Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_...Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_(2)(PO_(4))_(3)(LVP@C)nanoparticles on carbon nanofibers(CNFs)has been achieved by an electrospinning technique followed by calcination.The protective carbon coating prevents the aggregation of the LVP nanoparticles and suppresses V dissolution by preventing direct contact with aqueous electrolytes.The CNFs derived from the electrospun nanofibers provide a 3D network to increase the electronic conductivity of the LVP electrode,and the LVP@C-CNF hybrid film can be directly used as a freestanding cathode for zinc-ion batteries without adding conductive additives and binders.A mechanism for the formation of a uniform and continuous carbon coating has been proposed.This nanostructure,combined with the uniform and intact carbon coverage,significantly increases the electronic conductivity.This LVP@C-CNF freestanding electrode has an excellent rate capability(47.3%retention at 2 C)and cycling stability(61.2%retention after 100 cycles)within the voltage range 0.6 V to 1.95 V and is highly suitable for zinc-ion battery applications.展开更多
A novel trace nickel(Ni)doped tungsten(W)matrix with coated Ni on W grains was prepared by powder metallurgy method.The introduction of Ni can inhibit the reaction between W and barium-calcium aluminates(Ba-Ca alumina...A novel trace nickel(Ni)doped tungsten(W)matrix with coated Ni on W grains was prepared by powder metallurgy method.The introduction of Ni can inhibit the reaction between W and barium-calcium aluminates(Ba-Ca aluminates)during the impregnation process of the matrix.After cathode activation,the surface Ba:O molar ratio is 0.88:1.00,much higher than the Ba dispenser cathode without Ni doping.The XPS results of the cathode surface showed that the metallic Ba appeared on the activated cathode surface,forming dipoles with oxygen,and effectively reducing the cathode surface work function.The pulse electron emission current density at 1100℃_(b)(brightness temperature)was 18.26 A/cm^(2),and the calculated work function was 1.97 eV.It has a low evaporation rate and the accelerated lifetime test predict a lifetime of over 160000 h.First-principles calculations showed that the charge transfer and dipole moment in the NiW-BaO system were both increased compared to the Ba dispenser cathode,thus improving the emission performance of the Ni-W mixed matrix cathode.展开更多
Long-life energy storage batteries are integral to energy storage systems and electric vehicles,with lithium-ion batteries(LIBs)currently being the preferred option for extended usage-life energy storage.To further ex...Long-life energy storage batteries are integral to energy storage systems and electric vehicles,with lithium-ion batteries(LIBs)currently being the preferred option for extended usage-life energy storage.To further extend the life span of LIBs,it is essential to intensify investments in battery design,manufacturing processes,and the advancement of ancillary materials.The pursuit of long durability introduces new challenges for battery energy density.The advent of electrode material offers effective support in enhancing the battery’s long-duration performance.Often underestimated as part of the cathode composition,the binder plays a pivotal role in the longevity and electrochemical performance of the electrode.Maintaining the mechanical integrity of the electrode through judicious binder design is a fundamental requirement for achieving consistent long-life cycles and high energy density.This paper primarily concentrates on the commonly employed cathode systems in lithium-ion batteries,elucidates the significance of binders for both,discusses the application status,strengths,and weaknesses of novel binders,and ultimately puts forth corresponding optimization strategies.It underscores the critical function of binders in enhancing battery performance and advancing the sustainable development of lithium-ion batteries,aiming to offer fresh insights and perspectives for the design of high-performance LIBs.展开更多
Layered transition metal oxide cathode materials have garnered increasing attention for sodium-ion batteries(SIBs).However,they are plagued by the Jahn-Teller distortion of MnO6,Na^(+)/vacancy ordering,and irreversibl...Layered transition metal oxide cathode materials have garnered increasing attention for sodium-ion batteries(SIBs).However,they are plagued by the Jahn-Teller distortion of MnO6,Na^(+)/vacancy ordering,and irreversible lattice oxygen loss,which collectively lead to capacity fading and voltage decay.Herein,we report a P2-type material,Na_(0.67)Ni_(0.3)Mn_(0.6)Li_(0.09)Sn_(0.01)O_(2)(NNMO-Li0.09Sn0.01),modified with two closed-shell dopants(i.e.,Li^(+)and Sn^(4+)).Benefiting from the unique electronic configurations of closed-shell ions,NNMO-Li0.09Sn0.01 exhibits enhanced structural and electrochemical stability.Specifically,the incorporation of Li^(+)increases the Mn^(4+)/Mn3+ratio,thereby mitigating Jahn-Teller distortion during(de)sodiation process.In addition,Li^(+)disrupts the Ni/Mn ordering in the transition metal layer,suppressing Na^(+)/vacancy ordering.Meanwhile,the introduction of Sn^(4+)forms stronger Sn-O bonds(548 kJ mol-1),thereby enhancing the bonding strength between neighboring transition metal ions and surrounding oxygen atoms,effectively reducing oxygen loss during cycling.NNMO-Li0.09Sn0.01 exhibits significantly improved cycling stability,delivering a specific capacity of 90.3 mAh g^(-1)with 62.9%capacity retention after 50 cycles at 0.1 C(1 C=200 mA g^(-1)),along with 90.3%voltage retention.This substitution strategy based on closed-shell ions offers a viable approach for enhancing the structural stability of wide-voltage layered oxide cathodes.展开更多
Co-free Li-rich Li_(1.2)Ni_(0.2)Mn_(0.6)O_(2)(LR)cathode shows the highest working capacity that can be applied to high-energy density Li-ion batteries(LIBs).However,poor cycle stability and voltage decay caused by ph...Co-free Li-rich Li_(1.2)Ni_(0.2)Mn_(0.6)O_(2)(LR)cathode shows the highest working capacity that can be applied to high-energy density Li-ion batteries(LIBs).However,poor cycle stability and voltage decay caused by phase transition are always hindering its further development.Herein,a novel medium-entropy Li-rich Mn-based cathode material(LRMEF)was synthesized via a simple sol-gel method.The introduction of multivalent ions(Al^(3+)/Cu^(2+)doping at Mn sites and F−doping at O sites)effectively mitigates the Jahn-Teller distortion of Mn ions and suppresses oxygen release.High-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)images confirm that this synergistic doping strategy induces the in-situ formation of an approximately 3 nm-thick spinel surface layer,which significantly enhances structural stability and ion diffusion kinetics.Besides,a series of in-situ/ex-situ characterization methods and density functional theory(DFT)calculations have been carried out to fundamentally shed light on the optimized structure-activity relationship and reaction mechanism.As a result,the LR material with entropy regulation and anion doping exhibits excellent cycling stability(189.2 mAh g^(−1)at 1 C with 84%capacity retention after 300 cycles),rate performance(164.1 mAh g^(−1)at 5 C),and voltage retention(82.7%at 1 C after 300 cycles),demonstrating great application prospects in future high-energy-density LIBs.展开更多
The high voltage of Li||LiCoO_(2) battery can increase the energy density.However,the cycling performance associated with cathode structural stability remains challenging.To address this question,we proposed an electr...The high voltage of Li||LiCoO_(2) battery can increase the energy density.However,the cycling performance associated with cathode structural stability remains challenging.To address this question,we proposed an electrolyte strategy for improving the performance of 4.6 V Li||LiCoO_(2) battery by using trimethylsilyl isocyanate(TMIS)as electrolyte additive.The trimethylsilyl group of TMIS can trap HF while the isocyanate group brings polyamide components to the CEI and the SEI.By the synergistic action,the Co3+dissolution problem of the LiCoO_(2) cathode was effectively curbed.Furthermore,TMIS regulates the construction of anion-dominated LiF-rich SEI by influencing the solvation structure of Li+.As expected,the 4.6 V Li||LiCoO_(2) battery with TMIS retains 77.9% initial capacity after 200 cycles at 0.5 C.展开更多
The implementation of multifunctional application scenarios for mobile terminal devices has increased the energy density requirements of batteries.Increasing the charging voltage can rapidly increase the specific capa...The implementation of multifunctional application scenarios for mobile terminal devices has increased the energy density requirements of batteries.Increasing the charging voltage can rapidly increase the specific capacity of layered transition metal oxides;however,it also exacerbates the release of lattice oxygen and the contraction of the unit cell.Ternary materials are designed in a secondary particle state to meet the requirements of power battery applications.Therefore,to create ternary materials that can operate under ultrahigh voltages,attention should be given to both surface modification and particle integrity maintenance.By utilizing elemental selenium(Se)with a low melting point,easy sublimation,and multiple variable valence states,deep grain boundary modification was implemented inside the particles.The performance of the cathode material was evaluated through pouch cells,and the improvement mechanism was explored through molecular dynamics simulation calculations.Under the protection of a three-dimensional Se-rich modified layer,LiNi_(1/3)Co_(1/3)Mn_(1/3)O_(2)achieved stable operation at ultrahigh voltages(4.6 V vs.Li/Li^(+));a sacrificial protection mechanism based on the chronic decomposition of the Se-rich layer was proposed to explain the efficacy of Se modification in stabilizing ternary materials.This deep grain boundary modification based on elemental Se provides a new solution for the ultrahigh-voltage operation of transition metal oxides and provides a scientific basis and technical support for solving the interface contact problem of all-solid-state batteries.展开更多
Lithium manganese silicate(Li-Mn-Si-O)cathodes are key components of lithium-ion batteries,and their physical and mechanical properties are strongly influenced by their underlying crystal structures.In this study,a ra...Lithium manganese silicate(Li-Mn-Si-O)cathodes are key components of lithium-ion batteries,and their physical and mechanical properties are strongly influenced by their underlying crystal structures.In this study,a range of machine learning(ML)algorithms were developed and compared to predict the crystal systems of Li-Mn-Si-O cathode materials using density functional theory(DFT)data obtained from the Materials Project database.The dataset comprised 211 compositions characterized by key descriptors,including formation energy,energy above the hull,bandgap,atomic site number,density,and unit cell volume.These features were utilized to classify the materials into monoclinic(0)and triclinic(1)crystal systems.A comprehensive comparison of various classification algorithms including Decision Tree,Random Forest,XGBoost,Support VectorMachine,k-Nearest Neighbor,Stochastic Gradient Descent,Gaussian Naive Bayes,Gaussian Process,and Artificial Neural Network(ANN)was conducted.Among these,the optimized ANN architecture(6–14-14-14-1)exhibited the highest predictive performance,achieving an accuracy of 95.3%,aMatthews correlation coefficient(MCC)of 0.894,and an F-score of 0.963,demonstrating excellent consistency with DFT-predicted crystal structures.Meanwhile,RandomForest and Gaussian Processmodels also exhibited reliable and consistent predictive capability,indicating their potential as complementary approaches,particularly when data are limited or computational efficiency is required.This comparative framework provides valuable insights into model selection for crystal system classification in complex cathode materials.展开更多
Carbon-based air cathodes offer low cost,high electrical conductivity,and structural tunability.However,they suffer from limited catalytic activity and inefficient gas transport,and they typically rely on noble metal ...Carbon-based air cathodes offer low cost,high electrical conductivity,and structural tunability.However,they suffer from limited catalytic activity and inefficient gas transport,and they typically rely on noble metal additives or complex multilayer configurations.To tackle these issues,this study devised a self-activated integrated carbon-based air cathode.By integrating in situ catalytic site construction with structural optimization,the strategy not only induces the formation of oxygen functional groups(─C─OH,─C═O,─COOH),hierarchical pores,and uniformly distributed active sites,but also establishes a favorable electronic and mass-transport environment.Furthermore,the roll-pressing-based integrated design streamlines electrode construction,reinforces interfacial bonding,and significantly enhances mechanical stability.Density functional theory(DFT)calculations show that oxygen functional groups initiate hydrogen bonding interaction and promote charge enrichment,which improves the activity of the cathode and facilitates intermediate adsorption/desorption in oxygen reduction and evolution reactions processes.As a result,the integrated air cathode-based rechargeable zinc-air batteries(RZABs)achieve a high specific capacity of 811 mAh g^(-1).It also performs well in quasi-solid-state RZABs and silicon-air batteries systems across a wide temperature range,demonstrating strong adaptability and application potential.This study provides a scalable and cost-effective design strategy for high-performance carbon-based air cathodes,offering new insights into advancing durable and practical metal-air energy systems.展开更多
O3-types layered cathode materials in sodium-ion batteries(SIBs)suffer from the obvious lattice distortion induced by the complex phase transitions during Na^(+)intercalation/deintercalation process,leading to severe ...O3-types layered cathode materials in sodium-ion batteries(SIBs)suffer from the obvious lattice distortion induced by the complex phase transitions during Na^(+)intercalation/deintercalation process,leading to severe structural collapse and performance degradation.Herein,a series of high valence tantalum(Ta^(5+))doped Na(Ni_(0.4)Fe_(0.2)Mn_(0.4))_(1−x)Ta_(x)O_(2)(x=0/0.0025/0.005/0.01)secondary spherical particles are firstly developed,where Ta^(5+)doping enables the refined primary grain with a tightly stacked rod-like morphology.Comprehensive structural analysis via Neutron powder diffraction(NPD)and Synchrotron radiation X-ray diffraction(SXRD)reveals an expanded NaO_(2)slab and a reduction in Na site vacancy.The potential charge compensation mechanism is further illustrated by X-ray absorption spectroscopy(XAS)and X-ray photoelectron spectroscopy(XPS),unveiling a partial reduction from Ni^(3+)to Ni^(2+)with Ta^(5+)doping.In situ X-ray diffraction(in situ XRD)suggests that the decorated sample undergoes a volume change as low as 0.8%,in contrast with the pristine one(1.5%).Thus,the optimized sample with x=0.005 retains an enhanced capacity retention up to 70.4%at 1 C after 300 cycles in half-cell and delivers a high energy density of 251 Wh kg^(-1)(0.1 C)and with a good capacity retention of 81.0%at 1 C after 200 cycles in full-cell.Our findings provide new insights into the mechanism of high valence Ta^(5+)doping in stabilizing layered oxides cathode materials for SIBs.展开更多
The outstanding performance of O3-type NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2)(NFM111)at both high and low temperatures coupled with its impressive specific capacity makes it an excellent cathode material for sodium-ion batte...The outstanding performance of O3-type NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2)(NFM111)at both high and low temperatures coupled with its impressive specific capacity makes it an excellent cathode material for sodium-ion batteries.However,its poor cycling,owing to highpressure phase transitions,is one of its disadvantages.In this study,Cu/Ti was introduced into NFM111 cathode material using a solidphase method.Through both theoretically and experimentally,this study found that Cu doping provides a higher redox potential in NFM111,improving its reversible capacity and charge compensation process.The introduction of Ti would enhance the cycling stability of the material,smooth its charge and discharge curves,and suppress its high-voltage phase transitions.Accordingly,the NaNi_(0.27)Fe_(0.28)Mn_(0.33)Cu_(0.05)Ti_(0.06)O_(2)sample used in the study exhibited a remarkable rate performance of 142.97 mAh·g^(-1)at 0.1 C(2.0-4.2 V)and an excellent capacity retention of 72.81%after 300 cycles at 1C(1C=150 mA·g^(-1)).展开更多
Rechargeable magnesium batteries(RMBs)possess the merits of greater theoretical capacity,cheaper magnesium metal and not easily producing branched crystals,and greater safety.Therefore,the current researches mainly co...Rechargeable magnesium batteries(RMBs)possess the merits of greater theoretical capacity,cheaper magnesium metal and not easily producing branched crystals,and greater safety.Therefore,the current researches mainly concentrate on the exploration of high-performance RMBs in the initial stage,but still face many gigantic challenges.Herein,petal-shaped nanorods CoS/CuS materials are successfully synthesized as RMBs cathode materials through a two-step metal sulfide template-free solvent-thermal synthesis method,which can effectively improve the reaction kinetics due to the petal-like nano-structure and provide rich electrochemically active sites to decrease the transport barrier of Mg^(2+),thus contributing to the enhancement of the reaction kinetics of magnesium storage in RMBs.The electrochemical performance test illustrates that CoS/CuS composite nanomaterials can considerably improve the charging and discharging specific capacity of the batteries as well as the voltage of the batteries due to the existing synergistic effect between them.The specific capacity of CoS/CuS cathode still can still be maintained as high as 62.8 mAh g^(−1)after 300 cycles at 200 mA g^(−1).And the specific capacity of this electrode material changes from 180.6 mAh g^(−1)to 30 mAh g^(−1)at the current densities from 100 mA g^(−1)to 1000 mA g^(−1),and when the current density is restored to 100 mA g^(−1),the specific capacity gradually recovered to 178.6 mAh g^(−1),which showed better rate performance and ultra-high cycling stability.This work highlights how the introduction of CuS into CoS nanostructures can benefit the reversibility and cyclicity of the magnesium storage reaction and offers an original and practical route for the modification of RMBs electrode materials with good electrochemical properties.展开更多
Waste graphitization cathode carbon blocks are a type of hazardous solid waste generated during the aluminum electrolysis process,and their proper disposal is a key step in the resource utilization of discarded graphi...Waste graphitization cathode carbon blocks are a type of hazardous solid waste generated during the aluminum electrolysis process,and their proper disposal is a key step in the resource utilization of discarded graphite.This study utilizes the porous“defect advantage”of a cathode carbon block matrix to prepare silicon-doped and asphalt-coated detoxified and purified waste graphitization cathode carbon blocks for use as high-performance silicon/carbon composite anode materials.The results show that the uniformly silicondoped silicon/carbon composite material features a unique amorphous carbon-encapsulated“locked silicon”structure,which effectively addresses issues such as cathode volume expansion,excessive growth of the solid electrolyte interphase(SEI)film,and poor electrical contact between active materials.Consequently,electrochemical performance is enhanced.After assembly in a half-cell,the PSCC/10%Si@C(purified waste graphitization cathode carbon/10%Si@C)material exhibits optimal electrochemical stability,with an initial charging specific capacity of 514.5 mAh/g at 0.1 C(1 C=170 mA/g)and a capacity retention rate of 95.1%after 100 cycles.At a charge rate of 2.0 C,a specific capacity of 216.9 mAh/g is achieved.This technology provides a new pathway for the economical and high-value utilization of waste cathode carbon blocks and the development of low-cost,high-performance anode materials.展开更多
Cation disordering is a common issue in Ni-rich cathodes that significantly degrades cycle life and compromises safety.The cubic rock-salt phase formation and the slow oxidation kinetics of Ni^(2+)during solid-state s...Cation disordering is a common issue in Ni-rich cathodes that significantly degrades cycle life and compromises safety.The cubic rock-salt phase formation and the slow oxidation kinetics of Ni^(2+)during solid-state sintering are widely recognized as the principal causes of these structural defects.To solve this issue,a topotactic soft-chemical precursor engineering strategy is proposed for use in aqueous solution.By utilizing the layered structure of the precursor,this method allows for selective proton extraction and efficient Ni^(2+)oxidation,along with rapid Li+intercalation to form a layered lithiated intermediate.This intermediate crystallizes without further phase transitions during subsequent heat treatment,preventing structural defects caused by complex phase evolution and slow ion diffusion.The resulting cathode exhibits a long-range ordered layered structure and a uniform phase distribution,enabling efficient Li+insertion and extraction.Electrochemical tests reveal a high discharge capacity of 229.6 mAh g^(−1)and an initial coulombic efficiency of 95.77%at 0.1 C,greatly exceeding the performance of a conventionally synthesized cathode(210.3 mAh g^(−1),88.93%).Improved Li^(+)transport kinetics reduces phase-transition hysteresis and alleviates stress concentration,resulting in better cycling stability with a capacity retention of 85.3%after 300 cycles,compared to 61.5%for the conventional sample.This work presents a scalable and effective synthesis route for Ni-rich cathodes with reduced structural disorder and extended lifespan,providing valuable insights into how the regulation of intermediate phases influences electrochemical performance in high-performance Ni-rich cathodes.展开更多
The growing need for higher energy density in rechargeable batteries necessitates the exploration of cathode materials with enhanced specific energy for lithium-ion batteries.Due to their exceptional cost-effectivenes...The growing need for higher energy density in rechargeable batteries necessitates the exploration of cathode materials with enhanced specific energy for lithium-ion batteries.Due to their exceptional cost-effectiveness and specific capacity,lithium-rich manganese-based cathode materials(LRMs)obtain in-creasing attention in the pursuit of enhancing energy density and reducing costs.The implementation has faced obstacles in various applications due to substantial capacity and voltage degradation,insufficient safety performance,and restricted rate capability during cycling.These issues arise from the migration of transition metal,the release of oxygen,and structural transformation.In this review,we provide an integrated survey of the structure,lithium storage mechanism,challenges,and origins of LRMs,as well as recent advancements in various coating strategies.Particularly,the significance of optimizing the design of the cathode electrolyte interphase was emphasized to enhance electrode performance.Furthermore,future perspective was also addressed alongside in-situ measurements,advanced synthesis techniques,and the application of machine learning to overcome encountered challenges in LRMs.展开更多
Rechargeable magnesium batteries(RMBs)are a cutting-edge energy storage solution,with several advantages over the state-of-art lithiumion batteries(LIBs).The use of magnesium(Mg)metal as an anode material provides a m...Rechargeable magnesium batteries(RMBs)are a cutting-edge energy storage solution,with several advantages over the state-of-art lithiumion batteries(LIBs).The use of magnesium(Mg)metal as an anode material provides a much higher gravimetric capacity compared to graphite,which is currently used as the anode material in LIBs.Despite the significant advances in electrolyte,the development of cathode material is limited to materials that operate at low average discharge voltage(<1.0 V vs.Mg/Mg^(2+)),and developing high voltage cathodes remains challenging.Only a few materials have been shown to intercalate Mg^(2+)ions reversibly at high voltage.This review focuses on the structural aspects of cathode material that can operate at high voltage,including the Mg^(2+)intercalation mechanism in relation to its electrochemical properties.The materials are categorized into transition metal oxides and polyanions and subcategorized by the intrinsic Mg^(2+)diffusion path.This review also provides insights into the future development of each material,aiming to stimulate and guide researchers working in this field towards further advancements in high voltage cathodes.展开更多
Lithium-rich manganese-based oxides(LRMOs;xLi_(2)MnO_(3)(1−x)LiMO_(2);M=transition metal,0<x<1)with excellent specific capacity(>300 mAh/g)and high operating voltage(≥4.8V)are the preferred cathode materials...Lithium-rich manganese-based oxides(LRMOs;xLi_(2)MnO_(3)(1−x)LiMO_(2);M=transition metal,0<x<1)with excellent specific capacity(>300 mAh/g)and high operating voltage(≥4.8V)are the preferred cathode materials for high-specific-energy lithium metal batteries(LMBs)[1].However,LRMOs face a series of serious problems such as irreversible lattice oxygen loss,transition metal(TM)migration,phase transfer,and interfacial side reactions at high voltages,resulting in rapid decay of capacity and voltage[2,3].In situ generating well-functional CEI through electrolyte engineering can effectively address these challenges[4].展开更多
Solid-state lithium batteries(SSLBs)are regarded as an essential growth path in energy storage systems due to their excellent safety and high energy density.In particular,SSLBs using conversion-type cathode materials ...Solid-state lithium batteries(SSLBs)are regarded as an essential growth path in energy storage systems due to their excellent safety and high energy density.In particular,SSLBs using conversion-type cathode materials have received widespread attention because of their high theoretical energy densities,low cost,and sustainability.Despite the great progress in research and development of SSLBs based on conversiontype cathodes,their practical applications still face challenges such as blocked ionic-electronic migration pathways,huge volume change,interfacial incompatibility,and expensive processing costs.This review focuses on the advantages and critical issues of coupling conversion-type cathodes with solid-state electrolytes(SSEs),as well as state-of-the-art progress in various promising cathodes(e.g.,FeS_(2),CuS,FeF_(3),FeF_(2),and S)in SSLBs.Furthermore,representative research on conversion-type solid-state full cells is discussed to offer enlightenment for their practical application.Significantly,the energy density exhibited by the S cathode stands out impressively,while sulfide SSEs and halide SSEs have demonstrated immense potential for coupling with conversion-type cathodes.Finally,perspectives on conversion-type cathodes are provided at the material,interface,composite electrode,and battery levels,with a view to accelerating the development of conversion-type cathodes for high-energy–density SSLBs.展开更多
Ni-rich layered oxide cathode materials such as LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM811)face poor interfacial stability and serious side reactions with sulfide solid-state electrolytes.This problem is thought to be exa...Ni-rich layered oxide cathode materials such as LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM811)face poor interfacial stability and serious side reactions with sulfide solid-state electrolytes.This problem is thought to be exacerbated by the gradually accumulated basicity of the surface with the Ni content increasing.Herein,the acidic Li_(3)PO_(4)coating layer on NCM811 particles is introduced by ball-milling approach to neutralize the basicity and aggrandize the interfacial stability.The tailored surface structure and components of NCM811 not only suppress the direct contact of cathode particles with sulfide solid-state electrolyte,but also facilitate electrochemical dynamics by driving the Li+migration across the interface and promoting the electron exchange.Thus,cells with Li_(3)PO_(4)coating layer yield 101.3 mAh g^(-1)specific capacity at 2.0 C and highly reversed discharging capacity after suffering from harsh work conditions.Additionally,the stable coating layer broadens the electrochemical windows of cells,delivering long cycle stability(>100 cycles 0.5 C).This contribution highlights the importance of basicity regulation of Ni-rich layered oxide cathode and offers a low-cost and effective approach to design the interfacial structures for the development of all solid-state batteries.展开更多
文摘Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_(2)(PO_(4))_(3)(LVP@C)nanoparticles on carbon nanofibers(CNFs)has been achieved by an electrospinning technique followed by calcination.The protective carbon coating prevents the aggregation of the LVP nanoparticles and suppresses V dissolution by preventing direct contact with aqueous electrolytes.The CNFs derived from the electrospun nanofibers provide a 3D network to increase the electronic conductivity of the LVP electrode,and the LVP@C-CNF hybrid film can be directly used as a freestanding cathode for zinc-ion batteries without adding conductive additives and binders.A mechanism for the formation of a uniform and continuous carbon coating has been proposed.This nanostructure,combined with the uniform and intact carbon coverage,significantly increases the electronic conductivity.This LVP@C-CNF freestanding electrode has an excellent rate capability(47.3%retention at 2 C)and cycling stability(61.2%retention after 100 cycles)within the voltage range 0.6 V to 1.95 V and is highly suitable for zinc-ion battery applications.
基金supported by the National Natural Science Foundation of China(Nos.U2341209 and 52130407).
文摘A novel trace nickel(Ni)doped tungsten(W)matrix with coated Ni on W grains was prepared by powder metallurgy method.The introduction of Ni can inhibit the reaction between W and barium-calcium aluminates(Ba-Ca aluminates)during the impregnation process of the matrix.After cathode activation,the surface Ba:O molar ratio is 0.88:1.00,much higher than the Ba dispenser cathode without Ni doping.The XPS results of the cathode surface showed that the metallic Ba appeared on the activated cathode surface,forming dipoles with oxygen,and effectively reducing the cathode surface work function.The pulse electron emission current density at 1100℃_(b)(brightness temperature)was 18.26 A/cm^(2),and the calculated work function was 1.97 eV.It has a low evaporation rate and the accelerated lifetime test predict a lifetime of over 160000 h.First-principles calculations showed that the charge transfer and dipole moment in the NiW-BaO system were both increased compared to the Ba dispenser cathode,thus improving the emission performance of the Ni-W mixed matrix cathode.
基金We would like to show gratitude to the Yunnan Province Basic Research Major Project(202501BC070006(Y.Wang))Key Industry Science and Technology Projects for University Services in Yunnan Province(FWCY ZNT2024002(Y.Wang))+3 种基金National Natural Science Foundation of China(22279070(L.Wang))and(U21A20170(X.He))the Ministry of Science and Technology of China(2019YFA0705703(L.Wang))Beijing Natural Science Foundation(L242005(X.He))Key Industry Science and Technology Projects for University Services in Yunnan Province(FWCY BSPY2024011(T.Lai)).
文摘Long-life energy storage batteries are integral to energy storage systems and electric vehicles,with lithium-ion batteries(LIBs)currently being the preferred option for extended usage-life energy storage.To further extend the life span of LIBs,it is essential to intensify investments in battery design,manufacturing processes,and the advancement of ancillary materials.The pursuit of long durability introduces new challenges for battery energy density.The advent of electrode material offers effective support in enhancing the battery’s long-duration performance.Often underestimated as part of the cathode composition,the binder plays a pivotal role in the longevity and electrochemical performance of the electrode.Maintaining the mechanical integrity of the electrode through judicious binder design is a fundamental requirement for achieving consistent long-life cycles and high energy density.This paper primarily concentrates on the commonly employed cathode systems in lithium-ion batteries,elucidates the significance of binders for both,discusses the application status,strengths,and weaknesses of novel binders,and ultimately puts forth corresponding optimization strategies.It underscores the critical function of binders in enhancing battery performance and advancing the sustainable development of lithium-ion batteries,aiming to offer fresh insights and perspectives for the design of high-performance LIBs.
基金supported by the Ministry of Science and Technology of China(2025YFE0100200)the Natural Science Foundation of Tianjin(24JCJQJC00220 and 24ZXZSSS00310)+3 种基金the National Natural Science Foundation of China(22479080,92372203,and 92372001)the Open Foundation of Shanghai Jiao Tong University Shaoxing Research Institute of Renewable Energy and Molecular Engineering(JDSX2023003)the Fundamental Research Funds for the Central Universities of Nankai University(020-63253167)the"111 Center"(B25010)。
文摘Layered transition metal oxide cathode materials have garnered increasing attention for sodium-ion batteries(SIBs).However,they are plagued by the Jahn-Teller distortion of MnO6,Na^(+)/vacancy ordering,and irreversible lattice oxygen loss,which collectively lead to capacity fading and voltage decay.Herein,we report a P2-type material,Na_(0.67)Ni_(0.3)Mn_(0.6)Li_(0.09)Sn_(0.01)O_(2)(NNMO-Li0.09Sn0.01),modified with two closed-shell dopants(i.e.,Li^(+)and Sn^(4+)).Benefiting from the unique electronic configurations of closed-shell ions,NNMO-Li0.09Sn0.01 exhibits enhanced structural and electrochemical stability.Specifically,the incorporation of Li^(+)increases the Mn^(4+)/Mn3+ratio,thereby mitigating Jahn-Teller distortion during(de)sodiation process.In addition,Li^(+)disrupts the Ni/Mn ordering in the transition metal layer,suppressing Na^(+)/vacancy ordering.Meanwhile,the introduction of Sn^(4+)forms stronger Sn-O bonds(548 kJ mol-1),thereby enhancing the bonding strength between neighboring transition metal ions and surrounding oxygen atoms,effectively reducing oxygen loss during cycling.NNMO-Li0.09Sn0.01 exhibits significantly improved cycling stability,delivering a specific capacity of 90.3 mAh g^(-1)with 62.9%capacity retention after 50 cycles at 0.1 C(1 C=200 mA g^(-1)),along with 90.3%voltage retention.This substitution strategy based on closed-shell ions offers a viable approach for enhancing the structural stability of wide-voltage layered oxide cathodes.
基金financially supported by the Research and Development Program of China (2022YFA1505700)the National Natural Science Foundation of China (22475214, 22205232, 52102216)+6 种基金the Natural Science Foundation of Fujian Province (2023J06044,2022J01625, 2022-S-002)the Talent Plan of Shanghai BranchChinese Academy of Sciences (CASSHB-QNPD-2023-020)the Selfdeployment Project Research Program of Haixi Institutes,Chinese Academy of Sciences (CXZX-2022-JQ06 and CXZX-2022-GH03)the Anhui Key Laboratory of Nanomaterials and Nanotechnology,the Major Science and Technology Projects in Anhui Province(202305a12020006)the Open Project of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry (2025-22)the Innovation Training Program for College Students(2025019300A, 20250193008)
文摘Co-free Li-rich Li_(1.2)Ni_(0.2)Mn_(0.6)O_(2)(LR)cathode shows the highest working capacity that can be applied to high-energy density Li-ion batteries(LIBs).However,poor cycle stability and voltage decay caused by phase transition are always hindering its further development.Herein,a novel medium-entropy Li-rich Mn-based cathode material(LRMEF)was synthesized via a simple sol-gel method.The introduction of multivalent ions(Al^(3+)/Cu^(2+)doping at Mn sites and F−doping at O sites)effectively mitigates the Jahn-Teller distortion of Mn ions and suppresses oxygen release.High-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)images confirm that this synergistic doping strategy induces the in-situ formation of an approximately 3 nm-thick spinel surface layer,which significantly enhances structural stability and ion diffusion kinetics.Besides,a series of in-situ/ex-situ characterization methods and density functional theory(DFT)calculations have been carried out to fundamentally shed light on the optimized structure-activity relationship and reaction mechanism.As a result,the LR material with entropy regulation and anion doping exhibits excellent cycling stability(189.2 mAh g^(−1)at 1 C with 84%capacity retention after 300 cycles),rate performance(164.1 mAh g^(−1)at 5 C),and voltage retention(82.7%at 1 C after 300 cycles),demonstrating great application prospects in future high-energy-density LIBs.
基金supported by the National Natural Science Foundation of China(Nos.U21A20311 and 52400163).
文摘The high voltage of Li||LiCoO_(2) battery can increase the energy density.However,the cycling performance associated with cathode structural stability remains challenging.To address this question,we proposed an electrolyte strategy for improving the performance of 4.6 V Li||LiCoO_(2) battery by using trimethylsilyl isocyanate(TMIS)as electrolyte additive.The trimethylsilyl group of TMIS can trap HF while the isocyanate group brings polyamide components to the CEI and the SEI.By the synergistic action,the Co3+dissolution problem of the LiCoO_(2) cathode was effectively curbed.Furthermore,TMIS regulates the construction of anion-dominated LiF-rich SEI by influencing the solvation structure of Li+.As expected,the 4.6 V Li||LiCoO_(2) battery with TMIS retains 77.9% initial capacity after 200 cycles at 0.5 C.
基金supported by the National Natural Science Foundation of China (52302259)the China Postdoctoral Science Foundation (CPSF) under Grant Number 2023M741479+4 种基金the Postdoctoral Fellowship Program of CPSF under Grant Number GZB20240280the Jiangxi Provincial Natural Science Foundation (20224ACB218006)the financial support from High-level Talent Research Special Funds of Jiangxi University of Science and Technology (Grant No. 205200100670)the Jiangxi Provincial Key Laboratory of Power Energy Storage Batteries and Materials (2024SSY10011)the Major Scientific and Technological Research R&D Special Project of Jiangxi Province(20244AFI92002)
文摘The implementation of multifunctional application scenarios for mobile terminal devices has increased the energy density requirements of batteries.Increasing the charging voltage can rapidly increase the specific capacity of layered transition metal oxides;however,it also exacerbates the release of lattice oxygen and the contraction of the unit cell.Ternary materials are designed in a secondary particle state to meet the requirements of power battery applications.Therefore,to create ternary materials that can operate under ultrahigh voltages,attention should be given to both surface modification and particle integrity maintenance.By utilizing elemental selenium(Se)with a low melting point,easy sublimation,and multiple variable valence states,deep grain boundary modification was implemented inside the particles.The performance of the cathode material was evaluated through pouch cells,and the improvement mechanism was explored through molecular dynamics simulation calculations.Under the protection of a three-dimensional Se-rich modified layer,LiNi_(1/3)Co_(1/3)Mn_(1/3)O_(2)achieved stable operation at ultrahigh voltages(4.6 V vs.Li/Li^(+));a sacrificial protection mechanism based on the chronic decomposition of the Se-rich layer was proposed to explain the efficacy of Se modification in stabilizing ternary materials.This deep grain boundary modification based on elemental Se provides a new solution for the ultrahigh-voltage operation of transition metal oxides and provides a scientific basis and technical support for solving the interface contact problem of all-solid-state batteries.
基金supported by the Learning&Academic Research Institution for Master’s,PhD students,and Postdocs LAMP Program of the National Research Foundation of Korea(NRF)grant funded by the Ministry of Education(No.RS-2023-00301974)This work was also supported by the Glocal University 30 Project fund of Gyeongsang National University in 2025.
文摘Lithium manganese silicate(Li-Mn-Si-O)cathodes are key components of lithium-ion batteries,and their physical and mechanical properties are strongly influenced by their underlying crystal structures.In this study,a range of machine learning(ML)algorithms were developed and compared to predict the crystal systems of Li-Mn-Si-O cathode materials using density functional theory(DFT)data obtained from the Materials Project database.The dataset comprised 211 compositions characterized by key descriptors,including formation energy,energy above the hull,bandgap,atomic site number,density,and unit cell volume.These features were utilized to classify the materials into monoclinic(0)and triclinic(1)crystal systems.A comprehensive comparison of various classification algorithms including Decision Tree,Random Forest,XGBoost,Support VectorMachine,k-Nearest Neighbor,Stochastic Gradient Descent,Gaussian Naive Bayes,Gaussian Process,and Artificial Neural Network(ANN)was conducted.Among these,the optimized ANN architecture(6–14-14-14-1)exhibited the highest predictive performance,achieving an accuracy of 95.3%,aMatthews correlation coefficient(MCC)of 0.894,and an F-score of 0.963,demonstrating excellent consistency with DFT-predicted crystal structures.Meanwhile,RandomForest and Gaussian Processmodels also exhibited reliable and consistent predictive capability,indicating their potential as complementary approaches,particularly when data are limited or computational efficiency is required.This comparative framework provides valuable insights into model selection for crystal system classification in complex cathode materials.
基金funded by the National Nature Science Foundation of China(62264006,62574102)“Thousand Talents Program”of Yunnan Province for Young Talents,Innovative Research Teams(in Science and Technology)in the University of Yunnan Province(IRTSTYN),XingDian Talent Support Program for Young Talents,and Frontier Research Team of Kunming University 2023,The Basic Research Project of Yunnan Province(Nos.202201AU070022)+2 种基金Kunming University Talent Introduction Fund(Nos.YJL20024)Yunnan Province Education Department Scientific Research Fund Project(Nos.2024Y759)Undergraduate Innovation and Entrepreneurship Training Program Project of Yunnan Provincial(202411393005)。
文摘Carbon-based air cathodes offer low cost,high electrical conductivity,and structural tunability.However,they suffer from limited catalytic activity and inefficient gas transport,and they typically rely on noble metal additives or complex multilayer configurations.To tackle these issues,this study devised a self-activated integrated carbon-based air cathode.By integrating in situ catalytic site construction with structural optimization,the strategy not only induces the formation of oxygen functional groups(─C─OH,─C═O,─COOH),hierarchical pores,and uniformly distributed active sites,but also establishes a favorable electronic and mass-transport environment.Furthermore,the roll-pressing-based integrated design streamlines electrode construction,reinforces interfacial bonding,and significantly enhances mechanical stability.Density functional theory(DFT)calculations show that oxygen functional groups initiate hydrogen bonding interaction and promote charge enrichment,which improves the activity of the cathode and facilitates intermediate adsorption/desorption in oxygen reduction and evolution reactions processes.As a result,the integrated air cathode-based rechargeable zinc-air batteries(RZABs)achieve a high specific capacity of 811 mAh g^(-1).It also performs well in quasi-solid-state RZABs and silicon-air batteries systems across a wide temperature range,demonstrating strong adaptability and application potential.This study provides a scalable and cost-effective design strategy for high-performance carbon-based air cathodes,offering new insights into advancing durable and practical metal-air energy systems.
基金supported by the National Natural Science Foundation of China (52402298, 52172224, 52202228, 22479112)the Science and Technology Correspondent Project of Tianjin(24YDTPJC00240)+3 种基金Science Research Project of Hebei Education Department (BJK2022011)Central Funds Guiding the Local Science and Technology Development of Hebei Province (236Z4404G)the Beijing Tianjin Hebei Basic Research Cooperation Special Project(E2024202273)Tianjin Sci.&Tech. Program (22YFYSHZ00220)
文摘O3-types layered cathode materials in sodium-ion batteries(SIBs)suffer from the obvious lattice distortion induced by the complex phase transitions during Na^(+)intercalation/deintercalation process,leading to severe structural collapse and performance degradation.Herein,a series of high valence tantalum(Ta^(5+))doped Na(Ni_(0.4)Fe_(0.2)Mn_(0.4))_(1−x)Ta_(x)O_(2)(x=0/0.0025/0.005/0.01)secondary spherical particles are firstly developed,where Ta^(5+)doping enables the refined primary grain with a tightly stacked rod-like morphology.Comprehensive structural analysis via Neutron powder diffraction(NPD)and Synchrotron radiation X-ray diffraction(SXRD)reveals an expanded NaO_(2)slab and a reduction in Na site vacancy.The potential charge compensation mechanism is further illustrated by X-ray absorption spectroscopy(XAS)and X-ray photoelectron spectroscopy(XPS),unveiling a partial reduction from Ni^(3+)to Ni^(2+)with Ta^(5+)doping.In situ X-ray diffraction(in situ XRD)suggests that the decorated sample undergoes a volume change as low as 0.8%,in contrast with the pristine one(1.5%).Thus,the optimized sample with x=0.005 retains an enhanced capacity retention up to 70.4%at 1 C after 300 cycles in half-cell and delivers a high energy density of 251 Wh kg^(-1)(0.1 C)and with a good capacity retention of 81.0%at 1 C after 200 cycles in full-cell.Our findings provide new insights into the mechanism of high valence Ta^(5+)doping in stabilizing layered oxides cathode materials for SIBs.
基金supported by the Low-Cost Long-Life Batteries program,China(No.WL-24-08-01)the National Natural Science Foundation of China(No.22279007)。
文摘The outstanding performance of O3-type NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2)(NFM111)at both high and low temperatures coupled with its impressive specific capacity makes it an excellent cathode material for sodium-ion batteries.However,its poor cycling,owing to highpressure phase transitions,is one of its disadvantages.In this study,Cu/Ti was introduced into NFM111 cathode material using a solidphase method.Through both theoretically and experimentally,this study found that Cu doping provides a higher redox potential in NFM111,improving its reversible capacity and charge compensation process.The introduction of Ti would enhance the cycling stability of the material,smooth its charge and discharge curves,and suppress its high-voltage phase transitions.Accordingly,the NaNi_(0.27)Fe_(0.28)Mn_(0.33)Cu_(0.05)Ti_(0.06)O_(2)sample used in the study exhibited a remarkable rate performance of 142.97 mAh·g^(-1)at 0.1 C(2.0-4.2 V)and an excellent capacity retention of 72.81%after 300 cycles at 1C(1C=150 mA·g^(-1)).
基金financially supported by the National Natural Science Foundation of China(Nos.21804008,52102209)the International Technological Collaboration Project of Shanghai(No.17520710300)+1 种基金Anhui Provincial Natural Science Foundation(No.2108085QE197)Guangdong Basic and Applied Basic Research Foundation(Nos.2022A1515010834,2020A1515110221).
文摘Rechargeable magnesium batteries(RMBs)possess the merits of greater theoretical capacity,cheaper magnesium metal and not easily producing branched crystals,and greater safety.Therefore,the current researches mainly concentrate on the exploration of high-performance RMBs in the initial stage,but still face many gigantic challenges.Herein,petal-shaped nanorods CoS/CuS materials are successfully synthesized as RMBs cathode materials through a two-step metal sulfide template-free solvent-thermal synthesis method,which can effectively improve the reaction kinetics due to the petal-like nano-structure and provide rich electrochemically active sites to decrease the transport barrier of Mg^(2+),thus contributing to the enhancement of the reaction kinetics of magnesium storage in RMBs.The electrochemical performance test illustrates that CoS/CuS composite nanomaterials can considerably improve the charging and discharging specific capacity of the batteries as well as the voltage of the batteries due to the existing synergistic effect between them.The specific capacity of CoS/CuS cathode still can still be maintained as high as 62.8 mAh g^(−1)after 300 cycles at 200 mA g^(−1).And the specific capacity of this electrode material changes from 180.6 mAh g^(−1)to 30 mAh g^(−1)at the current densities from 100 mA g^(−1)to 1000 mA g^(−1),and when the current density is restored to 100 mA g^(−1),the specific capacity gradually recovered to 178.6 mAh g^(−1),which showed better rate performance and ultra-high cycling stability.This work highlights how the introduction of CuS into CoS nanostructures can benefit the reversibility and cyclicity of the magnesium storage reaction and offers an original and practical route for the modification of RMBs electrode materials with good electrochemical properties.
基金supported by the National Natural Science Foundation of China(No.52274346).
文摘Waste graphitization cathode carbon blocks are a type of hazardous solid waste generated during the aluminum electrolysis process,and their proper disposal is a key step in the resource utilization of discarded graphite.This study utilizes the porous“defect advantage”of a cathode carbon block matrix to prepare silicon-doped and asphalt-coated detoxified and purified waste graphitization cathode carbon blocks for use as high-performance silicon/carbon composite anode materials.The results show that the uniformly silicondoped silicon/carbon composite material features a unique amorphous carbon-encapsulated“locked silicon”structure,which effectively addresses issues such as cathode volume expansion,excessive growth of the solid electrolyte interphase(SEI)film,and poor electrical contact between active materials.Consequently,electrochemical performance is enhanced.After assembly in a half-cell,the PSCC/10%Si@C(purified waste graphitization cathode carbon/10%Si@C)material exhibits optimal electrochemical stability,with an initial charging specific capacity of 514.5 mAh/g at 0.1 C(1 C=170 mA/g)and a capacity retention rate of 95.1%after 100 cycles.At a charge rate of 2.0 C,a specific capacity of 216.9 mAh/g is achieved.This technology provides a new pathway for the economical and high-value utilization of waste cathode carbon blocks and the development of low-cost,high-performance anode materials.
基金the financial support from the Central South University Fundamental Research Funds (Grant No.2025ZZTS0444)the Innovation-Driven Research Program(Grant No. 2023 CXQD053)+3 种基金the National Natural Science Foundation of China (Grant No. 52274310)the financial support (Project No.H202111040350002)the provision of the hydroxide precursors from Ningbo Ronbay New Energy Technology Co.,Ltdsupported in part by the High-Performance Computing Center of Central South University
文摘Cation disordering is a common issue in Ni-rich cathodes that significantly degrades cycle life and compromises safety.The cubic rock-salt phase formation and the slow oxidation kinetics of Ni^(2+)during solid-state sintering are widely recognized as the principal causes of these structural defects.To solve this issue,a topotactic soft-chemical precursor engineering strategy is proposed for use in aqueous solution.By utilizing the layered structure of the precursor,this method allows for selective proton extraction and efficient Ni^(2+)oxidation,along with rapid Li+intercalation to form a layered lithiated intermediate.This intermediate crystallizes without further phase transitions during subsequent heat treatment,preventing structural defects caused by complex phase evolution and slow ion diffusion.The resulting cathode exhibits a long-range ordered layered structure and a uniform phase distribution,enabling efficient Li+insertion and extraction.Electrochemical tests reveal a high discharge capacity of 229.6 mAh g^(−1)and an initial coulombic efficiency of 95.77%at 0.1 C,greatly exceeding the performance of a conventionally synthesized cathode(210.3 mAh g^(−1),88.93%).Improved Li^(+)transport kinetics reduces phase-transition hysteresis and alleviates stress concentration,resulting in better cycling stability with a capacity retention of 85.3%after 300 cycles,compared to 61.5%for the conventional sample.This work presents a scalable and effective synthesis route for Ni-rich cathodes with reduced structural disorder and extended lifespan,providing valuable insights into how the regulation of intermediate phases influences electrochemical performance in high-performance Ni-rich cathodes.
基金the support from the National Natural Science Foun-dation of China(Grant No.U21A20311)the Distinguished Scientist Fellowship Program(DSFP)at King Saud University,Riyadh,Saudi Arabia.
文摘The growing need for higher energy density in rechargeable batteries necessitates the exploration of cathode materials with enhanced specific energy for lithium-ion batteries.Due to their exceptional cost-effectiveness and specific capacity,lithium-rich manganese-based cathode materials(LRMs)obtain in-creasing attention in the pursuit of enhancing energy density and reducing costs.The implementation has faced obstacles in various applications due to substantial capacity and voltage degradation,insufficient safety performance,and restricted rate capability during cycling.These issues arise from the migration of transition metal,the release of oxygen,and structural transformation.In this review,we provide an integrated survey of the structure,lithium storage mechanism,challenges,and origins of LRMs,as well as recent advancements in various coating strategies.Particularly,the significance of optimizing the design of the cathode electrolyte interphase was emphasized to enhance electrode performance.Furthermore,future perspective was also addressed alongside in-situ measurements,advanced synthesis techniques,and the application of machine learning to overcome encountered challenges in LRMs.
基金supported by the Nano&Material Technology Development Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(RS-2024-00446825)by the Technology Innovation Program(RS-2024-00418815)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea).
文摘Rechargeable magnesium batteries(RMBs)are a cutting-edge energy storage solution,with several advantages over the state-of-art lithiumion batteries(LIBs).The use of magnesium(Mg)metal as an anode material provides a much higher gravimetric capacity compared to graphite,which is currently used as the anode material in LIBs.Despite the significant advances in electrolyte,the development of cathode material is limited to materials that operate at low average discharge voltage(<1.0 V vs.Mg/Mg^(2+)),and developing high voltage cathodes remains challenging.Only a few materials have been shown to intercalate Mg^(2+)ions reversibly at high voltage.This review focuses on the structural aspects of cathode material that can operate at high voltage,including the Mg^(2+)intercalation mechanism in relation to its electrochemical properties.The materials are categorized into transition metal oxides and polyanions and subcategorized by the intrinsic Mg^(2+)diffusion path.This review also provides insights into the future development of each material,aiming to stimulate and guide researchers working in this field towards further advancements in high voltage cathodes.
文摘Lithium-rich manganese-based oxides(LRMOs;xLi_(2)MnO_(3)(1−x)LiMO_(2);M=transition metal,0<x<1)with excellent specific capacity(>300 mAh/g)and high operating voltage(≥4.8V)are the preferred cathode materials for high-specific-energy lithium metal batteries(LMBs)[1].However,LRMOs face a series of serious problems such as irreversible lattice oxygen loss,transition metal(TM)migration,phase transfer,and interfacial side reactions at high voltages,resulting in rapid decay of capacity and voltage[2,3].In situ generating well-functional CEI through electrolyte engineering can effectively address these challenges[4].
基金National Natural Science Foundation of China(22322903,52072061)Natural Science Foundation of Sichuan,China(2023NSFSC1914)Beijing National Laboratory for Condensed Matter Physics(2023BNLCMPKF015)。
文摘Solid-state lithium batteries(SSLBs)are regarded as an essential growth path in energy storage systems due to their excellent safety and high energy density.In particular,SSLBs using conversion-type cathode materials have received widespread attention because of their high theoretical energy densities,low cost,and sustainability.Despite the great progress in research and development of SSLBs based on conversiontype cathodes,their practical applications still face challenges such as blocked ionic-electronic migration pathways,huge volume change,interfacial incompatibility,and expensive processing costs.This review focuses on the advantages and critical issues of coupling conversion-type cathodes with solid-state electrolytes(SSEs),as well as state-of-the-art progress in various promising cathodes(e.g.,FeS_(2),CuS,FeF_(3),FeF_(2),and S)in SSLBs.Furthermore,representative research on conversion-type solid-state full cells is discussed to offer enlightenment for their practical application.Significantly,the energy density exhibited by the S cathode stands out impressively,while sulfide SSEs and halide SSEs have demonstrated immense potential for coupling with conversion-type cathodes.Finally,perspectives on conversion-type cathodes are provided at the material,interface,composite electrode,and battery levels,with a view to accelerating the development of conversion-type cathodes for high-energy–density SSLBs.
基金supported by the National Natural Science Foundation of China(22379121)the Shenzhen Foundation Research Fund(JCYJ20210324104412034)+1 种基金the Fundamental Research Funds for the Central Universities(G2024KY05103)the“Scientists+Engineers”Team in Qinchuangyuan of Shaanxi Province(2024QCY-KXJ-023)。
文摘Ni-rich layered oxide cathode materials such as LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM811)face poor interfacial stability and serious side reactions with sulfide solid-state electrolytes.This problem is thought to be exacerbated by the gradually accumulated basicity of the surface with the Ni content increasing.Herein,the acidic Li_(3)PO_(4)coating layer on NCM811 particles is introduced by ball-milling approach to neutralize the basicity and aggrandize the interfacial stability.The tailored surface structure and components of NCM811 not only suppress the direct contact of cathode particles with sulfide solid-state electrolyte,but also facilitate electrochemical dynamics by driving the Li+migration across the interface and promoting the electron exchange.Thus,cells with Li_(3)PO_(4)coating layer yield 101.3 mAh g^(-1)specific capacity at 2.0 C and highly reversed discharging capacity after suffering from harsh work conditions.Additionally,the stable coating layer broadens the electrochemical windows of cells,delivering long cycle stability(>100 cycles 0.5 C).This contribution highlights the importance of basicity regulation of Ni-rich layered oxide cathode and offers a low-cost and effective approach to design the interfacial structures for the development of all solid-state batteries.
