Currently,the effective and clean suppression of lithium-ion battery(LIB)fires remains a challenge.The present work investigates the use of various inhibitor doses(Xin)of dodecafluoro-2-methylpentan-3-one(C_(6) F_(12)...Currently,the effective and clean suppression of lithium-ion battery(LIB)fires remains a challenge.The present work investigates the use of various inhibitor doses(Xin)of dodecafluoro-2-methylpentan-3-one(C_(6) F_(12)O)in 300 Ah LIBs,and systematically examines the thermal and toxic hazards of the extinguished batteries via real scale combustion and gas analysis.The inhibitor is shown to be completely effective.The inhibition mechanism involves a combination of chemical inhibition and physical cooling.While the chemical inhibition effect tends to saturate with increasing Xin,the physical cooling remains effective at higher inhibitor doses.However,extinguishing the battery fire with a high Xin of C_(6)F_(12)O is found to incur serious toxicity problems.These results are expected to provide a guideline for the design of inhibitor doses for the suppression of LIB fires.展开更多
Lithium ion batteries(LIB)can rupture and result in thermal runaway and battery fires.In the process of transporting lithium ion batteries using trains,the massive collection of batteries can cause train fire and pose...Lithium ion batteries(LIB)can rupture and result in thermal runaway and battery fires.In the process of transporting lithium ion batteries using trains,the massive collection of batteries can cause train fire and pose significant danger to the public.This is especially critical when the fire occurs amid a heavily populated metropolitan environment.This paper reports the 3D analysis of a warehouse with possible train fire due to LIB rupture and the fire propagation at a rail yard.Six critical fire cases with the battery train in close vicinity to the warehouse were considered.The six fire cases are the worst-case scenarios of a Monte Carlo simulation of different fire cases that may occur to an actual steel storage facility at the Capital Railyard,Raleigh,North Carolina.A 3D finite element(FE)frame model was constructed for the steel warehouse and the most critical fire cases were simulated.The results indicated that several structural components of the warehouse would experience large stresses and deflections during the simulated battery fires and resulting in instability to the structure.Specifically,members of the roof frame represent the most critical elements and that the members can result in large deformations as early as 4 minutes after the fire starts.Furthermore,effective utilization of fire protection can delay somewhat the fire effects and extend time to failure to 45 minutes and in one of the simulated cases,prevent structural instability.Thus,fire from LIB waste transport using train is a very realistic problem due to the thermal runaway,and the analysis performed in current study can be used as a preventive investigation technique for buildings that may be exposed to the train fire risk.展开更多
Each morning at Yangluo Port in Wuhan,Hubei Province,the all-electric cargo vessel Huahang Xinneng No.1 completes a battery swap in under 10 minutes before returning to service with nearly 8,000 kWh of power onboard。
The growing use of lithium-ion batteries in electric transportation and grid-scale storage systems has intensified the need for accurate and highly generalizable state-of-health(SOH)estimation.Conventional approaches ...The growing use of lithium-ion batteries in electric transportation and grid-scale storage systems has intensified the need for accurate and highly generalizable state-of-health(SOH)estimation.Conventional approaches often suffer from reduced accuracy under dynamically uncertain state-of-charge(SOC)operating ranges and heterogeneous aging stresses.This study presents a unified SOH estimation framework that integrates physics-informed modeling,subspace identification,and Transformer-based learning.A reduced-order model is derived from simplified electrochemical dynamics,providing an interpretable and computationally efficient representation of battery behavior.Subspace identification across a wide SOC and SOH range yields degradation-sensitive features,which the Transformer uses to capture long-range aging dynamics via multi-head self-attention.Experiments on LiFePO4 cells under joint-cell training show consistently accurate SOH estimation,with a maximum error of 1.39%,demonstrating the framework’s effectiveness in decoupling SOC and SOH effects.In cross-cell validation,where training and validation are performed on different cells,the model maintains a maximum error of 2.06%,confirming strong generalization to unseen aging trajectories.Comparative experiments on LiFePO_(4)and public LiCoO_(2)datasets confirm the framework’s cross-chemistry applicability.By extracting low-dimensional,physically interpretable features via subspace identification,the framework significantly reduces training cost while maintaining high SOH estimation accuracy,outperforming conventional data-driven models lacking physical guidance.展开更多
Aqueous Zn-iodine batteries(ZIBs)face the formidable challenges towards practical implementation,including metal corrosion and rampant dendrite growth on the Zn anode side,and shuttle effect of polyiodide species from...Aqueous Zn-iodine batteries(ZIBs)face the formidable challenges towards practical implementation,including metal corrosion and rampant dendrite growth on the Zn anode side,and shuttle effect of polyiodide species from the cathode side.These challenges lead to poor cycle stability and severe self-discharge.From the fabrication and cost point of view,it is technologically more viable to deploy electrolyte engineering than electrode protection strategies.More importantly,a synchronous method for modulation of both cathode and anode is pivotal,which has been often neglected in prior studies.In this work,cationic poly(allylamine hydrochloride)(Pah^(+))is adopted as a low-cost dual-function electrolyte additive for ZIBs.We elaborate the synchronous effect by Pah^(+)in stabilizing Zn anode and immobilizing polyiodide anions.The fabricated Zn-iodine coin cell with Pah^(+)(ZnI_(2) loading:25 mg cm^(−2))stably cycles 1000 times at 1 C,and a single-layered 3.4 cm^(2) pouch cell(N/P ratio~1.5)with the same mass loading cycles over 300 times with insignificant capacity decay.展开更多
Lithium-sulfur(Li-S)batteries boast a theoretical energy density as high as 2600 Wh·kg^(−1),positioning them as a highly attractive option for future advanced energy storage systems.Challenges such as slow transf...Lithium-sulfur(Li-S)batteries boast a theoretical energy density as high as 2600 Wh·kg^(−1),positioning them as a highly attractive option for future advanced energy storage systems.Challenges such as slow transformation kinetics and shuttle effects associated with lithium polysulfides(LiPSs)have seriously hindered their practical applications.In this paper,we present a new method for the synthesis of hollow carbon-sphere-supported Co monatomic catalysts(Co-N-C).This new synthesis method achieves pyrolytic coordination using a precursor rich in imide(-RC=N-)polymers.This synthesis method not only improves the adsorbability and catalytic activity of LiPS but also significantly weakens the shuttle effect and generates Co-N-C with superior conductivity,abundant hollow structures,and a high specific surface area,thus efficiently capturing and restricting the movement of LiPS intermediates.The dispersed Co monoatomic catalysts(Co SACs)were anchored to a highly conductive nitrogen-doped carbon framework and exhibited symmetric N-coordination active sites(Co-N_(4))to ensure fast redox kinetics of LiPS and Li_(2)S_(2)/Li_(2)S solid-state products.The lithium-sulfur battery with Co-N-C as the sulfur carrier showed excellent discharging capacity of 1146.6 mAh·g^(−1) at a discharge rate of 0.5 C and maintained excellent performance at a high discharge rate of 2 C.The capacity decay rate in 500 cycles was only 0.086%per cycle,reflecting excellent long-term cycle stability.This study highlights the key role of the synergistic effect between single-atom cobalt catalysts and hollow carbon spheres in enhancing the efficiency of lithium-sulfur(Li-S)batteries.It also provides valuable insights into the construction and fabrication of highly active monatomic catalysts.The catalytic conversion efficiency of lithium polysulfides is significantly enhanced when embedded in hollow carbon architectures,which serves as a critical strategy for optimizing the electrochemical behavior of next-generation Li-S batteries.展开更多
Lithium-ion batteries(LIBs)are widely deployed,from grid-scale storage to electric vehicles.LIBs remain stationary most of their service life,where calendar aging degrades capacity.Understanding the mechanisms of LIB ...Lithium-ion batteries(LIBs)are widely deployed,from grid-scale storage to electric vehicles.LIBs remain stationary most of their service life,where calendar aging degrades capacity.Understanding the mechanisms of LIB calendar aging is crucial for extending battery lifespan.However,LIB calendar aging is influenced by multiple factors,including battery material,its state,and storage environment.Calendar aging experiments are also time-consuming,costly,and lack standardized testing conditions.This study employs a data-driven approach to establish a cross-scale database linking materials,side-reaction mechanisms,and calendar aging of LIBs.MELODI(Mechanism-informed,Explainable,Learning-based Optimization for Degradation Identification)is proposed to identify calendar aging mechanisms and quantify the effects of multi-scale factors.Results reveal that cathode material loss drives up to 91.42%of calendar aging degradation in high-nickel(Ni)batteries,while solid electrolyte interphase growth dominates in lithium iron phosphate(LFP)and low-Ni batteries,contributing up to 82.43%of degradation in LFP batteries and 99.10%of decay in low-Ni batteries,respectively.This study systematically quantifies calendar aging in commercial LIBs under varying materials,states of charge,and temperatures.These findings offer quantitative guidance for experimental design or battery use,and implications for emerging applications like aerial robotics,vehicle-to-grid,and embodied intelligence systems.展开更多
Conversion of ammonia into hydrogen,a crucial pathway for the hydrogen economy,is severely constrained by the intricacy of the required equipment and the low efficiency.Herein,Pd@Pt Ni Co Ru Ir coreshell mesoporous bi...Conversion of ammonia into hydrogen,a crucial pathway for the hydrogen economy,is severely constrained by the intricacy of the required equipment and the low efficiency.Herein,Pd@Pt Ni Co Ru Ir coreshell mesoporous bifunctional electrocatalysts were fabricated via a one-step wet-chemical reduction approach.By utilizing the limiting effect of triblock copolymers,gradient distribution control of six metal elements(Pd core and Pt/Ni/Co/Ru/Ir high-entropy alloys shell) was achieved,where the high-entropy alloy shell forms high-density active sites through lattice distortion effect.With the help of lattice distortion and mesoporous-confinement-enabled interfacial coupling effects,Pd@Pt Ni Co Ru Ir catalyst exhibited exceptional bifunctional performance in alkaline media:A low hydrogen evolution reaction(HER) overpotential of 30.5 m V at 10 m A/cm^(2) and a high ammonia oxidation reaction(AOR) peak current density of 19.6 m A/cm^(2) at 0.7 V vs.RHE,representing a 3.83-fold enhancement over commercial Pt/C.Moreover,a rechargeable Zn-NH_(3) battery system was constructed and achieved 92.3 % Faradaic efficiency(FE) for NH_(3)-to-H_(2) conversion with outstanding stability at 16 m A/cm^(2),thereby providing an innovative solution for efficient ammonia decomposition-based hydrogen production.展开更多
The pseudo-two-dimensional(P2D)model plays an important role in exploring physicochemical mechanisms,predicting the state of health,and improving the fast charge capability for Li-ion batteries(LIBs).However,the fast ...The pseudo-two-dimensional(P2D)model plays an important role in exploring physicochemical mechanisms,predicting the state of health,and improving the fast charge capability for Li-ion batteries(LIBs).However,the fast charge leads to the lithium concentration gradient in the solid and electrolyte phases and the non-uniform electrochemical reaction at the solid/electrolyte interface.In order to decouple charge transfer reactions in LIBs under dynamic conditions,understanding the spatio-temporal resolution of the P2D model is urgently required.Till now,the study of this aspect is still insufficient.This work studies the spatio-temporal resolution for dynamic/static electrochemical impedance spectroscopy(DEIS/SEIS)on multiple scales.In detail,DEIS and SEIS with spatio-temporal resolutions are used to decouple charge transfer reactions in LIBs based on the numerical solution of the P2D model in the frequency domain.The calculated results indicate that decoupling solid diffusion requires a high spatial resolution along the r-direction in particles,decoupling electrolyte diffusion and interfacial transfer reaction requires a high spatial resolution along the x-direction,and decoupling charge transfer reactions in LIBs at an extremely low state of charge(SOC)requires an extremely high temporal resolution along the t-direction.Finally,the optimal range of spatio-temporal resolutions for DEIS/SEIS is derived,and the method to decouple charge transfer reactions with spatio-temporal resolutions is developed.展开更多
Developing high-performance Ni cathodes and understanding the relationship between electron states of Ni 3d orbital and energy storage mechanism from an atomic-orbital perspective are crucial yet challenging for alkal...Developing high-performance Ni cathodes and understanding the relationship between electron states of Ni 3d orbital and energy storage mechanism from an atomic-orbital perspective are crucial yet challenging for alkaline nickel-zinc batteries.Herein,we innovatively design P-NiMoO_(4)/NiSe_(2)heterostructures with rich oxygen vacancy via a selective component segregation.The P substitution in NiMoO_(4)activate Ni atoms,leading to the spin-state transition of Ni-3d orbitals from high-spin to low-spin,which promote the uniform and rapid nucleation of NiSe_(2)on the surface of NiMoO_(4)during subsequent selenization process.After selenization,the in situ formed P-NiMoO_(4)/NiSe_(2)heterostructures exhibits continuous increased unoccupied states of Ni 3d-orbitals and higher Ni valence state.The synergistic effect of P doping and selenization modulate the d-band center(ɛd)level of Ni 3d,thereby promoting d-p orbital hybridization between Ni 3d and O 2p of OH−as well as OH−adsorption ability.Consequently,the P-NiMoO_(4)/NiSe_(2)exhibits a top-level specific capacity of 390.7 mA h g^(−1)at 1 A g^(−1),2.8-fold higher than that of pristine NiMoO_(4),accompanied by remarkable rate capability and structural stability.Moreover,the assembled pouch-type battery and flexible devices demonstrate the practical application potential.This work provides fundamental insights into orbital-level engineering of battery materials for enhanced redox kinetics and cycling stability.展开更多
The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulat...The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulate the electronic structure of MoS_(2),thereby obtaining a multifunctional catalyst that serves as an efficient sulfur host.The W/V dual single-atomdoped MoS_(2)grown on carbon nanofibers(CMWVS)demonstrates a strong adsorption ability for lithium polysulfides,suppressing the shuttle effects.Additionally,the doping process also results in the phase transition from 2H-MoS_(2)to 1T-MoS_(2)and generates sufficient edge sulfur atoms,promoting the charge/electron transfer and enriching the reaction sites.All these merits contribute to the superior conversion reaction kinetics,leading to the outstanding Li-S battery performance.When fabricated as cathodes by compositing with sulfur,the CMWVS/S cathode delivers a high capacity of 1481.7 mAh g^(-1)at 0.1 C(1 C=1672 mAh g^(-1))and maintains 816.3 m Ah g^(-1)after 1000 cycles at 1.0 C,indicating outstanding cycling stability.Even under a high sulfur loading of 7.9 mg cm^(-2)and lean electrolyte conditions(E/S ratio of 9.0μL mg^(-1)),the cathode achieves a high areal capacity of 8.2 m Ah cm^(-2),showing great promise for practical Li-S battery applications.This work broadens the scope of doping strategies in transition-metal dichalcogenides by tailoring their electronic structures,providing insightful direction for the rational development of high-efficiency electrocatalysts for advanced Li-S battery applications.展开更多
Single-atom catalysts(SACs)have garnered significant attention in lithium-sulfur(Li-S)batteries for their potential to mitigate the severe polysulfide shuttle effect and sluggish redox kinetics.However,the development...Single-atom catalysts(SACs)have garnered significant attention in lithium-sulfur(Li-S)batteries for their potential to mitigate the severe polysulfide shuttle effect and sluggish redox kinetics.However,the development of highly efficient SACs and a comprehensive understanding of their structure-activity relationships remain enormously challenging.Herein,a novel kind of Fe-based SAC featuring an asymmetric FeN_(5)-TeN_(4) coordination structure was precisely designed by introducing Te atom adjacent to the Fe active center to enhance the catalytic activity.Theoretical calculations reveal that the neighboring Te atom modulates the local coordination environment of the central Fe site,elevating the d-band center closer to the Fermi level and strengthening the d-p orbital hybridization between the catalyst and sulfur species,thereby immobilizing polysulfides and improving the bidirectional catalysis of Li-S redox.Consequently,the Fe-Te atom pair catalyst endows Li-S batteries with exceptional rate performance,achieving a high specific capacity of 735 mAh g^(−1) at 5 C,and remarkable cycling stability with a low decay rate of 0.038%per cycle over 1000 cycles at 1 C.This work provides fundamental insights into the electronic structure modulation of SACs and establishes a clear correlation between precisely engineered atomic configurations and their enhanced catalytic performance in Li-S electrochemistry.展开更多
To ease the scarcity of lithium(Li)resource and cut down on environmental pollution,an efficient,selective,inexpensive and sustainable Li recycling process from waste batteries is needed,which is yet to be achieved.He...To ease the scarcity of lithium(Li)resource and cut down on environmental pollution,an efficient,selective,inexpensive and sustainable Li recycling process from waste batteries is needed,which is yet to be achieved.Here,we report a low-potential photoelectrochemical(PEC)system that selectively and efficiently extracts Li metals from multi-cation electrolytes under 1 sun illumination.Based on the difference of redox potential,we can get rid of the disturbance of other cations(i.e.,Fe,Co and Ni ions)by a bias-free PEC device to realize the extraction of high-purity Li metals on a coplanar Si-based photocathode-TiO_(2) photoanode tandem device at 2 V of applied bias(far less than the redox potentials of Li^(+)/Li).In such system,the extraction rate of Li metals(purity>99.5%)exceeds 1.35 g h^(-1)m^(-2)with 90%of Faradaic efficiency.Long-term experiments,different electrode/electrolyte tests,and various price assessments further demonstrate the stability,compatibility and economy of PEC extraction system,enabling a solar-driven pathway for the recycling of critical metal resources.展开更多
Rechargeable Zn/Sn-air batteries have received considerable attention as promising energy storage devices.However,the electrochemical performance of these batteries is significantly constrained by the sluggish electro...Rechargeable Zn/Sn-air batteries have received considerable attention as promising energy storage devices.However,the electrochemical performance of these batteries is significantly constrained by the sluggish electrocatalytic reaction kinetics at the cathode.The integration of light energy into Zn/Sn-air batteries is a promising strategy for enhancing their performance.However,the photothermal and photoelectric effects generate heat in the battery under prolonged solar irradiation,leading to air cathode instability.This paper presents the first design and synthesis of Ni_(2)-1,5-diamino-4,8-dihydroxyanthraquinone(Ni_(2)DDA),an electronically conductiveπ-d conjugated metal-organic framework(MOF).Ni_(2)DDA exhibits both photoelectric and photothermal effects,with an optical band gap of~1.14 eV.Under illumination,Ni_(2)DDA achieves excellent oxygen evolution reaction performance(with an overpotential of 245 mV vs.reversible hydrogen electrode at 10 mA cm^(−2))and photothermal stability.These properties result from the synergy between the photoelectric and photothermal effects of Ni_(2)DDA.Upon integration into Zn/Sn-air batteries,Ni_(2)DDA ensures excellent cycling stability under light and exhibits remarkable performance in high-temperature environments up to 80℃.This study experimentally confirms the stable operation of photo-assisted Zn/Sn-air batteries under high-temperature conditions for the first time and provides novel insights into the application of electronically conductive MOFs in photoelectrocatalysis and photothermal catalysis.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
Poly(ethylene oxide)(PEO)and its derivatives based gel polymer electrolytes(GPEs)are severely limited in advanced and safe lithium-ion batteries(LIBs)owing to the intrinsically high flammability of liquid electrolytes...Poly(ethylene oxide)(PEO)and its derivatives based gel polymer electrolytes(GPEs)are severely limited in advanced and safe lithium-ion batteries(LIBs)owing to the intrinsically high flammability of liquid electrolytes and PEO.Directly adding flame retardants to the GPEs can suppress their flammability and thus improve the safety of LIBs,but results in deteriorative electrochemical performance.Herein,a novel GPE with chemically bonded flame retardant(i.e.diethyl vinylphosphonate)in cross-linked polyethylene glycol diacrylate matrix,featuring both high-safety and high-performance,is designed.This as-prepared GPE storing the commercial 1 mol L^(-1) LiPF6 electrolyte resists high temperature of 200℃and cannot be ignited as well as possesses a high ionic conductivity(0.60 m S cm^(-1))and good compatibility with lithium.Notably,the LiFePO_(4)/Li battery with this GPE delivers a satisfactory capacity of 142.2 m A h g^(-1) and a superior cycling performance with a capacity retention of 96.3%and a coulombic efficiency of close to 100%for 350 cycles at 0.2 C under ambient temperature.Furthermore,the battery can achieve steady charge–discharge for 100 cycles with a coulombic efficiency of 99.5%at 1 C under 80℃and run normally even at a high temperature of 150℃or under the exposure to butane flame.Differential scanning calorimetry manifests significantly improved battery safety compared to commercial battery systems.This work provides a new pathway for developing next-generation advanced LIBs with enhanced performance and high safety.展开更多
Battery safety has attracted considerable attention worldwide due to the rapid development of wearable electronics and the steady increase in the production and use of electric vehicles.As battery failures are often a...Battery safety has attracted considerable attention worldwide due to the rapid development of wearable electronics and the steady increase in the production and use of electric vehicles.As battery failures are often associated with mechanical-thermal coupled behaviors,protective shielding materials with excellent mechanical robustness and flame-retardant properties are highly desired to mitigate thermal runaway.However,most of the thermal insulating materials are not strong enough to protect batteries from mechanical abuse,which is one of the most critical scenarios with catastrophic consequences.Here,inspired by wood,we have developed an effective approach to engineer a hierarchical nanocomposite via self-assembly of calcium silicate hydrate and polyvinyl alcohol polymer chains(referred as CSH wood).The versatile protective material CSH wood demonstrates an unprecedented combination of light weight(0.018 g cm-3),high stiffness(204 MPa in the axial direction),negative Poisson's ratio(-0.15),remarkable toughness(6.67×105 J m-3),superior thermal insulation(0.0204 W m-1 K-1 in the radial direction),and excellent fire retardancy(UL94-V0).When applied as a protective cover or a protective layer within battery packages,the tough CSH wood can resist high-impact load and block heat diffusion to block or delay the spread of fire,therefore significantly reducing the risk of property damage or bodily injuries caused by battery explosions.This work provides new pathways for fabricating advanced thermal insulating materials with large scalability and demonstrates great potential for the protection of electronic devices.展开更多
Na-ion batteries are considered a promising next-generation battery alternative to Li-ion batteries,due to the abundant Na resources and low cost.Most efforts focus on developing new materials to enhance energy densit...Na-ion batteries are considered a promising next-generation battery alternative to Li-ion batteries,due to the abundant Na resources and low cost.Most efforts focus on developing new materials to enhance energy density and electrochemical performance to enable it comparable to Li-ion batteries,without considering thermal hazard of Na-ion batteries and comparison with Li-ion batteries.To address this issue,our work comprehensively compares commercial prismatic lithium iron phosphate(LFP) battery,lithium nickel cobalt manganese oxide(NCM523) battery and Na-ion battery of the same size from thermal hazard perspective using Accelerating Rate Calorimeter.The thermal hazard of the three cells is then qualitatively assessed from thermal stability,early warning and thermal runaway severity perspectives by integrating eight characteristic parameters.The Na-ion cell displays comparable thermal stability with LFP while LFP exhibits the lowest thermal runaway hazard and severity.However,the Na-ion cell displays the lowest safety venting temperature and the longest time interval between safety venting and thermal runaway,allowing the generated gas to be released as early as possible and detected in a timely manner,providing sufficient time for early warning.Finally,a database of thermal runaway characteristic temperature for Li-ion and Na-ion cells is collected and processed to delineate four thermal hazard levels for quantitative assessment.Overall,LFP cells exhibit the lowest thermal hazard,followed by the Na-ion cells and NCM523 cells.This work clarifies the thermal hazard discrepancy between the Na-ion cell and prevalent Li-ion cells,providing crucial guidance for development and application of Na-ion cell.展开更多
Graphdiyne(GDY)is a two-dimensional carbon allotrope with exceptional physical and chemical properties that is gaining increasing attention.However,its efficient and scalable synthesis remains a significant challenge....Graphdiyne(GDY)is a two-dimensional carbon allotrope with exceptional physical and chemical properties that is gaining increasing attention.However,its efficient and scalable synthesis remains a significant challenge.We present a microwave-assisted approach for its continuous,large-scale production which enables synthesis at a rate of 0.6 g/h,with a yield of up to 90%.The synthesized GDY nanosheets have an average diameter of 246 nm and a thickness of 4 nm.We used GDY as a stable coating for potassium(K)metal anodes(K@GDY),taking advantage of its unique molecular structure to provide favorable paths for K-ion transport.This modification significantly inhibited dendrite formation and improved the cycling stability of K metal batteries.Full-cells with perylene-3,4,9,10-tetracarboxylic dianhydride(PTCDA)cathodes showed the clear superiority of the K@GDY anodes over bare K anodes in terms of performance,stability,and cycle life.The K@GDY maintained a stable voltage plateau and gave an excellent capacity retention after 600 cycles with nearly 100%Coulombic efficiency.This work not only provides a scalable and efficient way for GDY synthesis but also opens new possibilities for its use in energy storage and other advanced technologies.展开更多
La-Mg-Ni-based hydrogen storage alloys with superlattice structures are the new generation anode material for nickel metal hydride(Ni-MH)batteries owing to the advantages of high capacity and exceptional activation pr...La-Mg-Ni-based hydrogen storage alloys with superlattice structures are the new generation anode material for nickel metal hydride(Ni-MH)batteries owing to the advantages of high capacity and exceptional activation properties.However,the cycling stability is not currently satisfactory enough which plagues its application.Herein,a strategy of partially substituting La with the Y element is proposed to boost the capacity durability of La-Mg-Ni-based alloys.Furthermore,phase structure regulation is implemented simultaneously to obtain the A5 B19-type alloy with good crystal stability specifically.It is found that Y promotes the phase formation of the Pr5 Co19-type phase after annealing at 985℃.The alloy containing Y contributes to the superior rate capability resulting from the promoted hydrogen diffusion rate.Notably,Y substitution enables strengthening the anti-pulverization ability of the alloy in terms of increasing the volume match between[A_(2)B_(4)]and[AB5]subunits,and effectively enhances the anti-corrosion ability of the alloy due to high electronegativity,realizing improved long-term cycling stability of the alloy from 74.2%to 78.5%after cycling 300 times.The work is expected to shed light on the composition and structure design of the La-Mg-Ni-based hydrogen storage alloy for Ni-MH batteries.展开更多
基金funded by the Science and Technology Project of the State Grid Corporation of China (Exploration study on Fire Extinguishing Technology of Lithium Ion Energy Storage Battery DG71-18-002)。
文摘Currently,the effective and clean suppression of lithium-ion battery(LIB)fires remains a challenge.The present work investigates the use of various inhibitor doses(Xin)of dodecafluoro-2-methylpentan-3-one(C_(6) F_(12)O)in 300 Ah LIBs,and systematically examines the thermal and toxic hazards of the extinguished batteries via real scale combustion and gas analysis.The inhibitor is shown to be completely effective.The inhibition mechanism involves a combination of chemical inhibition and physical cooling.While the chemical inhibition effect tends to saturate with increasing Xin,the physical cooling remains effective at higher inhibitor doses.However,extinguishing the battery fire with a high Xin of C_(6)F_(12)O is found to incur serious toxicity problems.These results are expected to provide a guideline for the design of inhibitor doses for the suppression of LIB fires.
文摘Lithium ion batteries(LIB)can rupture and result in thermal runaway and battery fires.In the process of transporting lithium ion batteries using trains,the massive collection of batteries can cause train fire and pose significant danger to the public.This is especially critical when the fire occurs amid a heavily populated metropolitan environment.This paper reports the 3D analysis of a warehouse with possible train fire due to LIB rupture and the fire propagation at a rail yard.Six critical fire cases with the battery train in close vicinity to the warehouse were considered.The six fire cases are the worst-case scenarios of a Monte Carlo simulation of different fire cases that may occur to an actual steel storage facility at the Capital Railyard,Raleigh,North Carolina.A 3D finite element(FE)frame model was constructed for the steel warehouse and the most critical fire cases were simulated.The results indicated that several structural components of the warehouse would experience large stresses and deflections during the simulated battery fires and resulting in instability to the structure.Specifically,members of the roof frame represent the most critical elements and that the members can result in large deformations as early as 4 minutes after the fire starts.Furthermore,effective utilization of fire protection can delay somewhat the fire effects and extend time to failure to 45 minutes and in one of the simulated cases,prevent structural instability.Thus,fire from LIB waste transport using train is a very realistic problem due to the thermal runaway,and the analysis performed in current study can be used as a preventive investigation technique for buildings that may be exposed to the train fire risk.
文摘Each morning at Yangluo Port in Wuhan,Hubei Province,the all-electric cargo vessel Huahang Xinneng No.1 completes a battery swap in under 10 minutes before returning to service with nearly 8,000 kWh of power onboard。
基金supported by the National Natural Science Foundation of China(No.52207228)the Beijing Natural Science Foundation,China(No.3224070)the National Natural Science Foundation of China(No.52077208).
文摘The growing use of lithium-ion batteries in electric transportation and grid-scale storage systems has intensified the need for accurate and highly generalizable state-of-health(SOH)estimation.Conventional approaches often suffer from reduced accuracy under dynamically uncertain state-of-charge(SOC)operating ranges and heterogeneous aging stresses.This study presents a unified SOH estimation framework that integrates physics-informed modeling,subspace identification,and Transformer-based learning.A reduced-order model is derived from simplified electrochemical dynamics,providing an interpretable and computationally efficient representation of battery behavior.Subspace identification across a wide SOC and SOH range yields degradation-sensitive features,which the Transformer uses to capture long-range aging dynamics via multi-head self-attention.Experiments on LiFePO4 cells under joint-cell training show consistently accurate SOH estimation,with a maximum error of 1.39%,demonstrating the framework’s effectiveness in decoupling SOC and SOH effects.In cross-cell validation,where training and validation are performed on different cells,the model maintains a maximum error of 2.06%,confirming strong generalization to unseen aging trajectories.Comparative experiments on LiFePO_(4)and public LiCoO_(2)datasets confirm the framework’s cross-chemistry applicability.By extracting low-dimensional,physically interpretable features via subspace identification,the framework significantly reduces training cost while maintaining high SOH estimation accuracy,outperforming conventional data-driven models lacking physical guidance.
基金supported by the financial support from the National Research Foundation,Singapore,under its Singapore-China Joint Flagship Project(Clean Energy).
文摘Aqueous Zn-iodine batteries(ZIBs)face the formidable challenges towards practical implementation,including metal corrosion and rampant dendrite growth on the Zn anode side,and shuttle effect of polyiodide species from the cathode side.These challenges lead to poor cycle stability and severe self-discharge.From the fabrication and cost point of view,it is technologically more viable to deploy electrolyte engineering than electrode protection strategies.More importantly,a synchronous method for modulation of both cathode and anode is pivotal,which has been often neglected in prior studies.In this work,cationic poly(allylamine hydrochloride)(Pah^(+))is adopted as a low-cost dual-function electrolyte additive for ZIBs.We elaborate the synchronous effect by Pah^(+)in stabilizing Zn anode and immobilizing polyiodide anions.The fabricated Zn-iodine coin cell with Pah^(+)(ZnI_(2) loading:25 mg cm^(−2))stably cycles 1000 times at 1 C,and a single-layered 3.4 cm^(2) pouch cell(N/P ratio~1.5)with the same mass loading cycles over 300 times with insignificant capacity decay.
基金supported by the National Natural Science Foundation of China(No.52064035)the Key Research and Development Program of Gansu Province,China(No.25YFGA024)the Natural Science Foundation of Zhejiang Province,China(No.LGG22E020003).
文摘Lithium-sulfur(Li-S)batteries boast a theoretical energy density as high as 2600 Wh·kg^(−1),positioning them as a highly attractive option for future advanced energy storage systems.Challenges such as slow transformation kinetics and shuttle effects associated with lithium polysulfides(LiPSs)have seriously hindered their practical applications.In this paper,we present a new method for the synthesis of hollow carbon-sphere-supported Co monatomic catalysts(Co-N-C).This new synthesis method achieves pyrolytic coordination using a precursor rich in imide(-RC=N-)polymers.This synthesis method not only improves the adsorbability and catalytic activity of LiPS but also significantly weakens the shuttle effect and generates Co-N-C with superior conductivity,abundant hollow structures,and a high specific surface area,thus efficiently capturing and restricting the movement of LiPS intermediates.The dispersed Co monoatomic catalysts(Co SACs)were anchored to a highly conductive nitrogen-doped carbon framework and exhibited symmetric N-coordination active sites(Co-N_(4))to ensure fast redox kinetics of LiPS and Li_(2)S_(2)/Li_(2)S solid-state products.The lithium-sulfur battery with Co-N-C as the sulfur carrier showed excellent discharging capacity of 1146.6 mAh·g^(−1) at a discharge rate of 0.5 C and maintained excellent performance at a high discharge rate of 2 C.The capacity decay rate in 500 cycles was only 0.086%per cycle,reflecting excellent long-term cycle stability.This study highlights the key role of the synergistic effect between single-atom cobalt catalysts and hollow carbon spheres in enhancing the efficiency of lithium-sulfur(Li-S)batteries.It also provides valuable insights into the construction and fabrication of highly active monatomic catalysts.The catalytic conversion efficiency of lithium polysulfides is significantly enhanced when embedded in hollow carbon architectures,which serves as a critical strategy for optimizing the electrochemical behavior of next-generation Li-S batteries.
基金supported by the National Key Research and Development Program of China(2024YFE0213000)the Postdoctoral Innovative Talents Support Program(BX20240232)+1 种基金the Natural Science Foundation of China for Young Scholars(72304031)the Fundamental Research Funds for the Central Universities(FRF-TP-22-024A1).
文摘Lithium-ion batteries(LIBs)are widely deployed,from grid-scale storage to electric vehicles.LIBs remain stationary most of their service life,where calendar aging degrades capacity.Understanding the mechanisms of LIB calendar aging is crucial for extending battery lifespan.However,LIB calendar aging is influenced by multiple factors,including battery material,its state,and storage environment.Calendar aging experiments are also time-consuming,costly,and lack standardized testing conditions.This study employs a data-driven approach to establish a cross-scale database linking materials,side-reaction mechanisms,and calendar aging of LIBs.MELODI(Mechanism-informed,Explainable,Learning-based Optimization for Degradation Identification)is proposed to identify calendar aging mechanisms and quantify the effects of multi-scale factors.Results reveal that cathode material loss drives up to 91.42%of calendar aging degradation in high-nickel(Ni)batteries,while solid electrolyte interphase growth dominates in lithium iron phosphate(LFP)and low-Ni batteries,contributing up to 82.43%of degradation in LFP batteries and 99.10%of decay in low-Ni batteries,respectively.This study systematically quantifies calendar aging in commercial LIBs under varying materials,states of charge,and temperatures.These findings offer quantitative guidance for experimental design or battery use,and implications for emerging applications like aerial robotics,vehicle-to-grid,and embodied intelligence systems.
基金provided by the National Natural Science Foundation of China (No.52573275)Taishan Scholars Program of Shandong Province (No.tsqn202507205)+4 种基金Youth Innovation Team of Higher Education Institutions in Shandong Province (No.2023KJ105)Collaborative Innovation Center of Yellow River Basin Pharmaceutical Green Manufacturing and Engineering Equipment,University of Jinan,Jinan 250022,ChinaJinan City University Integration Development Strategy Project (No.JNSX2023021)supported by Talents’ plan Foundation of Guangdong Second Provincial General Hospital (No.2024D003)Science and Technology Projects in Guangzhou (No.2025A04J4629)。
文摘Conversion of ammonia into hydrogen,a crucial pathway for the hydrogen economy,is severely constrained by the intricacy of the required equipment and the low efficiency.Herein,Pd@Pt Ni Co Ru Ir coreshell mesoporous bifunctional electrocatalysts were fabricated via a one-step wet-chemical reduction approach.By utilizing the limiting effect of triblock copolymers,gradient distribution control of six metal elements(Pd core and Pt/Ni/Co/Ru/Ir high-entropy alloys shell) was achieved,where the high-entropy alloy shell forms high-density active sites through lattice distortion effect.With the help of lattice distortion and mesoporous-confinement-enabled interfacial coupling effects,Pd@Pt Ni Co Ru Ir catalyst exhibited exceptional bifunctional performance in alkaline media:A low hydrogen evolution reaction(HER) overpotential of 30.5 m V at 10 m A/cm^(2) and a high ammonia oxidation reaction(AOR) peak current density of 19.6 m A/cm^(2) at 0.7 V vs.RHE,representing a 3.83-fold enhancement over commercial Pt/C.Moreover,a rechargeable Zn-NH_(3) battery system was constructed and achieved 92.3 % Faradaic efficiency(FE) for NH_(3)-to-H_(2) conversion with outstanding stability at 16 m A/cm^(2),thereby providing an innovative solution for efficient ammonia decomposition-based hydrogen production.
基金supported by the National Natural Science Foundation of China(Nos.22479092 and 22078190)。
文摘The pseudo-two-dimensional(P2D)model plays an important role in exploring physicochemical mechanisms,predicting the state of health,and improving the fast charge capability for Li-ion batteries(LIBs).However,the fast charge leads to the lithium concentration gradient in the solid and electrolyte phases and the non-uniform electrochemical reaction at the solid/electrolyte interface.In order to decouple charge transfer reactions in LIBs under dynamic conditions,understanding the spatio-temporal resolution of the P2D model is urgently required.Till now,the study of this aspect is still insufficient.This work studies the spatio-temporal resolution for dynamic/static electrochemical impedance spectroscopy(DEIS/SEIS)on multiple scales.In detail,DEIS and SEIS with spatio-temporal resolutions are used to decouple charge transfer reactions in LIBs based on the numerical solution of the P2D model in the frequency domain.The calculated results indicate that decoupling solid diffusion requires a high spatial resolution along the r-direction in particles,decoupling electrolyte diffusion and interfacial transfer reaction requires a high spatial resolution along the x-direction,and decoupling charge transfer reactions in LIBs at an extremely low state of charge(SOC)requires an extremely high temporal resolution along the t-direction.Finally,the optimal range of spatio-temporal resolutions for DEIS/SEIS is derived,and the method to decouple charge transfer reactions with spatio-temporal resolutions is developed.
基金supported by the National Natural Science Foundation of China(Grant no.22209083).The authors appreciate Shiyanjia Lab(www.shiyanjia.com)for providing invaluable assistance with the science analysis.
文摘Developing high-performance Ni cathodes and understanding the relationship between electron states of Ni 3d orbital and energy storage mechanism from an atomic-orbital perspective are crucial yet challenging for alkaline nickel-zinc batteries.Herein,we innovatively design P-NiMoO_(4)/NiSe_(2)heterostructures with rich oxygen vacancy via a selective component segregation.The P substitution in NiMoO_(4)activate Ni atoms,leading to the spin-state transition of Ni-3d orbitals from high-spin to low-spin,which promote the uniform and rapid nucleation of NiSe_(2)on the surface of NiMoO_(4)during subsequent selenization process.After selenization,the in situ formed P-NiMoO_(4)/NiSe_(2)heterostructures exhibits continuous increased unoccupied states of Ni 3d-orbitals and higher Ni valence state.The synergistic effect of P doping and selenization modulate the d-band center(ɛd)level of Ni 3d,thereby promoting d-p orbital hybridization between Ni 3d and O 2p of OH−as well as OH−adsorption ability.Consequently,the P-NiMoO_(4)/NiSe_(2)exhibits a top-level specific capacity of 390.7 mA h g^(−1)at 1 A g^(−1),2.8-fold higher than that of pristine NiMoO_(4),accompanied by remarkable rate capability and structural stability.Moreover,the assembled pouch-type battery and flexible devices demonstrate the practical application potential.This work provides fundamental insights into orbital-level engineering of battery materials for enhanced redox kinetics and cycling stability.
基金supported by the National Natural Science Foundation of China(52402166)the Science and Technology Development Fund+2 种基金Macao SAR(0065/2023/AFJ,0116/2022/A3)the Australian Research Council(DE220100154)the Natural Science Foundation of Guangdong Province(2025A1515011120)。
文摘The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulate the electronic structure of MoS_(2),thereby obtaining a multifunctional catalyst that serves as an efficient sulfur host.The W/V dual single-atomdoped MoS_(2)grown on carbon nanofibers(CMWVS)demonstrates a strong adsorption ability for lithium polysulfides,suppressing the shuttle effects.Additionally,the doping process also results in the phase transition from 2H-MoS_(2)to 1T-MoS_(2)and generates sufficient edge sulfur atoms,promoting the charge/electron transfer and enriching the reaction sites.All these merits contribute to the superior conversion reaction kinetics,leading to the outstanding Li-S battery performance.When fabricated as cathodes by compositing with sulfur,the CMWVS/S cathode delivers a high capacity of 1481.7 mAh g^(-1)at 0.1 C(1 C=1672 mAh g^(-1))and maintains 816.3 m Ah g^(-1)after 1000 cycles at 1.0 C,indicating outstanding cycling stability.Even under a high sulfur loading of 7.9 mg cm^(-2)and lean electrolyte conditions(E/S ratio of 9.0μL mg^(-1)),the cathode achieves a high areal capacity of 8.2 m Ah cm^(-2),showing great promise for practical Li-S battery applications.This work broadens the scope of doping strategies in transition-metal dichalcogenides by tailoring their electronic structures,providing insightful direction for the rational development of high-efficiency electrocatalysts for advanced Li-S battery applications.
基金supported by the National Natural Science Foundation(52302284,22002086,22204096)Shanghai Sailing Program(23YF1412200)the Fundamental Research Funds for the Central Universities(22120240314).
文摘Single-atom catalysts(SACs)have garnered significant attention in lithium-sulfur(Li-S)batteries for their potential to mitigate the severe polysulfide shuttle effect and sluggish redox kinetics.However,the development of highly efficient SACs and a comprehensive understanding of their structure-activity relationships remain enormously challenging.Herein,a novel kind of Fe-based SAC featuring an asymmetric FeN_(5)-TeN_(4) coordination structure was precisely designed by introducing Te atom adjacent to the Fe active center to enhance the catalytic activity.Theoretical calculations reveal that the neighboring Te atom modulates the local coordination environment of the central Fe site,elevating the d-band center closer to the Fermi level and strengthening the d-p orbital hybridization between the catalyst and sulfur species,thereby immobilizing polysulfides and improving the bidirectional catalysis of Li-S redox.Consequently,the Fe-Te atom pair catalyst endows Li-S batteries with exceptional rate performance,achieving a high specific capacity of 735 mAh g^(−1) at 5 C,and remarkable cycling stability with a low decay rate of 0.038%per cycle over 1000 cycles at 1 C.This work provides fundamental insights into the electronic structure modulation of SACs and establishes a clear correlation between precisely engineered atomic configurations and their enhanced catalytic performance in Li-S electrochemistry.
基金the National Natural Science Foundation of China(22479047,22409058)the Outstanding Youth Scientist Foundation of Hunan Province(2022JJ10023)the Provincial Natural Science Foundation of Guangdong(2023A1515011745)for financial support of this research。
文摘To ease the scarcity of lithium(Li)resource and cut down on environmental pollution,an efficient,selective,inexpensive and sustainable Li recycling process from waste batteries is needed,which is yet to be achieved.Here,we report a low-potential photoelectrochemical(PEC)system that selectively and efficiently extracts Li metals from multi-cation electrolytes under 1 sun illumination.Based on the difference of redox potential,we can get rid of the disturbance of other cations(i.e.,Fe,Co and Ni ions)by a bias-free PEC device to realize the extraction of high-purity Li metals on a coplanar Si-based photocathode-TiO_(2) photoanode tandem device at 2 V of applied bias(far less than the redox potentials of Li^(+)/Li).In such system,the extraction rate of Li metals(purity>99.5%)exceeds 1.35 g h^(-1)m^(-2)with 90%of Faradaic efficiency.Long-term experiments,different electrode/electrolyte tests,and various price assessments further demonstrate the stability,compatibility and economy of PEC extraction system,enabling a solar-driven pathway for the recycling of critical metal resources.
基金supported by the National Natural Science Foundation of China(No.62464010)Spring City Plan-Special Program for Young Talents(K202005007)+2 种基金Yunnan Talents Support Plan for Young Talents(XDYC-QNRC-2022-0482)Yunnan Local Colleges Applied Basic Research Projects(202101BA070001-138)Frontier Research Team of Kunming University 2023.
文摘Rechargeable Zn/Sn-air batteries have received considerable attention as promising energy storage devices.However,the electrochemical performance of these batteries is significantly constrained by the sluggish electrocatalytic reaction kinetics at the cathode.The integration of light energy into Zn/Sn-air batteries is a promising strategy for enhancing their performance.However,the photothermal and photoelectric effects generate heat in the battery under prolonged solar irradiation,leading to air cathode instability.This paper presents the first design and synthesis of Ni_(2)-1,5-diamino-4,8-dihydroxyanthraquinone(Ni_(2)DDA),an electronically conductiveπ-d conjugated metal-organic framework(MOF).Ni_(2)DDA exhibits both photoelectric and photothermal effects,with an optical band gap of~1.14 eV.Under illumination,Ni_(2)DDA achieves excellent oxygen evolution reaction performance(with an overpotential of 245 mV vs.reversible hydrogen electrode at 10 mA cm^(−2))and photothermal stability.These properties result from the synergy between the photoelectric and photothermal effects of Ni_(2)DDA.Upon integration into Zn/Sn-air batteries,Ni_(2)DDA ensures excellent cycling stability under light and exhibits remarkable performance in high-temperature environments up to 80℃.This study experimentally confirms the stable operation of photo-assisted Zn/Sn-air batteries under high-temperature conditions for the first time and provides novel insights into the application of electronically conductive MOFs in photoelectrocatalysis and photothermal catalysis.
基金supported by the National Natural Science Foundation of China(52402298,52172224,52202228,22479112)the Science and Technology Correspondent Project of Tianjin(24YDTPJC00240)+4 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)The authors appreciate a portion of this research used resources at the Spallation Neutron Source,a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory.This research also employed the resources of BL14B1 beam at Shanghai Synchrotron Radiation Facility(SSRF)(Proposal info:2023-SSRF-PT-503737).
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 National Natural Science Foundation of China(51773134)the Sichuan Science and Technology Program(2019YFH0112)the Fundamental Research Funds for the Central Universities。
文摘Poly(ethylene oxide)(PEO)and its derivatives based gel polymer electrolytes(GPEs)are severely limited in advanced and safe lithium-ion batteries(LIBs)owing to the intrinsically high flammability of liquid electrolytes and PEO.Directly adding flame retardants to the GPEs can suppress their flammability and thus improve the safety of LIBs,but results in deteriorative electrochemical performance.Herein,a novel GPE with chemically bonded flame retardant(i.e.diethyl vinylphosphonate)in cross-linked polyethylene glycol diacrylate matrix,featuring both high-safety and high-performance,is designed.This as-prepared GPE storing the commercial 1 mol L^(-1) LiPF6 electrolyte resists high temperature of 200℃and cannot be ignited as well as possesses a high ionic conductivity(0.60 m S cm^(-1))and good compatibility with lithium.Notably,the LiFePO_(4)/Li battery with this GPE delivers a satisfactory capacity of 142.2 m A h g^(-1) and a superior cycling performance with a capacity retention of 96.3%and a coulombic efficiency of close to 100%for 350 cycles at 0.2 C under ambient temperature.Furthermore,the battery can achieve steady charge–discharge for 100 cycles with a coulombic efficiency of 99.5%at 1 C under 80℃and run normally even at a high temperature of 150℃or under the exposure to butane flame.Differential scanning calorimetry manifests significantly improved battery safety compared to commercial battery systems.This work provides a new pathway for developing next-generation advanced LIBs with enhanced performance and high safety.
基金the financial support from the National Key Research and Development Program of China(No.2021YFF0500802)the National Natural Science Foundation of China(No.51890904,No.52022022,and No.52278247)the Scientific Research and Innovation Plan of Jiangsu Province(KYCX21_0090)。
文摘Battery safety has attracted considerable attention worldwide due to the rapid development of wearable electronics and the steady increase in the production and use of electric vehicles.As battery failures are often associated with mechanical-thermal coupled behaviors,protective shielding materials with excellent mechanical robustness and flame-retardant properties are highly desired to mitigate thermal runaway.However,most of the thermal insulating materials are not strong enough to protect batteries from mechanical abuse,which is one of the most critical scenarios with catastrophic consequences.Here,inspired by wood,we have developed an effective approach to engineer a hierarchical nanocomposite via self-assembly of calcium silicate hydrate and polyvinyl alcohol polymer chains(referred as CSH wood).The versatile protective material CSH wood demonstrates an unprecedented combination of light weight(0.018 g cm-3),high stiffness(204 MPa in the axial direction),negative Poisson's ratio(-0.15),remarkable toughness(6.67×105 J m-3),superior thermal insulation(0.0204 W m-1 K-1 in the radial direction),and excellent fire retardancy(UL94-V0).When applied as a protective cover or a protective layer within battery packages,the tough CSH wood can resist high-impact load and block heat diffusion to block or delay the spread of fire,therefore significantly reducing the risk of property damage or bodily injuries caused by battery explosions.This work provides new pathways for fabricating advanced thermal insulating materials with large scalability and demonstrates great potential for the protection of electronic devices.
基金supported by the National Key R&D Program of China(No.2022YFE0207400)supported by the Xiaomi Young Talents Programsupported by the Youth Innovation Promotion Association CAS(No.Y201768)。
文摘Na-ion batteries are considered a promising next-generation battery alternative to Li-ion batteries,due to the abundant Na resources and low cost.Most efforts focus on developing new materials to enhance energy density and electrochemical performance to enable it comparable to Li-ion batteries,without considering thermal hazard of Na-ion batteries and comparison with Li-ion batteries.To address this issue,our work comprehensively compares commercial prismatic lithium iron phosphate(LFP) battery,lithium nickel cobalt manganese oxide(NCM523) battery and Na-ion battery of the same size from thermal hazard perspective using Accelerating Rate Calorimeter.The thermal hazard of the three cells is then qualitatively assessed from thermal stability,early warning and thermal runaway severity perspectives by integrating eight characteristic parameters.The Na-ion cell displays comparable thermal stability with LFP while LFP exhibits the lowest thermal runaway hazard and severity.However,the Na-ion cell displays the lowest safety venting temperature and the longest time interval between safety venting and thermal runaway,allowing the generated gas to be released as early as possible and detected in a timely manner,providing sufficient time for early warning.Finally,a database of thermal runaway characteristic temperature for Li-ion and Na-ion cells is collected and processed to delineate four thermal hazard levels for quantitative assessment.Overall,LFP cells exhibit the lowest thermal hazard,followed by the Na-ion cells and NCM523 cells.This work clarifies the thermal hazard discrepancy between the Na-ion cell and prevalent Li-ion cells,providing crucial guidance for development and application of Na-ion cell.
基金supported by National Natural Science Foundation of China(52302034,52402060,52202201,52021006)Beijing National Laboratory for Molecular Sciences(BNLMS-CXTD202001)+1 种基金Shenzhen Science and Technology Innovation Commission(KQTD20221101115627004)China Postdoctoral Science Foundation(2024T170972)。
文摘Graphdiyne(GDY)is a two-dimensional carbon allotrope with exceptional physical and chemical properties that is gaining increasing attention.However,its efficient and scalable synthesis remains a significant challenge.We present a microwave-assisted approach for its continuous,large-scale production which enables synthesis at a rate of 0.6 g/h,with a yield of up to 90%.The synthesized GDY nanosheets have an average diameter of 246 nm and a thickness of 4 nm.We used GDY as a stable coating for potassium(K)metal anodes(K@GDY),taking advantage of its unique molecular structure to provide favorable paths for K-ion transport.This modification significantly inhibited dendrite formation and improved the cycling stability of K metal batteries.Full-cells with perylene-3,4,9,10-tetracarboxylic dianhydride(PTCDA)cathodes showed the clear superiority of the K@GDY anodes over bare K anodes in terms of performance,stability,and cycle life.The K@GDY maintained a stable voltage plateau and gave an excellent capacity retention after 600 cycles with nearly 100%Coulombic efficiency.This work not only provides a scalable and efficient way for GDY synthesis but also opens new possibilities for its use in energy storage and other advanced technologies.
基金the financial support by the National Nat-ural Science Foundation of China(Nos.52201282,52071281,52371239)the China Postdoctoral Science Foundation(No.2023M742945)+4 种基金Hebei Provincial Postdoctoral Science Foundation(No.B2023003023)the Science Research Project of Hebei Education Department(No.BJK2022033)the Natural Science Foundation of Hebei Province(No.C2022203003)the Inner Mongolia Science and Technology Major Project(No.2020ZD0012)the Baotou Science and Technology Planning Project(No.XM2022BT09).
文摘La-Mg-Ni-based hydrogen storage alloys with superlattice structures are the new generation anode material for nickel metal hydride(Ni-MH)batteries owing to the advantages of high capacity and exceptional activation properties.However,the cycling stability is not currently satisfactory enough which plagues its application.Herein,a strategy of partially substituting La with the Y element is proposed to boost the capacity durability of La-Mg-Ni-based alloys.Furthermore,phase structure regulation is implemented simultaneously to obtain the A5 B19-type alloy with good crystal stability specifically.It is found that Y promotes the phase formation of the Pr5 Co19-type phase after annealing at 985℃.The alloy containing Y contributes to the superior rate capability resulting from the promoted hydrogen diffusion rate.Notably,Y substitution enables strengthening the anti-pulverization ability of the alloy in terms of increasing the volume match between[A_(2)B_(4)]and[AB5]subunits,and effectively enhances the anti-corrosion ability of the alloy due to high electronegativity,realizing improved long-term cycling stability of the alloy from 74.2%to 78.5%after cycling 300 times.The work is expected to shed light on the composition and structure design of the La-Mg-Ni-based hydrogen storage alloy for Ni-MH batteries.
