profound researches toward the LDH-based electrochemical materials for energy storage.
文摘For several years now, electric vehicles (EVs) have been expected to become widely available in the micro-mobility field. However, the insufficiency of such vehicles’ battery-charging and discharging performance has limited their practical use. A hybrid energy storage system, which comprises a capacitor and battery, is a promising solution to this problem;however, to apply model-based designs, which are indispensable to embedded systems, such as the electronic control units used in EVs, a simple and accurate capacitor model is required. Within this framework, a lithium-ion capacitor (LIC) model is proposed, and its charging and discharging performances are evaluated against an actual LIC. The model corresponds accurately to the actual LIC, and the results indicate that the proposed LIC model will work well when used with Model-Based Design (MBD).
基金supported by the Basic Research Program of Shenzhen(No.JCYJ20190812161409163)the Basic and Applied Basic Research Program of Guangdong Province(No.2019A1515110531)the SIAT Innovation Program for Excellent Young Researchers。
文摘Separators are indispensable components of modern electrochemical energy storage devices such as lithium-ion batteries(LIBs).They perform the critical function of physically separating the electrodes to prevent short-circuits while permitting the ions to pass through.While conventional separators using polypropylene(PP) and polyethylene(PE) are prone to shrinkage and melting at relatively high temperatures(150℃ or above) causing short circuits and thermal runaway,separators made of thermally stable polyimides(PIs) are electrochemically stable and resistant to high temperatures,and possess good mechanical strength-making them a promising solution to the safety concerns of LIBs.In this review,the research progress on PI separators for use in LIBs is summarized with a special focus on molecular design and microstructural control.In view of the significant progress in advanced chemistries beyond LIBs,recent advances in PI-based membranes for applications in lithium-sulfur,lithium-metal,and solid-state batteries are also reviewed.Finally,practical issues are also discussed along with their prospects.
基金financially supported by the National Key R&D Program of China (No. 2019YFA0705104)Guangdong Province Science and Technology Department under Project (No. 2020A0505100014)。
文摘Developing high-performance lithium-ion batteries (LIBs) with high energy density, rate capability and long cycle life are essential for the ever-growing practical application. Among all battery components, the binder plays a key role in determining the preparation of electrodes and the improvement of battery performance, in spite of a low usage amount. The main function of binder is to bond the active material, conductive additive and current collector together and provide electron and ion channels to improve the kinetics of electrochemical reaction. With the ever-increasing requirement of high energy density by LIBs, technical challenges such as volume expansion and active material dissolution are attracting worldwide attentions, where binder is thought to provide a new solution.There are two main categories (organic solvent soluble binder and water-soluble binder) and abundant polar functional groups providing adhesion ability. It is of great significance to timely summarize the latest progress in battery binders and present the principles for designing novel binders with both robust binding interaction and outstanding electrode stabilization function. This review begins with an introduction of the binding mechanism and the related binding forces, including mechanical interlocking forces and interfacial forces. Then, we discussed four different strategies (the enhancement of binding force,the formation of three-dimensional (3D) network, the enhancement of conductivity and binders with special functions) for constructing ideal binder system in order to satisfy the specific demands of different batteries, such as LIBs and lithium–sulfur (Li–S) batteries. Finally, some prospective and promising directions of binder design are proposed based on the existing and emerging binders and guide the development of the next-generation LIBs.
文摘Lithium-ion batteries,first commercialized in 1991,have been thriving for the past 30 years and become an important basis for portable electronics and electric vehicles.However,this first generation of lithium-ion batteries built on the intercalation materials has limited energy density and can not meet the increased demand of various applications.Thus,a transition from intercalation to alloying chemistry for anodes is on call.Silicon,as the most attractive alloying anode material,has been on the research focus for next-generation highenergy density battery.Alloying mechanism benefits silicon a large capacity while brings silicon the challenge of volume expansion.This article discusses the structure design strategies to address the issues of large volume change and interface instability.
基金supported by the Key-Area Research and Development Program of Guangdong Province(Grant Nos.2019B090909001 and 2020B090920002)the National Natural Science Foundation of China(Grant Nos.51975218 and 51722504)+1 种基金Guangdong Science and Technology Plan Program(Grant No.2017KZ010105)Fundamental Research Funds for the Central Universities(Grant No.2018ZD31)。
文摘Electric vehicles(EVs)are globally undergoing rapid developments,and have great potentials to replace the traditional vehicles based on fossil fuels.Power-type lithium-ion batteries(LIBs)have been widely used for EVs,owing to high power densities,good charge/discharge stability,and long cycle life.The driving ranges and acceleration performances are gaining increasing concerns from customers,which depend highly on the power level of LIBs.With the increase in power outputs,rising heat generation significantly affects the battery performances,and in particular operation safety.Meanwhile,the cold-start performance is still an intractable problem under extreme conditions.These challenges put forward higher requirements for a dedicated battery thermal management system(BTMS).Compared to traditional BTMSs in EVs,the heat pipe-based BTMS has great application prospects owing to its compact structure,flexibility,low cost,and especially high thermal conductivity.Encompassing this topic,this review first introduces heat generation phenomena and temperature characteristics of LIBs.Multiple abuse conditions and thermal runaway issues are described afterward.Typical cooling and preheating methods for designing a BTMS are also discussed.More emphasis on this review is put on the use of various heat pipes for BTMSs to enhance the thermal performances of LIBs.For lack of wide application in actual EVs,more efforts should be made to extend the use of heat pipes for constructing an energy-efficient,cost-effective,and reliable BTMS to improve the performances and safety of EVs.
