To control the power hierarchy design of lithium-ion battery(LIB)builtup sets for electric vehicles(EVs),we offer intensive theoretical and experimental sets of choice anode/cathode architectonics that can be modulate...To control the power hierarchy design of lithium-ion battery(LIB)builtup sets for electric vehicles(EVs),we offer intensive theoretical and experimental sets of choice anode/cathode architectonics that can be modulated in full-scale LIB built-up models.As primary structural tectonics,heterogeneous composite superstructures of full-cell-LIB(anode//cathode)electrodes were designed in closely packed flower agave rosettes TiO2@C(FRTO@C anode)and vertical-star-tower LiFePO4@C(VST@C cathode)building blocks to regulate the electron/ion movement in the three-dimensional axes and orientation pathways.The superpower hierarchy surfaces and multi-directional orientation components may create isosurface potential electrodes with mobile electron movements,in-to-out interplay electron dominances,and electron/charge cloud distributions.This study is the first to evaluate the hotkeys of choice anode/cathode architectonics to assemble different LIB-electrode platforms with high-mobility electron/ion flows and high-performance capacity functionalities.Density functional theory calculation revealed that the FRTO@C anode and VST-(i)@C cathode architectonics are a superior choice for the configuration of full-scale LIB built-up models.The integrated FRTO@C//VST-(i)@C full-scale LIB retains a huge discharge capacity(~94.2%),an average Coulombic efficiency of 99.85%after 2000 cycles at 1 C,and a high energy density of 127 Wh kg?1,thereby satisfying scale-up commercial EV requirements.展开更多
The advancement of aqueous zinc metal batteries(ZMBs)is constrained by intrinsic interfacial issues in aqueous electrolyte systems.Here,using numerical simulation,we decipher the multi-scale causes of interfacial inst...The advancement of aqueous zinc metal batteries(ZMBs)is constrained by intrinsic interfacial issues in aqueous electrolyte systems.Here,using numerical simulation,we decipher the multi-scale causes of interfacial instability,elucidating the synergistic effect of macroscopic ineffective regions and microscopic passivation.Based on the analysis,we develop an electrolyte-triggered interphase construction strategy to resolve the interfacial failure.This strategy couples the in situ formation of hydrogel interphase on both the anode and cathode with the electrolyte filling process,thereby(1)facilitating contact between electrodes and the separator;(2)promoting anode reversibility through inducing a bilayer SEI that enhances Zn^(2+)desolvation kinetics and blocks electron tunneling;(3)ensuring long-term cathode cycling stability via restricting the irreversible dissolution of MnO_(2)and side-reactions.The resultant Zn metal anode exhibited a near-unity Coulombic efficiency(99.5%)for Zn plating/stripping at an extremely low current density of 0.1 mA cm^(-2)and the Zn/MnO_(2)full cell sustained 2000 full-duty-cycles with an exceptionally low decay rate of 0.0051%per-cycle.This work unlocks an alternative angle for promoting practical ZMB s toward more sustainable energy storage systems.展开更多
High-voltage Li-rich Mn-based oxide(LRMO)cathodes are promising for breaking through the energy density limits of lithium-ion batteries,yet their practical application remains limited by electrochemical performance de...High-voltage Li-rich Mn-based oxide(LRMO)cathodes are promising for breaking through the energy density limits of lithium-ion batteries,yet their practical application remains limited by electrochemical performance degradation caused by unstable cathode-electrolyte interphase(CEI)evolution during longterm cycling.To address this issue,we propose a novel surface modification strategy using La_(0.7)Sr_(0.3)MnO_(3-σ)(LSMO)nanodots,which exhibit high electronic co nductivity and excellent corrosion resistance.These nanodots act as stable anchoring sites,facilitating the formation of a robust CEI on LRMO,The LSMOmodified cathode demonstrates significantly improved anionic redox reversibility,effectively mitigating transition metal migration and lattice oxygen loss.Furthermore,the optimized interfacial electrochemical kinetics ensure sustained rapid Li+diffusion throughout cycling,while the formation of a stable trilayer CEI structure suppresses electrolyte decomposition.Benefiting from these synergistic effects,the LSMO nanodot-engineered LRMO cathode delivers outstanding cycling stability,retaining 97.4%capacity after 300 cycles at 1 C.This work not only highlights the critical role of nanodot heterostructures in stabilizing CEI but also provides a new approach to designing high-voltage cathodes with superior interfacial compatibility and long-term durability.展开更多
Aqueous zinc-iodine(Zn-I_(2))batteries show great potential as energy storage candidates due to their high-safety and low-cost,but confronts hydrogen evolution reaction(HER)and dendrite growth at anode side and polyio...Aqueous zinc-iodine(Zn-I_(2))batteries show great potential as energy storage candidates due to their high-safety and low-cost,but confronts hydrogen evolution reaction(HER)and dendrite growth at anode side and polyiodide shuttling at cathode side.Herein,"tennis racket"(TR)hydrogel electrolytes were prepared by the co-polymerization and co-blending of polyacrylamide(PAM),sodium lignosulfonate(SL),and sodium alginate(SA)to synchronously regulate cathode and anode of Zn-I_(2)batteries."Gridline structure"of TR can induce the uniform transportation of Zn^(2+)ions through the coordination effect to hinder HER and dendrite growth at anode side,as well as hit I_(3)^(-)ions as"tennis"via the strong repulsion force to avoid shuttle effect at cathode side.The synergistic effect of TR electrolyte endows Zn-Zn symmetric battery with high cycling stability over 4500 h and Zn-I_(2)cell with the stably cycling life of 15000 cycles at5 A g^(-1),outperforming the reported works.The practicability of TR electrolyte is verified by flexible Zn-I_(2)pouch battery.This work opens a route to synchronously regulate cathode and anode to enhance the electrochemical performance of Zn-I_(2)batteries.展开更多
Aqueous zinc-ion batteries(AZIBs)are gaining attention owing to their affordability,high safety,and high energy density,making them a promising solution for large-scale energy storage.However,their performance is hamp...Aqueous zinc-ion batteries(AZIBs)are gaining attention owing to their affordability,high safety,and high energy density,making them a promising solution for large-scale energy storage.However,their performance is hampered by the instability of both the anode-electrolyte interface and the cathode-electrolyte interface.The use of sodium gluconate(SG),an organic sodium salt with multiple hydroxyl groups,as an electrolyte additive is suggested.Experimental and theoretical analyses demonstrate that Na^(+)from SG can intercalate and deintercalate within the associated V_(2)O_(5) cathode during in situ electrochemical processes.This action supports the layered structure of V_(2)O_(5),prevents structural collapse and phase transitions,and enhances Zn^(2+)diffusion kinetics.Additionally,the gluconate anion disrupts the original Zn^(2+)solvation structure,mitigates water-induced side reactions,and suppresses Zn dendrite growth.The synchronous regulation of both the V_(2)O_(5) cathode and Zn anode by the SG additive leads to considerable performance improvements.Zn‖Zn symmetric batteries demonstrate a cycle life exceeding 2800 h at 0.5 mA cm^(-2)and 1 mAh cm^(-2).In Zn‖V_(2)O_(5) full batteries,a high specific capacity of 288.92 mAh g^(-1)and capacity retention of 82.29%are maintained over 1000 cycles at a current density of 2 A g^(-1).This multifunctional additive strategy offers a new pathway for the practical application of AZIBs.展开更多
Aluminum(Al)exhibits excellent electrical conductivity,mechanical ductility,and good chemical compatibility with high-ionic-conductivity electrolytes.This makes it more suitable as an anode material for all-solid-stat...Aluminum(Al)exhibits excellent electrical conductivity,mechanical ductility,and good chemical compatibility with high-ionic-conductivity electrolytes.This makes it more suitable as an anode material for all-solid-state lithium batteries(ASSLBs)compared to the overly reactive metallic lithium anode and the mechanically weak silicon anode.This study finds that the pre-lithiated Al anode demonstrates outstanding interfacial stability with the Li_6PS_5Cl(LPSCl)electrolyte,maintaining stable cycling for over 1200 h under conditions of deep charge-discharge.This paper combines the pre-lithiated Al anode with a high-nickel cathode,LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2),paired with the highly ionic conductive LPSCl electrolyte,to design an ASSLB with high energy density and stability.Using anode pre-lithiation techniques,along with dual-reinforcement technology between the electrolyte and the cathode active material,the ASSLB achieves stable cycling for 1000 cycles at a 0.2C rate,with a capacity retention rate of up to 82.2%.At a critical negative-to-positive ratio of 1.1,the battery's specific energy reaches up to 375 Wh kg^(-1),and it maintains over 85.9%of its capacity after 100 charge-discharge cycles.This work provides a new approach and an excellent solution for developing low-cost,high-stability all-solid-state batteries.展开更多
Flat-panel X-ray sources(FPXSs)have many advantages in terms of compactness and low-dose imaging,enhancing their capability for novel X-ray applications.Experimental analysis of the X-ray characteristics and optimizin...Flat-panel X-ray sources(FPXSs)have many advantages in terms of compactness and low-dose imaging,enhancing their capability for novel X-ray applications.Experimental analysis of the X-ray characteristics and optimizing the anode panel of an FPXS are time-consuming,expensive,and sometimes impractical.In this study,a FPXS was prepared using a ZnO nanowire cold cathode and a molybdenum film anode target.Monte Carlo(MC)simulations were utilized to optimize the anode panel and obtain the average fluence,average energy,and spatial distribution of the X-rays for the ZnO nanowire FPXS.The accuracy of the MC simulations was verified by comparing the measured and simulated energy spectra.Optimization of the anode target considers the material,thickness,and morphology,whereas optimization of the substrate focuses on the material and thickness.The results show that the difference between the positions of the K-shell peaks in the measured and simulated energy spectra is within 0.26 keV.At the acceleration voltages of 30 kV,60 kV,and 90 kV,the optimal thicknesses of the tungsten array anode were 0.65μm,2.45μm,and 5μm,respectively,while the molybdenum array anode has the optimal thicknesses of 1.45μm,5.25μm,and 24μm,respectively.The microsemi-ellipsoidal anode with a recessed design showed a 5%increase in the transmitted X-ray fluence compared with the film target.The sapphire substrate with a thickness of 0.78 mm exhibits a mechanical strength comparable to that of a glass substrate with a thickness of 3 mm,implying that the former can increase the average X-ray fluence by reducing the filtration of X-rays.The findings of this study provide valuable guidance for the fabrication and optimization of the ZnO nanowire FPXS.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
Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density...Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density.However,their practical commercialization is hindered by critical challenges on the anode side,including dendrite growth and parasitic reactions at the anode/electrolyte interface.Recent studies highlight that rational electrolyte structure engineering offers an effective route to mitigate these issues and strengthen the electrochemical performance of the zinc metal anode.In this review,we systematically summarize state-of-the-art strategies for electrolyte optimization,with a particular focus on the zinc salts regulation,electrolyte additives,and the construction of novel electrolytes,while elucidating the underlying design principles.We further discuss the key structure–property relationships governing electrolyte behavior to provide guidance for the development of next-generation electrolytes.Finally,future perspectives on advanced electrolyte design are proposed.This review aims to serve as a comprehensive reference for researchers exploring high-performance electrolyte engineering in AZIBs.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
Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully syn...Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully synthesize nano-sized Wadsley-Roth FeNb_(11)O_(29)through Fe-driven phase transformation of Nb_(2)O_(5),which delivers a high specific capacity(280.5 mA h g^(−1)at 0.25 C)along with abundant redox-active sites.Moreover,the Wadsley-Roth shear structure of FeNb_(11)O_(29)facilitates rapid Li^(+)diffusion and guarantees exceptional structural stability.Theoretical calculations further confirm that FeNb_(11)O_(29)has a narrow band gap,which significantly enhances the conductivity.Owing to these merits,FeNb_(11)O_(29)achieves a full charge/discharge cycle within merely 25 s at 75 C rate and retains remarkable cycling stability over 2500 cycles.As a consequence,our assembled FeNb_(11)O_(29)||LiFePO_(4)full cell demonstrates ultra-long cyclability(>10000 cycles)and outstanding fast-charging capability(complete cycling within 2 min at 30 C).These findings highlight nano-sized FeNb_(11)O_(29)as a highly promising anode candidate for next-generation fast-charging LIBs.展开更多
Aqueous sodium-ion batteries(ASIBs)have attracted great attention in aqueous batteries due to their merit of high safety.However,the constrained work potential and insufficient chemical stability of anode materials in...Aqueous sodium-ion batteries(ASIBs)have attracted great attention in aqueous batteries due to their merit of high safety.However,the constrained work potential and insufficient chemical stability of anode materials in aqueous electro-lytes hinder the large-scale application of ASIBs.Sodium titanium phosphate,NaTi_(2)(PO_(4))_(3)(NTP),is considered one of the most promising anode materials for ASIBs due to its excellent electrochemical performance and tunable structure.Recently,great achievements have been made in the development of NTP,however,a comprehensive review of existing studies is still lacking.This article firstly introduces the basic properties of NTP and analyzes the existing challenges.Subsequently,it will provide a comprehensive overview of the key strategies related to the design and modification of NTP materials with optimized electrochemical performance.Finally,based on the current research status and practical needs,suggestions,and future perspectives for advancing NTP in practical applications of ASIBs are presented.This review aims to guide the future research trajectory from basic material innovation to industrial applications,thus promoting the large-scale commercializa-tion of ASIBs.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
Vanadium-based materials have emerged as promising cathode candidates for aqueous zinc-ion batteries(AZIBs)due to their multivalent redox characteristics and diverse crystal structures,which enable high energy storage...Vanadium-based materials have emerged as promising cathode candidates for aqueous zinc-ion batteries(AZIBs)due to their multivalent redox characteristics and diverse crystal structures,which enable high energy storage capacity.Nevertheless,practical applications are hindered by several critical challenges,including vanadium species dissolution,side-product formation,sluggish Zn^(2+)diffusion kinetics,and low electrical conductivity.Organic functionalization,benefiting from its structural tunability and abundant functional groups,has been proven to be an effective strategy for enhancing the electrochemical performance of vanadium-based cathodes.This review systematically summarizes recent advances in organic-functionalized vanadium-based cathodes.First,the energy storage mechanism of vanadiumbased cathodes and the fundamental properties of organic compounds relevant to cathode optimization are outlined.Then,the functions of organic compounds are comprehensively analyzed from four key perspectives:capacity improvement,conductivity enhancement,Zn^(2+)diffusion kinetics optimization,and cycling stability promotion.Furthermore,the specific electrochemical performance modulation effects and practical application examples of this strategy are discussed in detail.Finally,current limitations and challenges in this field are highlighted,and corresponding solutions and future research directions are proposed,offering theoretical guidance and insights for the development of high-performance vanadium-based cathodes for AZIBs.展开更多
Lithium(Li)dendrites,resulting from poor ion desolvation and transport behavior at the anode/electrolyte interface during electrodeposition,severely impede the practicality of Li metal anodes.Inspired by the transmemb...Lithium(Li)dendrites,resulting from poor ion desolvation and transport behavior at the anode/electrolyte interface during electrodeposition,severely impede the practicality of Li metal anodes.Inspired by the transmembrane cascade transport mechanism of biological ion pumps,we design a biomimetic dual-cascade separator(BDS)based on gradient pore core–shell Gd_(2)O_(3)@ZIF-7 nanoparticles to stabilize Li metal anodes.The mesoporous Gd_(2)O_(3)core,via Lewis acidic surface,weakens Li^(+) -solvent interactions,thereby reconstructing the solvation structure and achieving pre-desolvation.The microporous ZIF-7 shell then promotes final desolvation through strong confinement effect and N-rich site coordination,while its nanochannels homogenize Li^(+) transport.This synergistic meso/microporous gradient creates a unique dual-cascade effect for ion desolvation and transport.Consequently,BDS achieves a low desolvation energy barrier,a high Li^(+) transference number(0.71),and dendrite-free Li deposition.The average Coulombic efficiency rises from 72.7%to 98.4%,the cycling performance of the Li||Li symmetrical cell improves by 3.2 times,and the capacity retention of LiFePO_4(LFP)||Li full cell increases from 38.3%to73.4%after 500 cycles.This work offers a novel separator design concept,deepens Li deposition understanding,and guides separators from passive protection to active regulation.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
Parasitic interface side reactions and uncontrollable Zn deposition seriously erode the cycling performance of aqueous zinc ion batteries,thus impeding the large-scale application.Herein,an organic acid molecule with ...Parasitic interface side reactions and uncontrollable Zn deposition seriously erode the cycling performance of aqueous zinc ion batteries,thus impeding the large-scale application.Herein,an organic acid molecule with a unique molecular structure,camphorsulfonic acid(CSA),is first proposed to remodel the interface microenvironment as an electrolyte additive.The proton provided by CSA can neutralize the hydroxide ions generated by side reactions and inhibit the accumulation of alkaline by-products.The sulfonic acid groups are firmly adsorbed on the Zn anode surface,thereby enabling the regulation of interfacial species.Specifically,oxygen-containing functional groups combined with hydrophobic rigid carbon rings achieve a water-poor interface environment and promote the transfer of Zn^(2+),providing a suitable environment for Zn deposition.As a result,Zn//Zn symmetrical battery can run for over 2800 h(2 mA cm^(-2)-2 mAh cm^(-2)),demonstrating 28-times lifespan compared to the battery without CSA.Furthermore,Zn//KVO full cell presents excellent performance of 800 cycles at 3 A g^(-1).Besides,the pouch cell with CSA can also operate a capacity of 153.8 mAh after 60 cycles at 0.5 A g^(-1) with96.5%capacity retention rate.This work provides an organism-inspired additive selection for stabilizing the interface chemistry of the Zn anode.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
Lithium-rich manganese-based cathode materials,as promising candidates for next-generation highenergy–density lithium-ion batteries due to their high specific capacity(>250 mAh g^(-1))and costeffectiveness,are lim...Lithium-rich manganese-based cathode materials,as promising candidates for next-generation highenergy–density lithium-ion batteries due to their high specific capacity(>250 mAh g^(-1))and costeffectiveness,are limited by severe capacity decay and voltage fade driven by irreversible structural transitions and oxygen release during cycling.Here,we report a Ti/Si dual-element modification strategy for cobalt-free Li_(1.2)Ni_(0.2)Mn_(0.6)O_(2)(LNMO)cathodes.The Ti/Si co-modified TS-LNMO cathode demonstrates superior structural stability and electrochemical performance.Bulk Ti^(4+)doping stabilizes the oxygen framework via robust Ti–O bonds and enhances the lattice oxygen redox reversibility,while an in situ formed Li_(2) SiO_(3) layer suppresses interfacial side reactions,enhances lithium-ion diffusion,and prevents HF-induced erosion.As a result,the TS-LNMO cathode achieves 90%capacity retention after 200 cycles at 0.5 C and maintains -80%capacity in full cells cycled to 4.8 V.Additionally,the TS-LNMO cathode exhibits impressive rate performance even at a high rate of 5 C.This work offers an effective strategy for advancing cobalt-free,high-performance lithium-rich cathodes for sustainable energy applications.展开更多
文摘To control the power hierarchy design of lithium-ion battery(LIB)builtup sets for electric vehicles(EVs),we offer intensive theoretical and experimental sets of choice anode/cathode architectonics that can be modulated in full-scale LIB built-up models.As primary structural tectonics,heterogeneous composite superstructures of full-cell-LIB(anode//cathode)electrodes were designed in closely packed flower agave rosettes TiO2@C(FRTO@C anode)and vertical-star-tower LiFePO4@C(VST@C cathode)building blocks to regulate the electron/ion movement in the three-dimensional axes and orientation pathways.The superpower hierarchy surfaces and multi-directional orientation components may create isosurface potential electrodes with mobile electron movements,in-to-out interplay electron dominances,and electron/charge cloud distributions.This study is the first to evaluate the hotkeys of choice anode/cathode architectonics to assemble different LIB-electrode platforms with high-mobility electron/ion flows and high-performance capacity functionalities.Density functional theory calculation revealed that the FRTO@C anode and VST-(i)@C cathode architectonics are a superior choice for the configuration of full-scale LIB built-up models.The integrated FRTO@C//VST-(i)@C full-scale LIB retains a huge discharge capacity(~94.2%),an average Coulombic efficiency of 99.85%after 2000 cycles at 1 C,and a high energy density of 127 Wh kg?1,thereby satisfying scale-up commercial EV requirements.
基金supported by the National Natural Science Foundation of China(62201369,52203142)Natural Science Foundation of Sichuan Province(2024NSFSC0226)the Open Fund of Key Laboratory of Green Chemical Technology of Fujian Province University(WYKF-EIGT2023-1)。
文摘The advancement of aqueous zinc metal batteries(ZMBs)is constrained by intrinsic interfacial issues in aqueous electrolyte systems.Here,using numerical simulation,we decipher the multi-scale causes of interfacial instability,elucidating the synergistic effect of macroscopic ineffective regions and microscopic passivation.Based on the analysis,we develop an electrolyte-triggered interphase construction strategy to resolve the interfacial failure.This strategy couples the in situ formation of hydrogel interphase on both the anode and cathode with the electrolyte filling process,thereby(1)facilitating contact between electrodes and the separator;(2)promoting anode reversibility through inducing a bilayer SEI that enhances Zn^(2+)desolvation kinetics and blocks electron tunneling;(3)ensuring long-term cathode cycling stability via restricting the irreversible dissolution of MnO_(2)and side-reactions.The resultant Zn metal anode exhibited a near-unity Coulombic efficiency(99.5%)for Zn plating/stripping at an extremely low current density of 0.1 mA cm^(-2)and the Zn/MnO_(2)full cell sustained 2000 full-duty-cycles with an exceptionally low decay rate of 0.0051%per-cycle.This work unlocks an alternative angle for promoting practical ZMB s toward more sustainable energy storage systems.
基金the financial support from the National Key Research and Development Program of China(2023YFB2504000)。
文摘High-voltage Li-rich Mn-based oxide(LRMO)cathodes are promising for breaking through the energy density limits of lithium-ion batteries,yet their practical application remains limited by electrochemical performance degradation caused by unstable cathode-electrolyte interphase(CEI)evolution during longterm cycling.To address this issue,we propose a novel surface modification strategy using La_(0.7)Sr_(0.3)MnO_(3-σ)(LSMO)nanodots,which exhibit high electronic co nductivity and excellent corrosion resistance.These nanodots act as stable anchoring sites,facilitating the formation of a robust CEI on LRMO,The LSMOmodified cathode demonstrates significantly improved anionic redox reversibility,effectively mitigating transition metal migration and lattice oxygen loss.Furthermore,the optimized interfacial electrochemical kinetics ensure sustained rapid Li+diffusion throughout cycling,while the formation of a stable trilayer CEI structure suppresses electrolyte decomposition.Benefiting from these synergistic effects,the LSMO nanodot-engineered LRMO cathode delivers outstanding cycling stability,retaining 97.4%capacity after 300 cycles at 1 C.This work not only highlights the critical role of nanodot heterostructures in stabilizing CEI but also provides a new approach to designing high-voltage cathodes with superior interfacial compatibility and long-term durability.
基金financially supported by the Energy Revolution S&T Program of Yulin Innovation Institute of Clean Energy(E411060316)the NSFC-CONICFT Joint Project(51961125207)+1 种基金the Special Fund(2024)of Basic Scientific Research Project at Undergraduate University in Liaoning Province(LJ212410152056)the Foundation(GZKF202301)of State Key Laboratory of Biobased Material and Green Papermaking,Qilu University of Technology,Shandong Academy of Sciences。
文摘Aqueous zinc-iodine(Zn-I_(2))batteries show great potential as energy storage candidates due to their high-safety and low-cost,but confronts hydrogen evolution reaction(HER)and dendrite growth at anode side and polyiodide shuttling at cathode side.Herein,"tennis racket"(TR)hydrogel electrolytes were prepared by the co-polymerization and co-blending of polyacrylamide(PAM),sodium lignosulfonate(SL),and sodium alginate(SA)to synchronously regulate cathode and anode of Zn-I_(2)batteries."Gridline structure"of TR can induce the uniform transportation of Zn^(2+)ions through the coordination effect to hinder HER and dendrite growth at anode side,as well as hit I_(3)^(-)ions as"tennis"via the strong repulsion force to avoid shuttle effect at cathode side.The synergistic effect of TR electrolyte endows Zn-Zn symmetric battery with high cycling stability over 4500 h and Zn-I_(2)cell with the stably cycling life of 15000 cycles at5 A g^(-1),outperforming the reported works.The practicability of TR electrolyte is verified by flexible Zn-I_(2)pouch battery.This work opens a route to synchronously regulate cathode and anode to enhance the electrochemical performance of Zn-I_(2)batteries.
基金supported by the Battery Energy Storage Testing Center of Chongqing through their provision of testing support and technical assistance。
文摘Aqueous zinc-ion batteries(AZIBs)are gaining attention owing to their affordability,high safety,and high energy density,making them a promising solution for large-scale energy storage.However,their performance is hampered by the instability of both the anode-electrolyte interface and the cathode-electrolyte interface.The use of sodium gluconate(SG),an organic sodium salt with multiple hydroxyl groups,as an electrolyte additive is suggested.Experimental and theoretical analyses demonstrate that Na^(+)from SG can intercalate and deintercalate within the associated V_(2)O_(5) cathode during in situ electrochemical processes.This action supports the layered structure of V_(2)O_(5),prevents structural collapse and phase transitions,and enhances Zn^(2+)diffusion kinetics.Additionally,the gluconate anion disrupts the original Zn^(2+)solvation structure,mitigates water-induced side reactions,and suppresses Zn dendrite growth.The synchronous regulation of both the V_(2)O_(5) cathode and Zn anode by the SG additive leads to considerable performance improvements.Zn‖Zn symmetric batteries demonstrate a cycle life exceeding 2800 h at 0.5 mA cm^(-2)and 1 mAh cm^(-2).In Zn‖V_(2)O_(5) full batteries,a high specific capacity of 288.92 mAh g^(-1)and capacity retention of 82.29%are maintained over 1000 cycles at a current density of 2 A g^(-1).This multifunctional additive strategy offers a new pathway for the practical application of AZIBs.
基金the technical support for Nano-X from Suzhou Institute of Nano-Tech and NanoBionics,Chinese Academy of Sciences(SINANO)supported by the National Key R&D Program of China(2021YFB3800300)+2 种基金the National Natural Science Foundation of China(22179059,22239002,92372201)the science and technology innovation fund for emission peak and carbon neutrality of Jiangsu province(BK20231512,BK20220034)the Key R&D project funded by department of science and technology of Jiangsu Province(BE2020003)。
文摘Aluminum(Al)exhibits excellent electrical conductivity,mechanical ductility,and good chemical compatibility with high-ionic-conductivity electrolytes.This makes it more suitable as an anode material for all-solid-state lithium batteries(ASSLBs)compared to the overly reactive metallic lithium anode and the mechanically weak silicon anode.This study finds that the pre-lithiated Al anode demonstrates outstanding interfacial stability with the Li_6PS_5Cl(LPSCl)electrolyte,maintaining stable cycling for over 1200 h under conditions of deep charge-discharge.This paper combines the pre-lithiated Al anode with a high-nickel cathode,LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2),paired with the highly ionic conductive LPSCl electrolyte,to design an ASSLB with high energy density and stability.Using anode pre-lithiation techniques,along with dual-reinforcement technology between the electrolyte and the cathode active material,the ASSLB achieves stable cycling for 1000 cycles at a 0.2C rate,with a capacity retention rate of up to 82.2%.At a critical negative-to-positive ratio of 1.1,the battery's specific energy reaches up to 375 Wh kg^(-1),and it maintains over 85.9%of its capacity after 100 charge-discharge cycles.This work provides a new approach and an excellent solution for developing low-cost,high-stability all-solid-state batteries.
基金supported by the National Key Research and Development Program of China(Nos.2022YFA1204203 and 2022YFA1204201)Opening Fund of the State Key Laboratory of Optoelectronic Materials and Technologies at Sun Yat-sen University(No.OEMT-2023-KF-01)+1 种基金National Natural Science Foundation of China(Nos.61971463,82272131,and 82202960)the Guangdong Basic and Applied Basic Research Foundation(No.2023A1515010537).
文摘Flat-panel X-ray sources(FPXSs)have many advantages in terms of compactness and low-dose imaging,enhancing their capability for novel X-ray applications.Experimental analysis of the X-ray characteristics and optimizing the anode panel of an FPXS are time-consuming,expensive,and sometimes impractical.In this study,a FPXS was prepared using a ZnO nanowire cold cathode and a molybdenum film anode target.Monte Carlo(MC)simulations were utilized to optimize the anode panel and obtain the average fluence,average energy,and spatial distribution of the X-rays for the ZnO nanowire FPXS.The accuracy of the MC simulations was verified by comparing the measured and simulated energy spectra.Optimization of the anode target considers the material,thickness,and morphology,whereas optimization of the substrate focuses on the material and thickness.The results show that the difference between the positions of the K-shell peaks in the measured and simulated energy spectra is within 0.26 keV.At the acceleration voltages of 30 kV,60 kV,and 90 kV,the optimal thicknesses of the tungsten array anode were 0.65μm,2.45μm,and 5μm,respectively,while the molybdenum array anode has the optimal thicknesses of 1.45μm,5.25μm,and 24μm,respectively.The microsemi-ellipsoidal anode with a recessed design showed a 5%increase in the transmitted X-ray fluence compared with the film target.The sapphire substrate with a thickness of 0.78 mm exhibits a mechanical strength comparable to that of a glass substrate with a thickness of 3 mm,implying that the former can increase the average X-ray fluence by reducing the filtration of X-rays.The findings of this study provide valuable guidance for the fabrication and optimization of the ZnO nanowire FPXS.
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supported by the Natural Science Foundation of China(Nos.52125202,52202100,and U24A2065)the Natural Science Foundation of Jiangsu Province(BK20243016)Fundamental Research Funds for the Central Universities,China Postdoctoral Science Foundation(No.2024T171166).
文摘Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density.However,their practical commercialization is hindered by critical challenges on the anode side,including dendrite growth and parasitic reactions at the anode/electrolyte interface.Recent studies highlight that rational electrolyte structure engineering offers an effective route to mitigate these issues and strengthen the electrochemical performance of the zinc metal anode.In this review,we systematically summarize state-of-the-art strategies for electrolyte optimization,with a particular focus on the zinc salts regulation,electrolyte additives,and the construction of novel electrolytes,while elucidating the underlying design principles.We further discuss the key structure–property relationships governing electrolyte behavior to provide guidance for the development of next-generation electrolytes.Finally,future perspectives on advanced electrolyte design are proposed.This review aims to serve as a comprehensive reference for researchers exploring high-performance electrolyte engineering in AZIBs.
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financially supported by the National Natural Science Foundation of China (52272209)
文摘Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully synthesize nano-sized Wadsley-Roth FeNb_(11)O_(29)through Fe-driven phase transformation of Nb_(2)O_(5),which delivers a high specific capacity(280.5 mA h g^(−1)at 0.25 C)along with abundant redox-active sites.Moreover,the Wadsley-Roth shear structure of FeNb_(11)O_(29)facilitates rapid Li^(+)diffusion and guarantees exceptional structural stability.Theoretical calculations further confirm that FeNb_(11)O_(29)has a narrow band gap,which significantly enhances the conductivity.Owing to these merits,FeNb_(11)O_(29)achieves a full charge/discharge cycle within merely 25 s at 75 C rate and retains remarkable cycling stability over 2500 cycles.As a consequence,our assembled FeNb_(11)O_(29)||LiFePO_(4)full cell demonstrates ultra-long cyclability(>10000 cycles)and outstanding fast-charging capability(complete cycling within 2 min at 30 C).These findings highlight nano-sized FeNb_(11)O_(29)as a highly promising anode candidate for next-generation fast-charging LIBs.
基金supported by the Natural Sci-ence Foundation of Fujian Province (No.2024J011210)the High-Level Talent Start-Up Foundation of Xiamen Institute of Technology (No.YKJ23017R)。
文摘Aqueous sodium-ion batteries(ASIBs)have attracted great attention in aqueous batteries due to their merit of high safety.However,the constrained work potential and insufficient chemical stability of anode materials in aqueous electro-lytes hinder the large-scale application of ASIBs.Sodium titanium phosphate,NaTi_(2)(PO_(4))_(3)(NTP),is considered one of the most promising anode materials for ASIBs due to its excellent electrochemical performance and tunable structure.Recently,great achievements have been made in the development of NTP,however,a comprehensive review of existing studies is still lacking.This article firstly introduces the basic properties of NTP and analyzes the existing challenges.Subsequently,it will provide a comprehensive overview of the key strategies related to the design and modification of NTP materials with optimized electrochemical performance.Finally,based on the current research status and practical needs,suggestions,and future perspectives for advancing NTP in practical applications of ASIBs are presented.This review aims to guide the future research trajectory from basic material innovation to industrial applications,thus promoting the large-scale commercializa-tion of ASIBs.
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financial support from the National Natural Science Foundation of China(No.21676036)the Natural Science Foundation of Chongqing(No.CSTB2023NSCQMSX0580)the Large-scale Equipment Sharing Fund of Chongqing University(No.202403150240 and 202503150091)。
文摘Vanadium-based materials have emerged as promising cathode candidates for aqueous zinc-ion batteries(AZIBs)due to their multivalent redox characteristics and diverse crystal structures,which enable high energy storage capacity.Nevertheless,practical applications are hindered by several critical challenges,including vanadium species dissolution,side-product formation,sluggish Zn^(2+)diffusion kinetics,and low electrical conductivity.Organic functionalization,benefiting from its structural tunability and abundant functional groups,has been proven to be an effective strategy for enhancing the electrochemical performance of vanadium-based cathodes.This review systematically summarizes recent advances in organic-functionalized vanadium-based cathodes.First,the energy storage mechanism of vanadiumbased cathodes and the fundamental properties of organic compounds relevant to cathode optimization are outlined.Then,the functions of organic compounds are comprehensively analyzed from four key perspectives:capacity improvement,conductivity enhancement,Zn^(2+)diffusion kinetics optimization,and cycling stability promotion.Furthermore,the specific electrochemical performance modulation effects and practical application examples of this strategy are discussed in detail.Finally,current limitations and challenges in this field are highlighted,and corresponding solutions and future research directions are proposed,offering theoretical guidance and insights for the development of high-performance vanadium-based cathodes for AZIBs.
基金the financial support from the National Natural Science Foundation of China(22408182)the Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region(NJYT24024)the Natural Science Foundation of Inner Mongolia Autonomous Region(2023QN02007 and 2025QN02009)。
文摘Lithium(Li)dendrites,resulting from poor ion desolvation and transport behavior at the anode/electrolyte interface during electrodeposition,severely impede the practicality of Li metal anodes.Inspired by the transmembrane cascade transport mechanism of biological ion pumps,we design a biomimetic dual-cascade separator(BDS)based on gradient pore core–shell Gd_(2)O_(3)@ZIF-7 nanoparticles to stabilize Li metal anodes.The mesoporous Gd_(2)O_(3)core,via Lewis acidic surface,weakens Li^(+) -solvent interactions,thereby reconstructing the solvation structure and achieving pre-desolvation.The microporous ZIF-7 shell then promotes final desolvation through strong confinement effect and N-rich site coordination,while its nanochannels homogenize Li^(+) transport.This synergistic meso/microporous gradient creates a unique dual-cascade effect for ion desolvation and transport.Consequently,BDS achieves a low desolvation energy barrier,a high Li^(+) transference number(0.71),and dendrite-free Li deposition.The average Coulombic efficiency rises from 72.7%to 98.4%,the cycling performance of the Li||Li symmetrical cell improves by 3.2 times,and the capacity retention of LiFePO_4(LFP)||Li full cell increases from 38.3%to73.4%after 500 cycles.This work offers a novel separator design concept,deepens Li deposition understanding,and guides separators from passive protection to active regulation.
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financially supported by The Excellent Youth Project of the Education Department of Hunan Province(No.24B0008)the National Natural Science Foundation of China(No.52377222)。
文摘Parasitic interface side reactions and uncontrollable Zn deposition seriously erode the cycling performance of aqueous zinc ion batteries,thus impeding the large-scale application.Herein,an organic acid molecule with a unique molecular structure,camphorsulfonic acid(CSA),is first proposed to remodel the interface microenvironment as an electrolyte additive.The proton provided by CSA can neutralize the hydroxide ions generated by side reactions and inhibit the accumulation of alkaline by-products.The sulfonic acid groups are firmly adsorbed on the Zn anode surface,thereby enabling the regulation of interfacial species.Specifically,oxygen-containing functional groups combined with hydrophobic rigid carbon rings achieve a water-poor interface environment and promote the transfer of Zn^(2+),providing a suitable environment for Zn deposition.As a result,Zn//Zn symmetrical battery can run for over 2800 h(2 mA cm^(-2)-2 mAh cm^(-2)),demonstrating 28-times lifespan compared to the battery without CSA.Furthermore,Zn//KVO full cell presents excellent performance of 800 cycles at 3 A g^(-1).Besides,the pouch cell with CSA can also operate a capacity of 153.8 mAh after 60 cycles at 0.5 A g^(-1) with96.5%capacity retention rate.This work provides an organism-inspired additive selection for stabilizing the interface chemistry of the Zn anode.
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supported by the National Natural Science Foundation of China(22379084)Department of Science and Technology of Guangdong Province(211233812024)Shenzhen Science and Technology Program(JCYJ20220818101007016,KJZD20240903101303005)。
文摘Lithium-rich manganese-based cathode materials,as promising candidates for next-generation highenergy–density lithium-ion batteries due to their high specific capacity(>250 mAh g^(-1))and costeffectiveness,are limited by severe capacity decay and voltage fade driven by irreversible structural transitions and oxygen release during cycling.Here,we report a Ti/Si dual-element modification strategy for cobalt-free Li_(1.2)Ni_(0.2)Mn_(0.6)O_(2)(LNMO)cathodes.The Ti/Si co-modified TS-LNMO cathode demonstrates superior structural stability and electrochemical performance.Bulk Ti^(4+)doping stabilizes the oxygen framework via robust Ti–O bonds and enhances the lattice oxygen redox reversibility,while an in situ formed Li_(2) SiO_(3) layer suppresses interfacial side reactions,enhances lithium-ion diffusion,and prevents HF-induced erosion.As a result,the TS-LNMO cathode achieves 90%capacity retention after 200 cycles at 0.5 C and maintains -80%capacity in full cells cycled to 4.8 V.Additionally,the TS-LNMO cathode exhibits impressive rate performance even at a high rate of 5 C.This work offers an effective strategy for advancing cobalt-free,high-performance lithium-rich cathodes for sustainable energy applications.
