Owing to the shortcomings of traditional electrode materials in alkalimetal-ion batteries(AIBs),such as limited reversible specific capacity,low power density,and poor cycling performance,it is particularly important ...Owing to the shortcomings of traditional electrode materials in alkalimetal-ion batteries(AIBs),such as limited reversible specific capacity,low power density,and poor cycling performance,it is particularly important to develop new electrode materials.Covalent organic frameworks(COFs)are crystalline porous polymers that incorporate organic building blocks into their periodic structures through dynamic covalent bonds.COFs are superior to organic materials because of their high designability,regular channels,and stable topology.Since the first report of D_(TP)-A_(NDI)-COF as a cathode material for lithium-ion batteries in 2015,research on COF electrode materials has made continuous progress and breakthroughs.This review briefly introduces the characteristics and current challenges associated with COF electrode materials.Furthermore,we summarize the basic reaction types and active sites according to the categories of covalent bonds,including B–O,C=N,C–N,and C=C.Finally,we emphasize the perspectives on basic structure and morphology design,dimension and size design,and conductivity improvement of COFs based on the latest progress in AIBs.We believe that this review provides important guidelines for the development of high-efficiency COF electrode materials and devices for AIBs.展开更多
Viologens known as a kind of promising negolyte materials for aqueous organic redox flow batteries,face a critical stability challenge due to the S_N2 nucleophilic attack by hydroxide ions(OH-)during the battery cycli...Viologens known as a kind of promising negolyte materials for aqueous organic redox flow batteries,face a critical stability challenge due to the S_N2 nucleophilic attack by hydroxide ions(OH-)during the battery cycling.In this work,a N-cyclic quaternary ammonium-grafted viologen molecule,viz.1,1'-bis(4,4'-dime thylpiperidiniumyl)-4,4'-bipyridinium tetrachloride((DBPPy)Cl_(4)),is developed by the molecular engineering strategy.The obtained(DBPPy)Cl_(4) molecule shows a decent solubility of 1.84 M and a redox potential of-0.52 V vs.Ag/AgCl,Experimental and theoretical results reveal that the grafted N-cyclic quaternary ammonium groups act as the steric hindrance to prevent nucleophilic attack by OH~-,increasing the alkali resistance of the electroactive molecule.The symmetrical battery with 0.50 M(DBPPy)Cl4shows negligible decay during the 13-day cycling test.As demonstration,the flow battery utilizing 1.0 M(DBPPy)Cl_(4) as the negolyte and 1-(1-oxyl-2,2',6,6'-tetramethylpiperidin-4-yl)-1'-(3-(trimethylammonio)propyl)-4,4'-bipyridinium trichloride as the posolyte exhibits a high capacity retention rate of 99.99%per cycle at 60 mA cm^(-2).展开更多
To develop emerging electrode materials and improve the performances of batteries,the machine learning techniques can provide insights to discover,design and develop battery new materials in high-throughput way.In thi...To develop emerging electrode materials and improve the performances of batteries,the machine learning techniques can provide insights to discover,design and develop battery new materials in high-throughput way.In this paper,two deep learning models are developed and trained with two feature groups extracted from the Materials Project datasets to predict the battery electrochemical performances including average voltage,specific capacity and specific energy.The deep learning models are trained with the multilayer perceptron as the core.The Bayesian optimization and Monte Carlo methods are applied to improve the prediction accuracy of models.Based on 10 types of ion batteries,the correlation coefficients are maintained above 0.9 compared to DFT calculation results and the mean absolute error of the prediction results for voltages of two models can reach 0.41 V and 0.20 V,respectively.The electrochemical performance prediction times for the two trained models on thousands of batteries are only 72.9 ms and 75.7 ms.Besides,the two deep learning models are applied to approach the screening of emerging electrode materials for sodium-ion and potassium-ion batteries.This work can contribute to a high-throughput computational method to accelerate the rational and fast materials discovery and design.展开更多
Owning various crystal structures and high theoretical capacity,metal tellurides are emerging as promising electrode materials for high-performance metal-ion batteries(MBs).Since metal telluride-based MBs are quite ne...Owning various crystal structures and high theoretical capacity,metal tellurides are emerging as promising electrode materials for high-performance metal-ion batteries(MBs).Since metal telluride-based MBs are quite new,fundamental issues raise regarding the energy storage mechanism and other aspects affecting electrochemical performance.Severe volume expansion,low intrinsic conductivity and slow ion diffusion kinetics jeopardize the performance of metal tellurides,so that rational design and engineering are crucial to circumvent these disadvantages.Herein,this review provides an in-depth discussion of recent investigations and progresses of metal tellurides,beginning with a critical discussion on the energy storage mechanisms of metal tellurides in various MBs.In the following,recent design and engineering strategies of metal tellurides,including morphology engineering,compositing,defect engineering and heterostructure construction,for high-performance MBs are summarized.The primary focus is to present a comprehensive understanding of the structural evolution based on the mechanism and corresponding effects of dimension control,composition,electron configuration and structural complexity on the electrochemical performance.In closing,outlooks and prospects for future development of metal tellurides are proposed.This work also highlights the promising directions of design and engineering strategies of metal tellurides with high performance and low cost.展开更多
Aqueous zinc(Zn)-ion batteries(AZIBs)have the potential to be used in massive energy storage owing to their low cost,eco-friendliness,safety,and good energy density.Significant research has been focused on enhancing t...Aqueous zinc(Zn)-ion batteries(AZIBs)have the potential to be used in massive energy storage owing to their low cost,eco-friendliness,safety,and good energy density.Significant research has been focused on enhancing the performance of AZIBs,but challenges persist.Vanadium-based oxides,known for their large interlayer spacing,are promising cathode materials.In this report,we synthesize Mg^(2+)-intercalated potassium vanadate(KVO)(MgKVO)via a single-step hydrothermal method and achieve a 12.2°Ainterlayer spacing.Mg^(2+) intercalation enhances the KVO performance,providing wide channels for Zn^(2+),which results in high capacity and ion diffusion.The combined action of K^(+) and Mg^(2+) intercalation enhances the electrical conductivity of MgKVO.This structural design endows MgKVO with excellent electrochemical performance.The AZIB with the MgKVO cathode delivers a high capacity of 457 mAh g^(-1) at 0.5 A g^(-1),excellent rate performance of 298 mAh g^(-1) at 5 A g^(-1),and outstanding cycling stability of 102%over 1300 cycles at 3 A g^(-1).Additionally,pseudocapacitance analysis reveals the high capacitance contribution and Zn^(2+)diffusion coefficient of MgKVO.Notably,ex-situ X-ray diffraction,X-ray photoelectron spectroscopy,and Raman analyses further demonstrate the Zn^(2+)insertion/extraction and Zn-ion storage mechanisms that occurred during cycling in the battery system.This study provides new insights into the intercalation of dual cations in vanadium oxides and offers new solutions for designing cathodes for high-capacity AZIBs.展开更多
Alkali metal-carbon dioxide(Li/Na/K-CO_(2))batteries are emerging electrochemical energy storage technologies in the context of the energy crisis and the urgent demand for carbon neutrality.Alkali metal-CO_(2) batteri...Alkali metal-carbon dioxide(Li/Na/K-CO_(2))batteries are emerging electrochemical energy storage technologies in the context of the energy crisis and the urgent demand for carbon neutrality.Alkali metal-CO_(2) batteries offer a new strategy for CO_(2) fixation and utilization,and thus has been receiving considerable attention in recent years.Considerable progress has been achieved since alkali metal-CO_(2) batteries were invented,especially in terms of development of new electrode materials,and yet,research is lacking on the underlying mechanisms of the systems.This is the first typical review focusing on the electrochemical mechanisms of metal-CO_(2) batteries that summarizes the current understanding of and provides insights into the thermodynamic reaction pathways,the kinetic characteristics,and the crucial factors determining the reaction mechanisms in alkali metal-CO_(2) batteries.The review starts with the fundamental concepts of alkali metal-CO_(2) batteries,followed by a comprehensive discussion of the working mechanisms on cathodes and anodes.Moreover,the operation mechanisms of state-of-the-art electrolytes,including liquid and(quasi-)solid-state electrolytes,are also described.Finally,we identify the unsolved problems in current alkali metal-CO_(2) batteries and propose potential topics for future research.展开更多
The ever-growing pursuit of high energy density batteries has triggered extensive efforts toward developing alkali metal(Li,Na,and K)battery(AMB)technologies owing to high theoretical capacities and low redox potentia...The ever-growing pursuit of high energy density batteries has triggered extensive efforts toward developing alkali metal(Li,Na,and K)battery(AMB)technologies owing to high theoretical capacities and low redox potentials of metallic anodes.Typically,for new battery systems,the electrolyte design is critical for realizing the battery electrochemistry of AMBs.Conventional electrolytes in alkali ion batteries are generally unsuitable for sustaining the stability owing to the hyper-reactivity and dendritic growth of alkali metals.In this review,we begin with the fundamentals of AMB electrolytes.Recent advancements in concentrated and fluorinated electrolytes,as well as functional electrolyte additives for boosting the stability of Li metal batteries,are summarized and discussed with a special focus on structure-composition-performance relationships.We then delve into the electrolyte formulations for Na-and K metal batteries,including those in which Na/K do not adhere to the Li-inherited paradigms.Finally,the challenges and the future research needs in advanced electrolytes for AMB are highlighted.This comprehensive review sheds light on the principles for the rational design of promising electrolytes and offers new inspirations for developing stable AMBs with high performance.展开更多
With the increasing demand for large-scale battery systems in electric vehicles（EVs） and smart renewable energy grids, organic materials including small molecules and polymers utilized as electrodes in rechargeable ...With the increasing demand for large-scale battery systems in electric vehicles（EVs） and smart renewable energy grids, organic materials including small molecules and polymers utilized as electrodes in rechargeable batteries have received increasing attraction. In recent years, two-dimensional（2D） organic materials possessing planar layered architecture exhibit optional chemical modification, high specific surface area as well as unique electrical/magnetic properties, which have been emerging as the promising functional materials for wide applications in optoelectronics, catalysis, sensing, etc. Integrating with high-density redox-active sites and hierarchical porous structure, significant achievements in 2D organic materials as cathode materials for alkali-metal-ion batteries have been witnessed. In this review, the recent progress in synthetic approaches, structure analyses, electrochemical characterizations of 2D organic materials as well as their application in alkali-metal-ion batteries containing lithium ion battery（LIB）, lithium sulfur battery（LSB）, lithium air battery（LAB） and sodium ion battery（SIB） are summarized systematically,and their current challenges including cycling stability and electron conductivity for cathode materials in battery fields are also discussed.展开更多
Rechargeable alkali metal-air batteries are considered as the most promising candidate for the power source of electric vehicles(EVs) due to their high energy density. However, the practical application of metal-air b...Rechargeable alkali metal-air batteries are considered as the most promising candidate for the power source of electric vehicles(EVs) due to their high energy density. However, the practical application of metal-air batteries is still challenging. In the past decade, many strategies have been purposed and explored, which promoted the development of metal-air batteries. The reaction mechanisms have been gradually clarified and catalysts have been rationally designed for air cathodes. In this review, we summarize the recent development of alkali metal-air batteries from four parts: metal anodes, electrolytes, air cathodes and reactant gases, wherein we highlight the important achievement in this filed. Finally problems and prospective are discussed towards the future development of alkali metal-air batteries.展开更多
Alkali metal ion batteries(AMIBs)are playing an irreplaceable part in the energy revolution,due to their intrinsic advantages of large capacity/power density and abundance of alkali metal ions in the earth’s crust.De...Alkali metal ion batteries(AMIBs)are playing an irreplaceable part in the energy revolution,due to their intrinsic advantages of large capacity/power density and abundance of alkali metal ions in the earth’s crust.Despite their great promise,the inborn deficiencies of commercial graphite and other anodes being researched so far call for the quest of better alternatives that exhibit all-round performance with the balance of energy/power density and cycling stability.Gallium-based materials,with impressive capacity utilization and self-healing ability,provide an anticipated solution to this conundrum.In this review,an overview on the recent progress of gallium-based anodes and their storage mechanism is presented.The current strategies used as engineering solutions to meet the scientific challenges ahead are discussed,in addition to the insightful outlook for possible future study.展开更多
Metal-ion batteries(MIBs),including alkali metal-ion(Li^(+),Na^(+),and K^(3)),multi-valent metal-ion(Zn^(2+),Mg^(2+),and Al^(3+)),metal-air,and metal-sulfur batteries,play an indispensable role in electrochemical ener...Metal-ion batteries(MIBs),including alkali metal-ion(Li^(+),Na^(+),and K^(3)),multi-valent metal-ion(Zn^(2+),Mg^(2+),and Al^(3+)),metal-air,and metal-sulfur batteries,play an indispensable role in electrochemical energy storage.However,the performance of MIBs is significantly influenced by numerous variables,resulting in multi-dimensional and long-term challenges in the field of battery research and performance enhancement.Machine learning(ML),with its capability to solve intricate tasks and perform robust data processing,is now catalyzing a revolutionary transformation in the development of MIB materials and devices.In this review,we summarize the utilization of ML algorithms that have expedited research on MIBs over the past five years.We present an extensive overview of existing algorithms,elucidating their details,advantages,and limitations in various applications,which encompass electrode screening,material property prediction,electrolyte formulation design,electrode material characterization,manufacturing parameter optimization,and real-time battery status monitoring.Finally,we propose potential solutions and future directions for the application of ML in advancing MIB development.展开更多
High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)M...High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.展开更多
Based on the density functional theory calculations,we have investigated the feasibility of two-dimensionalβ-GeS monolayer as high-performance anodes for alkali metal ion batteries.The results show that the electrica...Based on the density functional theory calculations,we have investigated the feasibility of two-dimensionalβ-GeS monolayer as high-performance anodes for alkali metal ion batteries.The results show that the electrical conductivity of β-GeS monolayer can be enhanced after adsorbing the alkali metal atoms owing to the semiconductor-to-metal transition.The low diffusion barriers of alkali metal atoms on the β-GeS surface indicate a rapid charge/discharge rate without metal clustering.Moreover,the low average open-circuit voltage(0.211 V)and a high theoretical capacity(1024 mAh·g^(-1))for Na suggest that theβ-GeS monolayer is a promising anode material for Na-ion batteries with high performance.展开更多
Alloyed based anode materials with high theoretical specific capacity and low reaction potential are considered to be highly potential high-energy density anode materials for alkali metal ion batteries(AMIBs).Thus,the...Alloyed based anode materials with high theoretical specific capacity and low reaction potential are considered to be highly potential high-energy density anode materials for alkali metal ion batteries(AMIBs).Thus,the design of alloyed based materials with high electrochemical performance has attracted great attention.Among the numerous characterization methods for guiding electrode materials design,in situ transmission electron microscopy(TEM)gradually plays an irreplaceable role due to its high temporal and spatial resolution in directly observing the change of morphology,crystal structure and element evolutions.Herein,we reviewed the two current research hotspots and mainly focused on the structure design of alloyed based electrode material under the guidance of in situ TEM.Specifically,various nanostructure designs of alloyed based electrode materials with guidance of in situ TEM were employed to solve the key scientific issues of the violent volume change during alloying/dealloying processes for enhanced electrochemical performances.Mainly through introducing buffer space in the electrode material to reduce volume change to improve structural stability,including porous structure(0 D),nanotube structure(1 D),simple hollow structure,yolk-shell structure and some hybrid hollow structures(3 D).Furthermore,the direct guidance of in situ TEM is expected for creating new opportunities to nextgeneration electrode material design for AMIBs.展开更多
Rechargeable aqueous metal-ion batteries(AMBs)have attracted extensive scientific and commercial interest due to their potential for cost-effective,highly safe,and scalable stationary energy storage.However,their limi...Rechargeable aqueous metal-ion batteries(AMBs)have attracted extensive scientific and commercial interest due to their potential for cost-effective,highly safe,and scalable stationary energy storage.However,their limited output voltage,inadequate energy density,and poor reversibility of ambiguous electrode reactions in aqueous electrolytes strongly limit their practical viability.This review aims to elucidate the challenges of existing AMBs from the material design to whole device applications.We summarize the emerging electrochemistry,fundamental properties,and key issues in interfacial behaviors of various classes of prevailing AMBs,including aqueous alkali metal-ion batteries and multivalent-ion batteries,and present an appraisal of recent advances for addressing the performance deficiency.Specifically,the progress of zinc-ion batteries is highlighted to provide a ubiquitous guideline for their commercialization in the grid-scale energy storage.Finally,we figure out the dominating general challenges for achieving high-performance AMBs,laying out a perspective for future breakthroughs.展开更多
The electrolyte is an essential component of a battery system since it is responsible for the conduction of ions between the electrodes.In the quest for cheaper alternatives to common organic electrolytes for lithium-...The electrolyte is an essential component of a battery system since it is responsible for the conduction of ions between the electrodes.In the quest for cheaper alternatives to common organic electrolytes for lithium-ion batteries(LIB),we formulated hybrid electrolytes comprising a mixture of Na,K,and Li alkaline salts with ethylene carbonate(EC),ethyl methyl carbonate(EMC),and lithium hexafluorophosphate(LiPF_(6)),giving a total salt concentration of 1.5 M;we determined their physicochemical properties and investigated their electrochemical behavior on a nickel cobalt aluminum oxide(NCA)cathode and graphite(Gr)anode.The electrolytes demonstrated a melting transition peak(T_(m)).eutectic behavior,and ionic conductivities(-13 mS cm^(-1))close to those of a commercial LIB electrolyte(SE,EC/EMC+1 M LiPF_(6))and activation energies of ca.3 kJ mol^(-1).The half-cell coin cells revealed high coulombic efficiency(99%),specific capacity(175 mAh g^(-1) at C/10),and capacity retention(92% for NaCF_(3)SO_(3))for the NCA cathode and a moderate performance(coulombic efficiency of 98%for 20 cycles)on the graphite anode after the formation of the SEI layer.The hybrid electrolytes were cycled at 25℃ in a Gr//NCA cell yielding specific capacities of ca.225 mAh g^(-1) at a C/5 rate,corroborating that the anion plays a key role and highlighting their potential for energy storage applications.展开更多
With the rapid development of electronics,electric vehicles,and grid energy storage stations,higher requirements have been put forward for advanced secondary batteries.Liquid metal/alloy electrodes have been considere...With the rapid development of electronics,electric vehicles,and grid energy storage stations,higher requirements have been put forward for advanced secondary batteries.Liquid metal/alloy electrodes have been considered as a promising development direction to achieve excellent electrochemical performance in metal-ion batteries,due to their specific advantages including the excellent electrode kinetics and self-healing ability against microstructural electrode damage.For conventional liquid batteries,high temperatures are needed to keep electrode liquid and ensure the high conductivity of molten salt electrolytes,which also brings the corrosion and safety issues.Ga-based metal/alloys,which can be operated at or near room temperature,are potential candidates to circumvent the above problems.In this review,the properties and advantages of Ga-based metal/alloys are summarized.Then,Ga-based liquid metal/alloys as anodes in various metal-ion batteries are reviewed in terms of their self-healing ability,battery configurations,working mechanisms,and so on.Furthermore,some views on the future development of Ga-based electrodes in batteries are provided.展开更多
Covalent organic frameworks(COFs)have emerged as promising electrode materials for rechargeable metal-ion batteries and have gained much attention in recent years due to their high specific surface area,inherent poros...Covalent organic frameworks(COFs)have emerged as promising electrode materials for rechargeable metal-ion batteries and have gained much attention in recent years due to their high specific surface area,inherent porosity,tunable molecular structure,robust framework,abundant active sites.Moreover,compared with inorganic materials and small organic molecules,COFs have the advantages of multi-electron transfer,short pathways,high cycling stability.Although great progress on COF-based electrodes has been made,the corresponding electrochemical performance is still far from satisfactory for practical applications.In this review,we first summarize the fundamental background of COFs,including the species of COFs(different active covalent bonds)and typical synthesis methods of COFs.Then,the key challenges and the latest research progress of COF-based cathodes and anodes for metal-ion batteries are reviewed,including Li-ion batteries,Na-ion batteries,K-ion batteries,Zn-ion batteries,et al.Moreover,the effective strategies to enhance electrochemical performance of COF-based electrodes are presented.Finally,this review also covers the typical superiorities of COFs used in energy devices,as well as providing some perspectives and outlooks in this field.We hope this review can provide fundamental guidance for the development of COFbased electrodes for metal-ion batteries in the further research.展开更多
基金This work was supported by the National Natural Science Foundation of China(grant no.22179063)Q.Z.gratefully acknowledges the funding support from the City University of Hong Kong(grant nos.9380117,7005620,and 7020040)and Hong Kong Institute for Advanced Study,City University of Hong Kong,Hong Kong,China.
文摘Owing to the shortcomings of traditional electrode materials in alkalimetal-ion batteries(AIBs),such as limited reversible specific capacity,low power density,and poor cycling performance,it is particularly important to develop new electrode materials.Covalent organic frameworks(COFs)are crystalline porous polymers that incorporate organic building blocks into their periodic structures through dynamic covalent bonds.COFs are superior to organic materials because of their high designability,regular channels,and stable topology.Since the first report of D_(TP)-A_(NDI)-COF as a cathode material for lithium-ion batteries in 2015,research on COF electrode materials has made continuous progress and breakthroughs.This review briefly introduces the characteristics and current challenges associated with COF electrode materials.Furthermore,we summarize the basic reaction types and active sites according to the categories of covalent bonds,including B–O,C=N,C–N,and C=C.Finally,we emphasize the perspectives on basic structure and morphology design,dimension and size design,and conductivity improvement of COFs based on the latest progress in AIBs.We believe that this review provides important guidelines for the development of high-efficiency COF electrode materials and devices for AIBs.
基金jointly supported by the Guangdong Major Project of Basic and Applied Basic Research (2023B0303000002)National Natural Science Foundation of China (22178126,22325802,U22A20417,22208110)+3 种基金Guangdong Basic and Applied Basic Research Foundation (2023B1515120005)Science and Technology Program of Guangzhou (2023B03J1281,2023A04J1357)China Postdoctoral Science Foundation (2023T160223)the State Key Laboratory of Pulp and Paper Engineering (2023ZD03)。
文摘Viologens known as a kind of promising negolyte materials for aqueous organic redox flow batteries,face a critical stability challenge due to the S_N2 nucleophilic attack by hydroxide ions(OH-)during the battery cycling.In this work,a N-cyclic quaternary ammonium-grafted viologen molecule,viz.1,1'-bis(4,4'-dime thylpiperidiniumyl)-4,4'-bipyridinium tetrachloride((DBPPy)Cl_(4)),is developed by the molecular engineering strategy.The obtained(DBPPy)Cl_(4) molecule shows a decent solubility of 1.84 M and a redox potential of-0.52 V vs.Ag/AgCl,Experimental and theoretical results reveal that the grafted N-cyclic quaternary ammonium groups act as the steric hindrance to prevent nucleophilic attack by OH~-,increasing the alkali resistance of the electroactive molecule.The symmetrical battery with 0.50 M(DBPPy)Cl4shows negligible decay during the 13-day cycling test.As demonstration,the flow battery utilizing 1.0 M(DBPPy)Cl_(4) as the negolyte and 1-(1-oxyl-2,2',6,6'-tetramethylpiperidin-4-yl)-1'-(3-(trimethylammonio)propyl)-4,4'-bipyridinium trichloride as the posolyte exhibits a high capacity retention rate of 99.99%per cycle at 60 mA cm^(-2).
基金supported by the National Natural Science Foundation of China(No.52102470).
文摘To develop emerging electrode materials and improve the performances of batteries,the machine learning techniques can provide insights to discover,design and develop battery new materials in high-throughput way.In this paper,two deep learning models are developed and trained with two feature groups extracted from the Materials Project datasets to predict the battery electrochemical performances including average voltage,specific capacity and specific energy.The deep learning models are trained with the multilayer perceptron as the core.The Bayesian optimization and Monte Carlo methods are applied to improve the prediction accuracy of models.Based on 10 types of ion batteries,the correlation coefficients are maintained above 0.9 compared to DFT calculation results and the mean absolute error of the prediction results for voltages of two models can reach 0.41 V and 0.20 V,respectively.The electrochemical performance prediction times for the two trained models on thousands of batteries are only 72.9 ms and 75.7 ms.Besides,the two deep learning models are applied to approach the screening of emerging electrode materials for sodium-ion and potassium-ion batteries.This work can contribute to a high-throughput computational method to accelerate the rational and fast materials discovery and design.
基金supported by the International Collaboration Program of Jilin Provincial Department of Science and Technology,China(20230402051GH)the National Natural Science Foundation of China(51932003,51902050)+2 种基金the Open Project Program of Key Laboratory of Preparation and Application of Environmental friendly Materials(Jilin Normal University)of Ministry of China(2021006)the Fundamental Research Funds for the Central Universities JLU“Double-First Class”Discipline for Materials Science&Engineering。
文摘Owning various crystal structures and high theoretical capacity,metal tellurides are emerging as promising electrode materials for high-performance metal-ion batteries(MBs).Since metal telluride-based MBs are quite new,fundamental issues raise regarding the energy storage mechanism and other aspects affecting electrochemical performance.Severe volume expansion,low intrinsic conductivity and slow ion diffusion kinetics jeopardize the performance of metal tellurides,so that rational design and engineering are crucial to circumvent these disadvantages.Herein,this review provides an in-depth discussion of recent investigations and progresses of metal tellurides,beginning with a critical discussion on the energy storage mechanisms of metal tellurides in various MBs.In the following,recent design and engineering strategies of metal tellurides,including morphology engineering,compositing,defect engineering and heterostructure construction,for high-performance MBs are summarized.The primary focus is to present a comprehensive understanding of the structural evolution based on the mechanism and corresponding effects of dimension control,composition,electron configuration and structural complexity on the electrochemical performance.In closing,outlooks and prospects for future development of metal tellurides are proposed.This work also highlights the promising directions of design and engineering strategies of metal tellurides with high performance and low cost.
基金supported by the National Research Foundation of Korea(NRF)grant sponsored by the Korean government(MSIP)(No.2018R1A6A1A03025708).
文摘Aqueous zinc(Zn)-ion batteries(AZIBs)have the potential to be used in massive energy storage owing to their low cost,eco-friendliness,safety,and good energy density.Significant research has been focused on enhancing the performance of AZIBs,but challenges persist.Vanadium-based oxides,known for their large interlayer spacing,are promising cathode materials.In this report,we synthesize Mg^(2+)-intercalated potassium vanadate(KVO)(MgKVO)via a single-step hydrothermal method and achieve a 12.2°Ainterlayer spacing.Mg^(2+) intercalation enhances the KVO performance,providing wide channels for Zn^(2+),which results in high capacity and ion diffusion.The combined action of K^(+) and Mg^(2+) intercalation enhances the electrical conductivity of MgKVO.This structural design endows MgKVO with excellent electrochemical performance.The AZIB with the MgKVO cathode delivers a high capacity of 457 mAh g^(-1) at 0.5 A g^(-1),excellent rate performance of 298 mAh g^(-1) at 5 A g^(-1),and outstanding cycling stability of 102%over 1300 cycles at 3 A g^(-1).Additionally,pseudocapacitance analysis reveals the high capacitance contribution and Zn^(2+)diffusion coefficient of MgKVO.Notably,ex-situ X-ray diffraction,X-ray photoelectron spectroscopy,and Raman analyses further demonstrate the Zn^(2+)insertion/extraction and Zn-ion storage mechanisms that occurred during cycling in the battery system.This study provides new insights into the intercalation of dual cations in vanadium oxides and offers new solutions for designing cathodes for high-capacity AZIBs.
基金support from the National Natural Science Foundation of China (52072257)the National Key Research and Development Program of China (2019YFE0118800).
文摘Alkali metal-carbon dioxide(Li/Na/K-CO_(2))batteries are emerging electrochemical energy storage technologies in the context of the energy crisis and the urgent demand for carbon neutrality.Alkali metal-CO_(2) batteries offer a new strategy for CO_(2) fixation and utilization,and thus has been receiving considerable attention in recent years.Considerable progress has been achieved since alkali metal-CO_(2) batteries were invented,especially in terms of development of new electrode materials,and yet,research is lacking on the underlying mechanisms of the systems.This is the first typical review focusing on the electrochemical mechanisms of metal-CO_(2) batteries that summarizes the current understanding of and provides insights into the thermodynamic reaction pathways,the kinetic characteristics,and the crucial factors determining the reaction mechanisms in alkali metal-CO_(2) batteries.The review starts with the fundamental concepts of alkali metal-CO_(2) batteries,followed by a comprehensive discussion of the working mechanisms on cathodes and anodes.Moreover,the operation mechanisms of state-of-the-art electrolytes,including liquid and(quasi-)solid-state electrolytes,are also described.Finally,we identify the unsolved problems in current alkali metal-CO_(2) batteries and propose potential topics for future research.
基金financial support from Natural Science Foundation of Inner Mongolia(No.2019MS05068)Inner Mongolia scientific and technological achievements transformation project(CGZH2018132)+3 种基金Inner Mongolia major science and technology project(2020ZD0024)the research project of Inner Mongolia Electric Power(Group)Co.,Ltd for post-doctoral studies,the Hong Kong Polytechnic University start-up funding,National Nature Science Foundation of China(No.51872157)Shenzhen Key Laboratory on Power Battery Safety Research(No.ZDSYS201707271615073)financial support from the Australian Research Council(DE190100445).
文摘The ever-growing pursuit of high energy density batteries has triggered extensive efforts toward developing alkali metal(Li,Na,and K)battery(AMB)technologies owing to high theoretical capacities and low redox potentials of metallic anodes.Typically,for new battery systems,the electrolyte design is critical for realizing the battery electrochemistry of AMBs.Conventional electrolytes in alkali ion batteries are generally unsuitable for sustaining the stability owing to the hyper-reactivity and dendritic growth of alkali metals.In this review,we begin with the fundamentals of AMB electrolytes.Recent advancements in concentrated and fluorinated electrolytes,as well as functional electrolyte additives for boosting the stability of Li metal batteries,are summarized and discussed with a special focus on structure-composition-performance relationships.We then delve into the electrolyte formulations for Na-and K metal batteries,including those in which Na/K do not adhere to the Li-inherited paradigms.Finally,the challenges and the future research needs in advanced electrolytes for AMB are highlighted.This comprehensive review sheds light on the principles for the rational design of promising electrolytes and offers new inspirations for developing stable AMBs with high performance.
基金the financial support from the 973 Programs of China(2013CBA01602)NSFC for Excellent Youth Scholars(51722304)+4 种基金NSFC(21720102002,21574080 and 61306018)Shanghai Committee of Science and Technology(15JC1490500,16JC1400703)and Open Project Program of the State Key Laboratory of Supramolecular Structure and Materials(sklssm201732,Jilin University)State Key Laboratory of Inorganic Synthesis and Preparative Chemistry(2016-08,Jilin University)State Key Laboratory for Mechanical Behavior of Materials(20161803,Xi’an Jiaotong University)
文摘With the increasing demand for large-scale battery systems in electric vehicles（EVs） and smart renewable energy grids, organic materials including small molecules and polymers utilized as electrodes in rechargeable batteries have received increasing attraction. In recent years, two-dimensional（2D） organic materials possessing planar layered architecture exhibit optional chemical modification, high specific surface area as well as unique electrical/magnetic properties, which have been emerging as the promising functional materials for wide applications in optoelectronics, catalysis, sensing, etc. Integrating with high-density redox-active sites and hierarchical porous structure, significant achievements in 2D organic materials as cathode materials for alkali-metal-ion batteries have been witnessed. In this review, the recent progress in synthetic approaches, structure analyses, electrochemical characterizations of 2D organic materials as well as their application in alkali-metal-ion batteries containing lithium ion battery（LIB）, lithium sulfur battery（LSB）, lithium air battery（LAB） and sodium ion battery（SIB） are summarized systematically,and their current challenges including cycling stability and electron conductivity for cathode materials in battery fields are also discussed.
基金supported by NSFC(21473094 and21421001)MOE Innovation Team(IRT13022) in China
文摘Rechargeable alkali metal-air batteries are considered as the most promising candidate for the power source of electric vehicles(EVs) due to their high energy density. However, the practical application of metal-air batteries is still challenging. In the past decade, many strategies have been purposed and explored, which promoted the development of metal-air batteries. The reaction mechanisms have been gradually clarified and catalysts have been rationally designed for air cathodes. In this review, we summarize the recent development of alkali metal-air batteries from four parts: metal anodes, electrolytes, air cathodes and reactant gases, wherein we highlight the important achievement in this filed. Finally problems and prospective are discussed towards the future development of alkali metal-air batteries.
基金the National Key R&D Research Program of China(Grant No.2018YFB0905400)the National Natural Science Foundation of China(Grant Nos.51872277,21606003,51902062,51972067,51802044,51925207 and U1910210)+2 种基金the Fundamental Research Funds for the Central Universities(WK2060140026)the DNL cooperation Fund,CAS(DNL180310)the Guangdong Natural Science Funds for Distinguished Young Scholar(Grant No.2019B151502039)。
文摘Alkali metal ion batteries(AMIBs)are playing an irreplaceable part in the energy revolution,due to their intrinsic advantages of large capacity/power density and abundance of alkali metal ions in the earth’s crust.Despite their great promise,the inborn deficiencies of commercial graphite and other anodes being researched so far call for the quest of better alternatives that exhibit all-round performance with the balance of energy/power density and cycling stability.Gallium-based materials,with impressive capacity utilization and self-healing ability,provide an anticipated solution to this conundrum.In this review,an overview on the recent progress of gallium-based anodes and their storage mechanism is presented.The current strategies used as engineering solutions to meet the scientific challenges ahead are discussed,in addition to the insightful outlook for possible future study.
基金supported by the National Natural Science Foundation of China(52203364,52188101,52020105010)the National Key R&D Program of China(2021YFB3800300,2022YFB3803400)+2 种基金the Strategic Priority Research Program of Chinese Academy of Science(XDA22010602)the China Postdoctoral Science Foundation(2022M713214)the China National Postdoctoral Program for Innovative Talents(BX2021321)。
文摘Metal-ion batteries(MIBs),including alkali metal-ion(Li^(+),Na^(+),and K^(3)),multi-valent metal-ion(Zn^(2+),Mg^(2+),and Al^(3+)),metal-air,and metal-sulfur batteries,play an indispensable role in electrochemical energy storage.However,the performance of MIBs is significantly influenced by numerous variables,resulting in multi-dimensional and long-term challenges in the field of battery research and performance enhancement.Machine learning(ML),with its capability to solve intricate tasks and perform robust data processing,is now catalyzing a revolutionary transformation in the development of MIB materials and devices.In this review,we summarize the utilization of ML algorithms that have expedited research on MIBs over the past five years.We present an extensive overview of existing algorithms,elucidating their details,advantages,and limitations in various applications,which encompass electrode screening,material property prediction,electrolyte formulation design,electrode material characterization,manufacturing parameter optimization,and real-time battery status monitoring.Finally,we propose potential solutions and future directions for the application of ML in advancing MIB development.
基金supported by the National Natural Science Foundation of China(52162030)the Yunnan Major Scientific and Technological Projects(202202AG050003)+4 种基金the Key Research and Development Program of Yunnan Province(202103AA080019)the Scientific Research Foundation of Kunming University of Science and Technology(20220122)the Graduate Student Top Innovative Talent Program of Kunming University of Science and Technology(CA23107M139A)the Analysis and Testing Foundation of Kunming University of Science and Technology(2023T20220122)the Shenzhen Science and Technology Program(KCXST20221021111201003)。
文摘High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.
基金Project supported by the the National Natural Science Foundation of China(Grant Nos.52062035 and 51861023)the Major Discipline Academic and Technical Leaders Training Program of Jiangxi Province,China(Grant No.20213BCJ22056).
文摘Based on the density functional theory calculations,we have investigated the feasibility of two-dimensionalβ-GeS monolayer as high-performance anodes for alkali metal ion batteries.The results show that the electrical conductivity of β-GeS monolayer can be enhanced after adsorbing the alkali metal atoms owing to the semiconductor-to-metal transition.The low diffusion barriers of alkali metal atoms on the β-GeS surface indicate a rapid charge/discharge rate without metal clustering.Moreover,the low average open-circuit voltage(0.211 V)and a high theoretical capacity(1024 mAh·g^(-1))for Na suggest that theβ-GeS monolayer is a promising anode material for Na-ion batteries with high performance.
基金supported by the National Natural Science Foundation of China(No.51621001)the National Key Research and Development Program of China(No.2016YFA0202604)Key Laboratory of Resource Chemistry,Ministry of Education Joint International Research Laboratory of Resource Chemistry and the open fund from Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion(No.2018TP1037-202005)。
文摘Alloyed based anode materials with high theoretical specific capacity and low reaction potential are considered to be highly potential high-energy density anode materials for alkali metal ion batteries(AMIBs).Thus,the design of alloyed based materials with high electrochemical performance has attracted great attention.Among the numerous characterization methods for guiding electrode materials design,in situ transmission electron microscopy(TEM)gradually plays an irreplaceable role due to its high temporal and spatial resolution in directly observing the change of morphology,crystal structure and element evolutions.Herein,we reviewed the two current research hotspots and mainly focused on the structure design of alloyed based electrode material under the guidance of in situ TEM.Specifically,various nanostructure designs of alloyed based electrode materials with guidance of in situ TEM were employed to solve the key scientific issues of the violent volume change during alloying/dealloying processes for enhanced electrochemical performances.Mainly through introducing buffer space in the electrode material to reduce volume change to improve structural stability,including porous structure(0 D),nanotube structure(1 D),simple hollow structure,yolk-shell structure and some hybrid hollow structures(3 D).Furthermore,the direct guidance of in situ TEM is expected for creating new opportunities to nextgeneration electrode material design for AMIBs.
基金supported by National Key Research and Development Program of China(2022YFB2404500)Shenzhen Outstanding Talents Training Fund。
文摘Rechargeable aqueous metal-ion batteries(AMBs)have attracted extensive scientific and commercial interest due to their potential for cost-effective,highly safe,and scalable stationary energy storage.However,their limited output voltage,inadequate energy density,and poor reversibility of ambiguous electrode reactions in aqueous electrolytes strongly limit their practical viability.This review aims to elucidate the challenges of existing AMBs from the material design to whole device applications.We summarize the emerging electrochemistry,fundamental properties,and key issues in interfacial behaviors of various classes of prevailing AMBs,including aqueous alkali metal-ion batteries and multivalent-ion batteries,and present an appraisal of recent advances for addressing the performance deficiency.Specifically,the progress of zinc-ion batteries is highlighted to provide a ubiquitous guideline for their commercialization in the grid-scale energy storage.Finally,we figure out the dominating general challenges for achieving high-performance AMBs,laying out a perspective for future breakthroughs.
文摘The electrolyte is an essential component of a battery system since it is responsible for the conduction of ions between the electrodes.In the quest for cheaper alternatives to common organic electrolytes for lithium-ion batteries(LIB),we formulated hybrid electrolytes comprising a mixture of Na,K,and Li alkaline salts with ethylene carbonate(EC),ethyl methyl carbonate(EMC),and lithium hexafluorophosphate(LiPF_(6)),giving a total salt concentration of 1.5 M;we determined their physicochemical properties and investigated their electrochemical behavior on a nickel cobalt aluminum oxide(NCA)cathode and graphite(Gr)anode.The electrolytes demonstrated a melting transition peak(T_(m)).eutectic behavior,and ionic conductivities(-13 mS cm^(-1))close to those of a commercial LIB electrolyte(SE,EC/EMC+1 M LiPF_(6))and activation energies of ca.3 kJ mol^(-1).The half-cell coin cells revealed high coulombic efficiency(99%),specific capacity(175 mAh g^(-1) at C/10),and capacity retention(92% for NaCF_(3)SO_(3))for the NCA cathode and a moderate performance(coulombic efficiency of 98%for 20 cycles)on the graphite anode after the formation of the SEI layer.The hybrid electrolytes were cycled at 25℃ in a Gr//NCA cell yielding specific capacities of ca.225 mAh g^(-1) at a C/5 rate,corroborating that the anion plays a key role and highlighting their potential for energy storage applications.
基金The authors gratefully acknowledge financial support by the Key Research and Development Program of Shandong Province(No.2021ZLGX01)the support of Taishan Scholar Foundation of Shandong Province.
文摘With the rapid development of electronics,electric vehicles,and grid energy storage stations,higher requirements have been put forward for advanced secondary batteries.Liquid metal/alloy electrodes have been considered as a promising development direction to achieve excellent electrochemical performance in metal-ion batteries,due to their specific advantages including the excellent electrode kinetics and self-healing ability against microstructural electrode damage.For conventional liquid batteries,high temperatures are needed to keep electrode liquid and ensure the high conductivity of molten salt electrolytes,which also brings the corrosion and safety issues.Ga-based metal/alloys,which can be operated at or near room temperature,are potential candidates to circumvent the above problems.In this review,the properties and advantages of Ga-based metal/alloys are summarized.Then,Ga-based liquid metal/alloys as anodes in various metal-ion batteries are reviewed in terms of their self-healing ability,battery configurations,working mechanisms,and so on.Furthermore,some views on the future development of Ga-based electrodes in batteries are provided.
基金the National Natural Science Foundation of China(No.51872186)Project funded by China Postdoctoral Science Foundation(No.2021M702316)Guangdong Basic and Applied Basic Research Foundation(No.2020A1515110999).
文摘Covalent organic frameworks(COFs)have emerged as promising electrode materials for rechargeable metal-ion batteries and have gained much attention in recent years due to their high specific surface area,inherent porosity,tunable molecular structure,robust framework,abundant active sites.Moreover,compared with inorganic materials and small organic molecules,COFs have the advantages of multi-electron transfer,short pathways,high cycling stability.Although great progress on COF-based electrodes has been made,the corresponding electrochemical performance is still far from satisfactory for practical applications.In this review,we first summarize the fundamental background of COFs,including the species of COFs(different active covalent bonds)and typical synthesis methods of COFs.Then,the key challenges and the latest research progress of COF-based cathodes and anodes for metal-ion batteries are reviewed,including Li-ion batteries,Na-ion batteries,K-ion batteries,Zn-ion batteries,et al.Moreover,the effective strategies to enhance electrochemical performance of COF-based electrodes are presented.Finally,this review also covers the typical superiorities of COFs used in energy devices,as well as providing some perspectives and outlooks in this field.We hope this review can provide fundamental guidance for the development of COFbased electrodes for metal-ion batteries in the further research.
