The widespread usage of rechargeable batteries in portable devices,electric vehicles,and energy storage systems has underscored the importance for accurately predicting their lifetimes.However,data scarcity often limi...The widespread usage of rechargeable batteries in portable devices,electric vehicles,and energy storage systems has underscored the importance for accurately predicting their lifetimes.However,data scarcity often limits the accuracy of prediction models,which is escalated by the incompletion of data induced by the issues such as sensor failures.To address these challenges,we propose a novel approach to accommodate data insufficiency through achieving external information from incomplete data samples,which are usually discarded in existing studies.In order to fully unleash the prediction power of incomplete data,we have investigated the Multiple Imputation by Chained Equations(MICE)method that diversifies the training data through exploring the potential data patterns.The experimental results demonstrate that the proposed method significantly outperforms the baselines in the most considered scenarios while reducing the prediction root mean square error(RMSE)by up to 18.9%.Furthermore,we have also observed that the penetration of incomplete data benefits the explainability of the prediction model through facilitating the feature selection.展开更多
Energy storage plays a critical role in sustainable development,with secondary batteries serving as vital technologies for efficient energy conversion and utilization.This review provides a comprehensive summary of re...Energy storage plays a critical role in sustainable development,with secondary batteries serving as vital technologies for efficient energy conversion and utilization.This review provides a comprehensive summary of recent advancements across various battery systems,including lithium-ion,sodium-ion,potassium-ion,and multivalent metal-ion batteries such as magnesium,zinc,calcium,and aluminum.Emerging technologies,including dual-ion,redox flow,and anion batteries,are also discussed.Particular attention is given to alkali metal rechargeable systems,such as lithium-sulfur,lithium-air,sodium-sulfur,sodium-selenium,potassium-sulfur,potassium-selenium,potassium-air,and zinc-air batteries,which have shown significant promise for high-energy applications.The optimization of key components—cathodes,anodes,electrolytes,and interfaces—is extensively analyzed,supported by advanced characterization techniques like time-of-flight secondary ion mass spectrometry(TOF-SIMS),synchrotron radiation,nuclear magnetic resonance(NMR),and in-situ spectroscopy.Moreover,sustainable strategies for recycling spent batteries,including pyrometallurgy,hydrometallurgy,and direct recycling,are critically evaluated to mitigate environmental impacts and resource scarcity.This review not only highlights the latest technological breakthroughs but also identifies key challenges in reaction mechanisms,material design,system integration,and waste battery recycling,and presents a roadmap for advancing high-performance and sustainable battery technologies.展开更多
Localized high-concentration electrolytes(LHCEs)are considered as promising electrolyte candidates to resolve technical issues of metal batteries owing to their unique interfacial properties and solvation structures.H...Localized high-concentration electrolytes(LHCEs)are considered as promising electrolyte candidates to resolve technical issues of metal batteries owing to their unique interfacial properties and solvation structures.Herein,we propose a self-assembly chemical strategy into the LCHEs induced by ordered nanostructure of zwitterionic co-solutes for highly efficient and ultrastable zinc(Zn)metal batteries.Through the systematic screening of six zwitterionic compounds,3-(decyldimethylammonio)propanesulfonate salt(C_(10))with the decyl chain and zwitterions was determined as an optimum to construct quasi-spherical aggregates with a periodic length of 3.77 nm,as confirmed by comprehensive synchronous small-angle X-ray scattering,Guinier,pair distance distribution function,Porod,and other spectroscopic characterizations and molecular dynamic simulation.In particularly,this self-assembled structure in electrolyte environments was attributed to increasing the proportion of both contact and aggregated ion pairs for the formation of LHCEs as well as to providing fast and selective Zn^(2+)conducting channels and uniform solid electrolyte interfaces for facilitated charge transfer kinetics.Moreover,the preferential adsorption of the self-assembled C_(10)on the Zn(002)surface modulated the electrical double layer to suppress hydrogen evolution and corrosion reactions.Consequently,the Zn‖Zn symmetric cells in Zn(OTf)_(2)/C_(10)electrolytes showed long-term plating/stripping behaviors over 2800 h at 1 mA cm^(-2)and 1 mAh cm^(-2)as well as over 1200 h even at 5 mA cm^(-2)and 5 mAh cm^(-2)with a very high depth of discharge of 42.7%.Furthermore,the ZnllVO_(2)/CNT full cells in Zn(OTf)_(2)/C_(10)electrolytes delivered a record-high capacity of 8.10 mAh cm^(-2)at an ultrahigh cathode mass loading of 50 mg cm^(-2)after 150 cycles.展开更多
Interfacial engineering of two-dimensional(2D)monometallic phosphides enables remarkable structural and electrochemical properties in energy storage devices.Herein,2D nanosheets(NSs)of FeP_(2)/Co_(2) P were grown on N...Interfacial engineering of two-dimensional(2D)monometallic phosphides enables remarkable structural and electrochemical properties in energy storage devices.Herein,2D nanosheets(NSs)of FeP_(2)/Co_(2) P were grown on Ni-foam(FCP)using a solution-based and phosphorization approach to be used as freestanding for high-performance energy storage devices.An effective phosphorization strategy is successfully de-veloped to improve the overall crystalline phase,tailor the morphology,and boost the electrochemical performances of electrodes.The FCP NSs electrode exhibits a battery-type redox behavior with a maxi-mum high areal capacity of 1.96 C cm^(-2) at 4 mA cm^(-2) in 6 M KOH aqueous electrolyte compared to the other counterparts.The superior electrochemical performance was achieved by increasing the electroac-tive sites and high conductivity via surface tailoring and fast redox reactions.Moreover,a supercapattery was assembled utilizing FCP and activated carbon(AC)electrodes and it revealed maximum specific en-ergy(E_(s))and specific power(P_(s))of 41.2 Wh kg^(-1) and 7578 W kg^(-1) with good cycling stability of 91%after 10,000 cycles at 5 A g^(-1).Eventually,the supercapattery has been explored in practical applications by lighting up light-emitting diodes(LEDs),representing the real-time performance of superior energy storage devices.展开更多
Particle-to-particle dry graphene coatings on Ni-rich layered oxide materials are proposed for highenergy lithium-ion batteries(LIBs)to mitigate the inherent and engineering challenges related to the electrochemically...Particle-to-particle dry graphene coatings on Ni-rich layered oxide materials are proposed for highenergy lithium-ion batteries(LIBs)to mitigate the inherent and engineering challenges related to the electrochemically fragile surfaces,as well as limiting electrode thickness and density.Utilizing a shear stress-based coating process without supplementary solvent or heat treatment,graphene sheets derived from graphene powder are applied onto the surface of spherical LiNi_(0.89)Co_(0.055)Mn_(0.055)O_(2)(NCM)material.This process achieves a coating thickness equivalent to or fewer than 10 layers of graphene and exposes the basal plane.The graphene-coated material increases particle hardness and mitigates degradation caused by inter-particle pressure,enabling the formation of high-density electrodes without pulverization.In the absence of additional carbon-conducting agents for the high-density composite electrode with a density of 4.0 g cm^(-3),it significantly enhances rate capability,demonstrating more than 5 times improvement by achieving 149.4 mAh g^(-1)at 2 C compared to the bare sample(28.9 mAh g^(-1)).Furthermore,the dry graphene coating enables the high areal capacity of 6.98 mAh cm^(-2).By exposing the basal plane of the graphene coating,the process enhances chemical stability,effectively inhibiting side reactions at the interface and mitigating cycle degradation.展开更多
Mg-based hydrogen storage materials have attracted much attention due to their high hydrogen content,abundant resources,and environmental friendliness.However,the high dehydrogenation temperature,slow kinetics and poo...Mg-based hydrogen storage materials have attracted much attention due to their high hydrogen content,abundant resources,and environmental friendliness.However,the high dehydrogenation temperature,slow kinetics and poor cycling stability are limiting its practical application.This work demonstrates the improved dehydrogenation kinetics and cycling stability of MgH_(2) modified by a hybrid of metallic Ni and layered MoS_(2)(denoted as“Ni-MoS_(2)”)introduced by ball milling,with Ni as the catalyst for MgH_(2) and MoS_(2) as the support for both Ni and MgH_(2).The onset dehydrogenation temperature of MgH_(2) is reduced to 198℃,and the rehydrogenation begins at a low temperature of 50℃.The MgH_(2)+10 wt%Ni-MoS_(2) composite has a fast dehydrogenation kinetics and can release 6.1 wt% hydrogen in 10 min at a constant temperature of 300℃,with the dehydrogenation activation energy significantly reduced from 151 to 85 kJ mol^(-1).During the cycling,the reversible capacity of the composite first exhibits a gradual increase for the initial 22 cycles and then maintains at 6.1 wt% from the 23th cycle to the 50th cycle.The Ni/MoS_(2) addition does not change the overall thermodynamic properties of MgH_(2) but can weaken the Mg-H bonds in the local regions as evident by theoretical calculation.Microstructure studies reveal that the metallic Ni will react with MgH_(2) to form Mg_(2)NiH_(0.3),which can act as a hydrogen pump,while the layered MoS_(2) serves as a support for the well dispersion of MgH_(2) and Ni.It is believed that the synergy of Mg_(2)NiH_(0.3) and layered MoS_(2) contributes to the significantly enhanced hydrogen storage of MgH_(2).This work provides a promising and simple strategy for enhancing the Mg-based hydrogen storage materials by combination of transition metals and layered materials introduced via simple ball milling.展开更多
As a hydrogen storage material,both AlH_(3)and LiNH_(2)possess a high hydrogen capacity.However,the dehydrogenated AlH_(3)can hardly absorb hydrogen under normal conditions,while LiNH_(2)will generate NH_(3)rather tha...As a hydrogen storage material,both AlH_(3)and LiNH_(2)possess a high hydrogen capacity.However,the dehydrogenated AlH_(3)can hardly absorb hydrogen under normal conditions,while LiNH_(2)will generate NH_(3)rather than H_(2)upon decomposition.In this work,we report thatthe combination of AlH_(3)and LiNH_(2)through simple ball milling leads to partial reversibility of the AlH_(3)-LiNH_(2)system and the suppression of NH_(3)liberation.The negatively charged H^(δ-)in AlH_(3)will react with the positively charged H^(δ+)in LiNH_(2)through a redox reaction to form Li_(2)NH,AlN,and H_(2)at 120-170℃.After dehydrogenation at above 270℃,Li_(3)AlN_(2)is generated,which is crucial for the reversibility of this system.The more the Li3AlN2generated,the better the reversibility of this system.The dehydrogenation capacity of AlH_(3)+2LiNH_(2)at the third cycle(3.0 wt%)is higher than that of AlH_(3)+LiNH_(2)(1.2 wt%)due to the generation of more Li3AlN2.The role of AIH_(3)/Al in the AlH_(3)-LiNH_(2)system is to fix the nitrogen into the form of AIN and Li_(3)AlN_(2)and thus suppress the liberation of NH_(3).Therefore,the synergy of AlH_(3)and LiNH_(2)leads to the reversibility of the Li-Al-NH system and the suppression of NH_(3).展开更多
Solid polymer electrolytes have garnered significant attention for lithium batteries because of their flexibility and safety.However,poor ionic conductivity,lithium dendrite formation,and high impedance hinder their p...Solid polymer electrolytes have garnered significant attention for lithium batteries because of their flexibility and safety.However,poor ionic conductivity,lithium dendrite formation,and high impedance hinder their practical application.In this study,a thin,flexible,3D hybrid solid electrolyte(3DHSE)is prepared by in situ thermal cross-linking polymerization with electrospun 3D nanowebs.The 3DHSE comprises Al-doped Li_(7)La_(3)Zr_(2)O_(12)(ALLZO)embedded in electrospun poly(vinylidene fluoride-cohexafluoropropylene)(PVDF-HFP)nonwoven 3D nanowebs and an in situ cross-linked polyethylene oxide(PEO)-based solid polymer electrolyte.The 3DHSE exhibits high tensile strength(6.55 MPa),a strain of 40.28%,enhanced ionic conductivity(7.86×10^(-4) S cm^(-1)),and a superior lithium-ion transference number(0.76)to that of the PVDF-HFP-based solid polymer electrolyte(PSPE).This enables highly stable lithium plating/stripping cycling for over 900 h at 25℃ with a current density of 0.2 mA cm^(-2).The LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM811)/3DHSE/Li cell has a higher capacity(140.56 mAh g^(-1) at 0.1 C)than the NCM811/PSPE/Li cell(124.88 mAh g^(-1) at 0.1 C)at 25℃.The 3DHSE enhances mechanical properties,stabilizes interfacial contact,improves ion transport,prevents NCM811 cracking,and significantly boosts cycling performance.This study highlights the potential of the 3DHSE as a candidate for advanced lithium polymer battery technology.展开更多
Lithium metal is a highly promising anode for next-generation rechargeable batteries due to its ultrahigh theoretical capacity(3860 mAh g^(-1))and the lowest electrochemical potential(-3.04 V vs.SHE).However,its pract...Lithium metal is a highly promising anode for next-generation rechargeable batteries due to its ultrahigh theoretical capacity(3860 mAh g^(-1))and the lowest electrochemical potential(-3.04 V vs.SHE).However,its practical application is hindered by dendritic growth,unstable solid electrolyte interphase(SEI),and electrically isolated"dead"lithium,which degrade cycling performance and safety.To mitigate these issues by lowering the local current density,three-dimensional(3D)porous scaffolds have been explored,yet their effectiveness remains limited due to the intrinsically lithiophobic nature of scaffold surfaces.Here,we present a facile and scalable strategy to construct 3D nickel scaffolds(NiOSc-400)with an oxygen-rich,lithiophilic NiO interface,using a two-step tunable surface modification route.NiOSc-400promotes uniform Li^(+)adsorption and nucleation,while facilitating the in-situ formation of a Li_(2)O-based quasi-SEI via a conversion reaction.NiOSc-400 exhibits excellent cycling stability with a Coulombic efficiency of 99.9%over 800 cycles at 0.5 mA cm^(-2)and maintains a low overpotential of 28.9 mV at 15 mA cm^(-2).This work provides a practically viable platform for dendrite-free,high-performance lithium metal anodes by rationally engineering interfacial chemistry and scaffold architecture.展开更多
Li/Mn-rich layered oxide(LMR)cathode active materials offer remarkably high specific discharge capacity(>250 mAh g^(-1))from both cationic and anionic redox.The latter necessitates harsh charging conditions to high...Li/Mn-rich layered oxide(LMR)cathode active materials offer remarkably high specific discharge capacity(>250 mAh g^(-1))from both cationic and anionic redox.The latter necessitates harsh charging conditions to high cathode potentials(>4.5 V vs Li|Li^(+)),which is accompanied by lattice oxygen release,phase transformation,voltage fade,and transition metal(TM)dissolution.In cells with graphite anode,TM dissolution is particularly detrimental as it initiates electrode crosstalk.Lithium difluorophosphate(LiDFP)is known for its pivotal role in suppressing electrode crosstalk through TM scavenging.In LMR‖graphite cells charged to an upper cutoff voltage(UCV)of 4.5 V,effective TM scavenging effects of LiDFP are observed.In contrast,for an UCV of 4.7 V,the scavenging effects are limited due to more severe TM dissolution compared an UCV of 4.5V.Given the saturation in solubility of the TM scavenging agents,which are LiDFP decomposition products,e.g.,PO_(4)^(3-) and PO_(3)F^(2-),higher concentrations of the LiDFP as precursor"cannot enhance the amount of scavenging species,they rather start to precipitate and damage the anode.展开更多
Integrating high-nickel layered oxide cathodes with aqueous slurry electrode preparation routes holds the potential to simultaneously meet the demands for high energy density and low-cost production of lithium-ion bat...Integrating high-nickel layered oxide cathodes with aqueous slurry electrode preparation routes holds the potential to simultaneously meet the demands for high energy density and low-cost production of lithium-ion batteries.However,the influence of dual exposure to air and liquid water as well as the heating treatment during aqueous slurry electrode processing on the high-nickel layered oxide electrode is yet to be understood.In this study,we systematically investigate the structural evolution and electro-chemical behaviors when LiNi_(0.83)Mn_(0.05)Co_(0.12)O_(2)(NMC83)is subjected to aqueous slurry processing.It was observed that the crystal structure near the surface of NMC83 is partially reconstructed to contain a mixture of rock-salt and layered phases when exposed to water,leading to the deteriorated rate capability of the NMC83 electrodes.This partial surface reconstruction layer completely converts into a pure rock-salt phase upon cycling,accompanied by the release of O_(2),Ni leaching,catalyzed decomposition of the electrolyte,and the formation of a thick cathode electrolyte interphase layer.The byproducts of the electrolyte and dissolved Ni could shuttle to the Li metal side,causing a crosstalk effect that results in a thick and unstable solid electrolyte interphase layer on the Li surface.These in combination severely undermined the cycling stability of the NMC83 electrodes obtained from the aqueous slurry.A mitigation strategy using molecular self-assembly technique was demonstrated to enhance the surface stability of water-treated NMC83.Our findings offer new insights for tailoring ambient environment stability and aqueous slurry processability for ultra-high nickel layered oxide and other water-sensitive cathode materials.展开更多
The deposition of ultrafine single-atom nickel particles on Nb_(2)C(MXene)was successfully achieved using a wet chemistry method to synthesize Ni@Nb_(2)C composite.This study explored the effect of Ni@Nb_(2)C on the h...The deposition of ultrafine single-atom nickel particles on Nb_(2)C(MXene)was successfully achieved using a wet chemistry method to synthesize Ni@Nb_(2)C composite.This study explored the effect of Ni@Nb_(2)C on the hydrogen absorption and desorption properties of MgH_(2) through theoretical calculations and experimental investigations.Under the catalytic action of Ni@Nb2C,the initial dehydrogenation temperature of MgH_(2) was reduced by 121℃,with approximately 4.26 wt.% of H_(2) desorbed at 225℃ in 100 min.The dehydrogenation activation energy of the MgH_(2)+Ni@Nb_(2)C composite dropped to 86.7 kJ·mol^(-1),a reduction of 60.5 kJ·mol^(-1) compared to pure MgH_(2).Density functional theory calculations indicated that the incorporation of Ni@Nb_(2)C enhanced the performance of MgH_(2) performance by improving interactions among Nb_(2)C,Ni,Mg,and H atoms.In the Ni@Nb_(2)C+MgH_(2) system,the lengths of Mg-H bonds(1.91-1.99 A)were found to be longer than those observed in pure MgH_(2)(1.71 A).The dehydrogenation energy for this system(1.08 eV)was lower than that for Nb_(2)C(1.52 eV).These findings suggest that the synergistic effect of Ni and Nb2C significantly enhances the hydrogenation/dehydrogenation kinetics of MgH_(2),thereby introducing a novel approach for catalytic modification of solid hydrogen storage materials through synergistic actions.展开更多
The robust respective formations of a solid electrolyte interphase(SEI)and pillar at the surfaces of hard carbon and O3-type positive electrodes are the consequences of integrating Li PF_6 salt into a sodium-ion batte...The robust respective formations of a solid electrolyte interphase(SEI)and pillar at the surfaces of hard carbon and O3-type positive electrodes are the consequences of integrating Li PF_6 salt into a sodium-ion battery electrolyte that considerably strengthens both interfaces of positive and negative electrodes.The improvement of cycle performances due to the formation of highly passivating SEI on the hard carbon electrode is induced by the alternated solvation structure following the addition of Li salt,which inhibits sodium-ion and electron leakage from further electrolyte decomposition.The SEI with incorporated Li is less soluble than Na-based SEI,and the passivation ability of the initially formed SEI can thus be well preserved.Conversely,the gas evolution caused by oxygen release is reduced considerably by the marginal surface intercalation of Li ions at the surface of the O3-positive electrode.Additionally,the Li F layer that forms on the O3 surface diminishes additional deterioration of the electrolyte after formation.Compared with the fluoroethylene carbonate additive that is typically applied,a simultaneously strengthened interface yields major improvements in capacity retention.展开更多
The increasingly severe energy crisis and environmental issues have raised higher requirements for grid-scale energy storage systems.Rechargeable batteries have enormous development prospects due to their flexibility ...The increasingly severe energy crisis and environmental issues have raised higher requirements for grid-scale energy storage systems.Rechargeable batteries have enormous development prospects due to their flexibility and environmental protection. However, the traditional organic liquid-based batteries cannot meet our needs for future advanced batteries in terms of safety, energy density, and stability under extreme working conditions. In this case, we comprehensively summarize various advanced battery technologies to overcome the above problems.Firstly, we highlight the advantage of solid-state batteries compared to liquid electrolytes. Specifically, we focus on the advantages and challenges of solid-state lithium/sodium batteries and other types of solid-state batteries associated with the electrodes, solid electrolytes and the electrode/electrolyte interphase. Secondly, we discuss the environmentally friendly and safe liquid-state battery and its application prospect.Thirdly, the battery improvement strategy has been proposed to enhance the application of batteries under extreme conditions. Subsequently, we emphasize the importance of theoretical calculations and AI technology in promoting the development of battery technology. Finally, the current challenges and future directions of battery technology are summarized. The combination of in-depth failure mechanism analysis, advanced characterization techniques, economic commercialization and machine learning enables the rapid development of advanced battery technology for sustainable energy storage.展开更多
Activating MoS_(2) with atomic metal doping is promising to harvest desirable Pt-matched hydrogen evolution reaction(HER)catalytic performance.Herein,we developed an efficient method to access edgerich lattice-distort...Activating MoS_(2) with atomic metal doping is promising to harvest desirable Pt-matched hydrogen evolution reaction(HER)catalytic performance.Herein,we developed an efficient method to access edgerich lattice-distorted MoS_(2) for highly efficient HER via in-situ sulphuration of atomic Co/Mo species that were well-dispersed in a formamide-derived N-doped carbonaceous(f-NC)substrate.Apart from others,pre-embedding Co/Mo species in f-NC controls the release of metal sources upon annealing in S vapor,grafting the as-made MoS_(2) with merits of short-range crystallinity,distorted lattices,rich defects,and more edges exposed.The content of atomic Co species embedded in MoS_(2) reaches up to 2.85 at.%,and its atomic dispersion has been systematically confirmed by using XRD,HRTEM,XPS,and XAS characterizations.The Co-doped MoS_(2) sample exhibits excellent HER activity,achieving overpotentials of 67 and155 m V at j=10 m A cm^(-2) in 1.0 M KOH and 0.5 M H_(2)SO_(4),respectively.Density functional theory simulations suggest that,compared with free-doping MoS_(2),the edged Co doping is responsible for the significantly improved HER activity.Our method,in addition to providing reliable Pt-matched HER catalysts,may also inspire the general synthesis of edge-rich metal-doped metal chalcogenide for a wide range of energy conversion applications.展开更多
Phosphorus doped silicon-carbon composite particles were synthesized through a DC arc plasma torch.Silane(SiH4) and methane(CH4) were introduced into the reaction chamber as the precursor of silicon and carbon,respect...Phosphorus doped silicon-carbon composite particles were synthesized through a DC arc plasma torch.Silane(SiH4) and methane(CH4) were introduced into the reaction chamber as the precursor of silicon and carbon,respectively.Phosphine(PH3) was used as a phosphorus dopant gas.Characterization of synthesized particles were carried out by scanning electron microscopy(SEM),X-ray diffractometry(XRD),X-ray photoelectron spectroscopy(XPS) and bulk resistivity measurement.Electrochemical properties were investigated by cyclic test and electrochemical voltage spectroscopy(EVS).In the experimental range,phosphorus doped silicon-carbon composite electrode exhibits enhanced cycle performance than intrinsic silicon and phosphorus doped silicon.It can be explained that incorporation of carbon into silicon acts as a buffer matrix and phosphorus doping plays an important role to enhance the conductivity of the electrode,which leads to the improvement of the cycle performance of the cell.展开更多
Lithium–sulfur batteries(LSBs)are regarded as promising candidates for the next-generation energy storage devices owing to their high-theoretical capacity(1675 mAh g^(−1))and affordable cost.However,several limitatio...Lithium–sulfur batteries(LSBs)are regarded as promising candidates for the next-generation energy storage devices owing to their high-theoretical capacity(1675 mAh g^(−1))and affordable cost.However,several limitations of LSBs such as the lithium polysulfide shuttle,large volume expansion,and low electrical conductivity of sulfur need to be resolved for practical applications.To address these limitations,herein,a multidimensional architectured hybrid(Co@CNT/nG),where Co_(3)O_(4) nanoparticles are encapsulated into threedimensional(3D)porous N-doped reduced graphene oxide interconnected with carbon nanotube(CNT)branches,is synthesized through a simple pyrolysis method.The synergistic effect achieved through the homogeneously distributed and encapsulated Co_(3)O_(4) nanoparticles,the interconnected CNT branches,and the 3D hierarchical porous structure and N-doping of Co@CNT/nG significantly suppresses the shuttle effect of lithium polysulfides and enhances the conversion redox kinetics for the improved sulfur utilization.We validate this effect through various measurements including symmetric cells,Li_(2)S nucleation,shuttle currents,Tafel slopes,diffusion coefficients,and post-mortem analyses.Importantly,Co@CNT/nG-70S-based LSB cells achieve a high-specific capacity of 1193.1 mAh g^(−1) at 0.1 C and a low capacity decay rate of 0.030%per cycle for 700 cycles at 5 C,delivering a high areal capacity of 5.62 mAh cm^(−2) even with a loading of 6.5 mg cm^(−2).展开更多
Lithium-sulfur(Li-S)batteries are receiving increasing attention as one of the potential next-generation batteries,owing to their high energy densities and low cost.However,practical Li-S batteries with high energy de...Lithium-sulfur(Li-S)batteries are receiving increasing attention as one of the potential next-generation batteries,owing to their high energy densities and low cost.However,practical Li-S batteries with high energy densities are extremely hindered by the sulfur loss,low Coulombic efficiency,and short cycling life originating from the polysulfide(LiPS)shuttle.In this study,two-dimensional(2D)ZnCo_(2)O_(4) microsheets fabricated by a facile hydrothermal process are employed to modify the separator,for improving the electrochemical performances of Li-S cells.The resulting 2D Zn Co_(2)O_(4)-coated separator features a coating thickness of approximately 10 lm,high ionic conductivity of 1.8 m S/cm,and low mass loading of 0.2 mg/cm^(2).This 2D ZnCo_(2)O_(4)-coated separator effectively inhibits Li PS shuttle by a strong chemical interaction with Li PS as well as promotes the redox kinetics by Zn CO2O4-coated layers,as determined by X-ray photoelectron spectroscopy analysis,self-discharge,time-dependent permeation test,Li symmetric cell test,and Li2S nucleation analyses.Consequently,the Li-S batteries based on the 2D Zn Co_(2)O_(4)-coated separator exhibit a high initial discharge capacity of 1292.2 m Ah/g at 0.1 C.Moreover,they exhibit excellent long cycle stability at 1 and 2 C with capacity retention of 84%and 86%even after800 cycles,corresponding to a capacity fading rate of 0.020%and 0.016%per cycle,respectively.Effectively,these Li-S cells with a high sulfur loading at 5.3 mg/cm^(2) and low electrolyte concentration of 9 l L/mg deliver a high discharge capacity of 4.99 m Ah/cm^(2) after 200 cycles at 0.1 C.展开更多
The solvent-free in situ polymerization technique has the potential to tailor-make conformal interfaces that are essential for developing durable and safe lithium metal polymer batteries(LMPBs).Hence,much attention ha...The solvent-free in situ polymerization technique has the potential to tailor-make conformal interfaces that are essential for developing durable and safe lithium metal polymer batteries(LMPBs).Hence,much attention has been given to the eco-friendly and rapid ultraviolet(UV)-induced in situ photopolymerization process to prepare solid-state polymer electrolytes.In this respect,an innovative method is proposed here to overcome the challenges of UV-induced photopolymerization(UV-curing)in the zones where UV-light cannot penetrate,especially in LMPBs where thick electrodes are used.The proposed frontal-inspired photopolymerization(FIPP)process is a diverged frontal-based technique that uses two classes(dual)of initiators to improve the slow reaction kinetics of allyl-based monomers/oligomers by at least 50%compared with the conventional UV-curing process.The possible reaction mechanism occurring in FIPP is demonstrated using density functional theory calculations and spectroscopic investigations.Indeed,the initiation mechanism identified for the FIPP relies on a photochemical pathway rather than an exothermic propagating front forms during the UV-irradiation step as the case with the classical frontal photopolymerization technique.Besides,the FIPP-based in situ cell fabrication using dual initiators is advantageous over both the sandwich cell assembly and conventional in situ photopolymerization in overcoming the limitations of mass transport and active material utilization in high energy and high power LMPBs that use thick electrodes.Furthermore,the LMPB cells fabricated using the in situ-FIPP process with high mass loading LiFePO_(4)electrodes(5.2 mg cm^(-2))demonstrate higher rate capability,and a 50%increase in specific capacity against a sandwich cell encouraging the use of this innovative process in large-scale solid-state battery production.展开更多
Aluminum hydride(AlH3) is a binary metal hydride that contains more than 10.1 wt% of hydrogen and possesses a high volumetric hydrogen density of 148 kg H2 m^(-3).Pristine AlH3 can readily release hydrogen at a modera...Aluminum hydride(AlH3) is a binary metal hydride that contains more than 10.1 wt% of hydrogen and possesses a high volumetric hydrogen density of 148 kg H2 m^(-3).Pristine AlH3 can readily release hydrogen at a moderate temperature below 200℃.Such high hydrogen density and low desorption temperature make AlH3 one of most promising hydrogen storage media for mobile application.This review covers the research activity on the structures,synthesis,decomposition thermodynamics and kinetics,regeneration and application validation of AlH3 over the past decades.Finally,the future research directions of AlH3 as a hydrogen storage material will be revealed.展开更多
文摘The widespread usage of rechargeable batteries in portable devices,electric vehicles,and energy storage systems has underscored the importance for accurately predicting their lifetimes.However,data scarcity often limits the accuracy of prediction models,which is escalated by the incompletion of data induced by the issues such as sensor failures.To address these challenges,we propose a novel approach to accommodate data insufficiency through achieving external information from incomplete data samples,which are usually discarded in existing studies.In order to fully unleash the prediction power of incomplete data,we have investigated the Multiple Imputation by Chained Equations(MICE)method that diversifies the training data through exploring the potential data patterns.The experimental results demonstrate that the proposed method significantly outperforms the baselines in the most considered scenarios while reducing the prediction root mean square error(RMSE)by up to 18.9%.Furthermore,we have also observed that the penetration of incomplete data benefits the explainability of the prediction model through facilitating the feature selection.
基金supported by the National Natural Science Foundation of China(Nos.U21A20311 and 22409147)。
文摘Energy storage plays a critical role in sustainable development,with secondary batteries serving as vital technologies for efficient energy conversion and utilization.This review provides a comprehensive summary of recent advancements across various battery systems,including lithium-ion,sodium-ion,potassium-ion,and multivalent metal-ion batteries such as magnesium,zinc,calcium,and aluminum.Emerging technologies,including dual-ion,redox flow,and anion batteries,are also discussed.Particular attention is given to alkali metal rechargeable systems,such as lithium-sulfur,lithium-air,sodium-sulfur,sodium-selenium,potassium-sulfur,potassium-selenium,potassium-air,and zinc-air batteries,which have shown significant promise for high-energy applications.The optimization of key components—cathodes,anodes,electrolytes,and interfaces—is extensively analyzed,supported by advanced characterization techniques like time-of-flight secondary ion mass spectrometry(TOF-SIMS),synchrotron radiation,nuclear magnetic resonance(NMR),and in-situ spectroscopy.Moreover,sustainable strategies for recycling spent batteries,including pyrometallurgy,hydrometallurgy,and direct recycling,are critically evaluated to mitigate environmental impacts and resource scarcity.This review not only highlights the latest technological breakthroughs but also identifies key challenges in reaction mechanisms,material design,system integration,and waste battery recycling,and presents a roadmap for advancing high-performance and sustainable battery technologies.
基金financially supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.NRF-2020R1A3B2079803 and No.RS-2024-00453815),Republic of Korea。
文摘Localized high-concentration electrolytes(LHCEs)are considered as promising electrolyte candidates to resolve technical issues of metal batteries owing to their unique interfacial properties and solvation structures.Herein,we propose a self-assembly chemical strategy into the LCHEs induced by ordered nanostructure of zwitterionic co-solutes for highly efficient and ultrastable zinc(Zn)metal batteries.Through the systematic screening of six zwitterionic compounds,3-(decyldimethylammonio)propanesulfonate salt(C_(10))with the decyl chain and zwitterions was determined as an optimum to construct quasi-spherical aggregates with a periodic length of 3.77 nm,as confirmed by comprehensive synchronous small-angle X-ray scattering,Guinier,pair distance distribution function,Porod,and other spectroscopic characterizations and molecular dynamic simulation.In particularly,this self-assembled structure in electrolyte environments was attributed to increasing the proportion of both contact and aggregated ion pairs for the formation of LHCEs as well as to providing fast and selective Zn^(2+)conducting channels and uniform solid electrolyte interfaces for facilitated charge transfer kinetics.Moreover,the preferential adsorption of the self-assembled C_(10)on the Zn(002)surface modulated the electrical double layer to suppress hydrogen evolution and corrosion reactions.Consequently,the Zn‖Zn symmetric cells in Zn(OTf)_(2)/C_(10)electrolytes showed long-term plating/stripping behaviors over 2800 h at 1 mA cm^(-2)and 1 mAh cm^(-2)as well as over 1200 h even at 5 mA cm^(-2)and 5 mAh cm^(-2)with a very high depth of discharge of 42.7%.Furthermore,the ZnllVO_(2)/CNT full cells in Zn(OTf)_(2)/C_(10)electrolytes delivered a record-high capacity of 8.10 mAh cm^(-2)at an ultrahigh cathode mass loading of 50 mg cm^(-2)after 150 cycles.
基金supported by Basic Science Research Pro-gram through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(No.NRF-2014R1A6A1030419)supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.2020112382).
文摘Interfacial engineering of two-dimensional(2D)monometallic phosphides enables remarkable structural and electrochemical properties in energy storage devices.Herein,2D nanosheets(NSs)of FeP_(2)/Co_(2) P were grown on Ni-foam(FCP)using a solution-based and phosphorization approach to be used as freestanding for high-performance energy storage devices.An effective phosphorization strategy is successfully de-veloped to improve the overall crystalline phase,tailor the morphology,and boost the electrochemical performances of electrodes.The FCP NSs electrode exhibits a battery-type redox behavior with a maxi-mum high areal capacity of 1.96 C cm^(-2) at 4 mA cm^(-2) in 6 M KOH aqueous electrolyte compared to the other counterparts.The superior electrochemical performance was achieved by increasing the electroac-tive sites and high conductivity via surface tailoring and fast redox reactions.Moreover,a supercapattery was assembled utilizing FCP and activated carbon(AC)electrodes and it revealed maximum specific en-ergy(E_(s))and specific power(P_(s))of 41.2 Wh kg^(-1) and 7578 W kg^(-1) with good cycling stability of 91%after 10,000 cycles at 5 A g^(-1).Eventually,the supercapattery has been explored in practical applications by lighting up light-emitting diodes(LEDs),representing the real-time performance of superior energy storage devices.
基金supported by the Hyundai NGV and Technology Innovation Program(20010900)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea)+1 种基金the support by BK21 FOUR(Human Tech Materials-based Global Elite Cultivation Center for Student Success)funded by the Ministry of Education(MOE,Korea)supported by the Technology Innovation Program Development Program(Grant No.20017477)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea)。
文摘Particle-to-particle dry graphene coatings on Ni-rich layered oxide materials are proposed for highenergy lithium-ion batteries(LIBs)to mitigate the inherent and engineering challenges related to the electrochemically fragile surfaces,as well as limiting electrode thickness and density.Utilizing a shear stress-based coating process without supplementary solvent or heat treatment,graphene sheets derived from graphene powder are applied onto the surface of spherical LiNi_(0.89)Co_(0.055)Mn_(0.055)O_(2)(NCM)material.This process achieves a coating thickness equivalent to or fewer than 10 layers of graphene and exposes the basal plane.The graphene-coated material increases particle hardness and mitigates degradation caused by inter-particle pressure,enabling the formation of high-density electrodes without pulverization.In the absence of additional carbon-conducting agents for the high-density composite electrode with a density of 4.0 g cm^(-3),it significantly enhances rate capability,demonstrating more than 5 times improvement by achieving 149.4 mAh g^(-1)at 2 C compared to the bare sample(28.9 mAh g^(-1)).Furthermore,the dry graphene coating enables the high areal capacity of 6.98 mAh cm^(-2).By exposing the basal plane of the graphene coating,the process enhances chemical stability,effectively inhibiting side reactions at the interface and mitigating cycle degradation.
基金supported by the Science and Technology Department of Guangxi Zhuang Autonomous[grant numbers 2025GXNSFFA069003]the National Natural Science Foundation of China[grant numbers 22379030]+1 种基金Bagui Young Scholars Program of Guangxi Zhuang Autonomous Regionthe high-performance computing platform of Guangxi University.
文摘Mg-based hydrogen storage materials have attracted much attention due to their high hydrogen content,abundant resources,and environmental friendliness.However,the high dehydrogenation temperature,slow kinetics and poor cycling stability are limiting its practical application.This work demonstrates the improved dehydrogenation kinetics and cycling stability of MgH_(2) modified by a hybrid of metallic Ni and layered MoS_(2)(denoted as“Ni-MoS_(2)”)introduced by ball milling,with Ni as the catalyst for MgH_(2) and MoS_(2) as the support for both Ni and MgH_(2).The onset dehydrogenation temperature of MgH_(2) is reduced to 198℃,and the rehydrogenation begins at a low temperature of 50℃.The MgH_(2)+10 wt%Ni-MoS_(2) composite has a fast dehydrogenation kinetics and can release 6.1 wt% hydrogen in 10 min at a constant temperature of 300℃,with the dehydrogenation activation energy significantly reduced from 151 to 85 kJ mol^(-1).During the cycling,the reversible capacity of the composite first exhibits a gradual increase for the initial 22 cycles and then maintains at 6.1 wt% from the 23th cycle to the 50th cycle.The Ni/MoS_(2) addition does not change the overall thermodynamic properties of MgH_(2) but can weaken the Mg-H bonds in the local regions as evident by theoretical calculation.Microstructure studies reveal that the metallic Ni will react with MgH_(2) to form Mg_(2)NiH_(0.3),which can act as a hydrogen pump,while the layered MoS_(2) serves as a support for the well dispersion of MgH_(2) and Ni.It is believed that the synergy of Mg_(2)NiH_(0.3) and layered MoS_(2) contributes to the significantly enhanced hydrogen storage of MgH_(2).This work provides a promising and simple strategy for enhancing the Mg-based hydrogen storage materials by combination of transition metals and layered materials introduced via simple ball milling.
基金financially supported by the National Natural Science Foundation of China(Nos.22379030,52001079,52261038)the Science and Technology Department of Guangxi Zhuang Autonomous(Nos.2024JJG160001,GuiKeAD21238022)the Innovation Project of Guangxi Graduate Education(No.YCBZ2023011)
文摘As a hydrogen storage material,both AlH_(3)and LiNH_(2)possess a high hydrogen capacity.However,the dehydrogenated AlH_(3)can hardly absorb hydrogen under normal conditions,while LiNH_(2)will generate NH_(3)rather than H_(2)upon decomposition.In this work,we report thatthe combination of AlH_(3)and LiNH_(2)through simple ball milling leads to partial reversibility of the AlH_(3)-LiNH_(2)system and the suppression of NH_(3)liberation.The negatively charged H^(δ-)in AlH_(3)will react with the positively charged H^(δ+)in LiNH_(2)through a redox reaction to form Li_(2)NH,AlN,and H_(2)at 120-170℃.After dehydrogenation at above 270℃,Li_(3)AlN_(2)is generated,which is crucial for the reversibility of this system.The more the Li3AlN2generated,the better the reversibility of this system.The dehydrogenation capacity of AlH_(3)+2LiNH_(2)at the third cycle(3.0 wt%)is higher than that of AlH_(3)+LiNH_(2)(1.2 wt%)due to the generation of more Li3AlN2.The role of AIH_(3)/Al in the AlH_(3)-LiNH_(2)system is to fix the nitrogen into the form of AIN and Li_(3)AlN_(2)and thus suppress the liberation of NH_(3).Therefore,the synergy of AlH_(3)and LiNH_(2)leads to the reversibility of the Li-Al-NH system and the suppression of NH_(3).
基金supported by the National Research Foundation of Korea(NRF)(no.:NRF-2020M3H4A3081874)the National Research Council of Science&Technology(NST)grant by the Korea government(MSIT)(no.:GTL24011-000)the Korea Research Institute of Chemical Technology(KRICT),Republic of Korea(no.KS2422-20).
文摘Solid polymer electrolytes have garnered significant attention for lithium batteries because of their flexibility and safety.However,poor ionic conductivity,lithium dendrite formation,and high impedance hinder their practical application.In this study,a thin,flexible,3D hybrid solid electrolyte(3DHSE)is prepared by in situ thermal cross-linking polymerization with electrospun 3D nanowebs.The 3DHSE comprises Al-doped Li_(7)La_(3)Zr_(2)O_(12)(ALLZO)embedded in electrospun poly(vinylidene fluoride-cohexafluoropropylene)(PVDF-HFP)nonwoven 3D nanowebs and an in situ cross-linked polyethylene oxide(PEO)-based solid polymer electrolyte.The 3DHSE exhibits high tensile strength(6.55 MPa),a strain of 40.28%,enhanced ionic conductivity(7.86×10^(-4) S cm^(-1)),and a superior lithium-ion transference number(0.76)to that of the PVDF-HFP-based solid polymer electrolyte(PSPE).This enables highly stable lithium plating/stripping cycling for over 900 h at 25℃ with a current density of 0.2 mA cm^(-2).The LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM811)/3DHSE/Li cell has a higher capacity(140.56 mAh g^(-1) at 0.1 C)than the NCM811/PSPE/Li cell(124.88 mAh g^(-1) at 0.1 C)at 25℃.The 3DHSE enhances mechanical properties,stabilizes interfacial contact,improves ion transport,prevents NCM811 cracking,and significantly boosts cycling performance.This study highlights the potential of the 3DHSE as a candidate for advanced lithium polymer battery technology.
基金supported by the research grant of the Gyeongsang National University in 2024supported by the National Research Foundation of Korea(NRF)grants funded by the Korean Government(NRF-2022R1C1C1011386)。
文摘Lithium metal is a highly promising anode for next-generation rechargeable batteries due to its ultrahigh theoretical capacity(3860 mAh g^(-1))and the lowest electrochemical potential(-3.04 V vs.SHE).However,its practical application is hindered by dendritic growth,unstable solid electrolyte interphase(SEI),and electrically isolated"dead"lithium,which degrade cycling performance and safety.To mitigate these issues by lowering the local current density,three-dimensional(3D)porous scaffolds have been explored,yet their effectiveness remains limited due to the intrinsically lithiophobic nature of scaffold surfaces.Here,we present a facile and scalable strategy to construct 3D nickel scaffolds(NiOSc-400)with an oxygen-rich,lithiophilic NiO interface,using a two-step tunable surface modification route.NiOSc-400promotes uniform Li^(+)adsorption and nucleation,while facilitating the in-situ formation of a Li_(2)O-based quasi-SEI via a conversion reaction.NiOSc-400 exhibits excellent cycling stability with a Coulombic efficiency of 99.9%over 800 cycles at 0.5 mA cm^(-2)and maintains a low overpotential of 28.9 mV at 15 mA cm^(-2).This work provides a practically viable platform for dendrite-free,high-performance lithium metal anodes by rationally engineering interfacial chemistry and scaffold architecture.
基金the Ministry for Culture and Science of North Rhine Westphalia(Germany)for funding this work within the International Graduate School for Battery Chemistry,Characterization,Analysis,Recycling,and Application(BACCARA)Open Access funding enabled and organized by Projekt DEAL。
文摘Li/Mn-rich layered oxide(LMR)cathode active materials offer remarkably high specific discharge capacity(>250 mAh g^(-1))from both cationic and anionic redox.The latter necessitates harsh charging conditions to high cathode potentials(>4.5 V vs Li|Li^(+)),which is accompanied by lattice oxygen release,phase transformation,voltage fade,and transition metal(TM)dissolution.In cells with graphite anode,TM dissolution is particularly detrimental as it initiates electrode crosstalk.Lithium difluorophosphate(LiDFP)is known for its pivotal role in suppressing electrode crosstalk through TM scavenging.In LMR‖graphite cells charged to an upper cutoff voltage(UCV)of 4.5 V,effective TM scavenging effects of LiDFP are observed.In contrast,for an UCV of 4.7 V,the scavenging effects are limited due to more severe TM dissolution compared an UCV of 4.5V.Given the saturation in solubility of the TM scavenging agents,which are LiDFP decomposition products,e.g.,PO_(4)^(3-) and PO_(3)F^(2-),higher concentrations of the LiDFP as precursor"cannot enhance the amount of scavenging species,they rather start to precipitate and damage the anode.
基金financially supported by the National Key R&D Program of China(2021YFB3800300)the National Natural Science Foundation of China(22179143 and 22309202)+1 种基金the Jiangsu Funding Program for Excellent Postdoctoral Talentthe Gusu Leading Talents Program(ZXL2023190)。
文摘Integrating high-nickel layered oxide cathodes with aqueous slurry electrode preparation routes holds the potential to simultaneously meet the demands for high energy density and low-cost production of lithium-ion batteries.However,the influence of dual exposure to air and liquid water as well as the heating treatment during aqueous slurry electrode processing on the high-nickel layered oxide electrode is yet to be understood.In this study,we systematically investigate the structural evolution and electro-chemical behaviors when LiNi_(0.83)Mn_(0.05)Co_(0.12)O_(2)(NMC83)is subjected to aqueous slurry processing.It was observed that the crystal structure near the surface of NMC83 is partially reconstructed to contain a mixture of rock-salt and layered phases when exposed to water,leading to the deteriorated rate capability of the NMC83 electrodes.This partial surface reconstruction layer completely converts into a pure rock-salt phase upon cycling,accompanied by the release of O_(2),Ni leaching,catalyzed decomposition of the electrolyte,and the formation of a thick cathode electrolyte interphase layer.The byproducts of the electrolyte and dissolved Ni could shuttle to the Li metal side,causing a crosstalk effect that results in a thick and unstable solid electrolyte interphase layer on the Li surface.These in combination severely undermined the cycling stability of the NMC83 electrodes obtained from the aqueous slurry.A mitigation strategy using molecular self-assembly technique was demonstrated to enhance the surface stability of water-treated NMC83.Our findings offer new insights for tailoring ambient environment stability and aqueous slurry processability for ultra-high nickel layered oxide and other water-sensitive cathode materials.
基金financially supported by the National Natural Science Foundation of China under Grant numbers 22379030,52001079 and 52261038the Guangxi Key Laboratory of Green Manufacturing for Ecological Aluminum Industry(GXGMEA2024)the Nanning Excellent Young Talents Cultivation Project for Scientific and Technological Innovation and Entrepreneurship(RC20220102).
文摘The deposition of ultrafine single-atom nickel particles on Nb_(2)C(MXene)was successfully achieved using a wet chemistry method to synthesize Ni@Nb_(2)C composite.This study explored the effect of Ni@Nb_(2)C on the hydrogen absorption and desorption properties of MgH_(2) through theoretical calculations and experimental investigations.Under the catalytic action of Ni@Nb2C,the initial dehydrogenation temperature of MgH_(2) was reduced by 121℃,with approximately 4.26 wt.% of H_(2) desorbed at 225℃ in 100 min.The dehydrogenation activation energy of the MgH_(2)+Ni@Nb_(2)C composite dropped to 86.7 kJ·mol^(-1),a reduction of 60.5 kJ·mol^(-1) compared to pure MgH_(2).Density functional theory calculations indicated that the incorporation of Ni@Nb_(2)C enhanced the performance of MgH_(2) performance by improving interactions among Nb_(2)C,Ni,Mg,and H atoms.In the Ni@Nb_(2)C+MgH_(2) system,the lengths of Mg-H bonds(1.91-1.99 A)were found to be longer than those observed in pure MgH_(2)(1.71 A).The dehydrogenation energy for this system(1.08 eV)was lower than that for Nb_(2)C(1.52 eV).These findings suggest that the synergistic effect of Ni and Nb2C significantly enhances the hydrogenation/dehydrogenation kinetics of MgH_(2),thereby introducing a novel approach for catalytic modification of solid hydrogen storage materials through synergistic actions.
基金supported by Ministry of TradeIndustry&Energy/Korea Evaluation Institute of Industrial Technology(MOTIE/KEIT)(No.RS-2024-00406080)an Institute of Information&Communications Technology Planning&Evaluation(IITP)grant funded by the Korean government(MSIT)(RS-2023-00221723)。
文摘The robust respective formations of a solid electrolyte interphase(SEI)and pillar at the surfaces of hard carbon and O3-type positive electrodes are the consequences of integrating Li PF_6 salt into a sodium-ion battery electrolyte that considerably strengthens both interfaces of positive and negative electrodes.The improvement of cycle performances due to the formation of highly passivating SEI on the hard carbon electrode is induced by the alternated solvation structure following the addition of Li salt,which inhibits sodium-ion and electron leakage from further electrolyte decomposition.The SEI with incorporated Li is less soluble than Na-based SEI,and the passivation ability of the initially formed SEI can thus be well preserved.Conversely,the gas evolution caused by oxygen release is reduced considerably by the marginal surface intercalation of Li ions at the surface of the O3-positive electrode.Additionally,the Li F layer that forms on the O3 surface diminishes additional deterioration of the electrolyte after formation.Compared with the fluoroethylene carbonate additive that is typically applied,a simultaneously strengthened interface yields major improvements in capacity retention.
基金funding support from National Key R&D Program of China (No. 2023YFB3809500)the National Natural Science Foundation of China (U24A20566, 22279121, 52525203, 52394170, 52394171, U24A2067, U22A20439)+2 种基金Joint Fund of Scientific and Technological Research and Development Program of Henan Province (222301420009)Key Research and Development Program of Henan Province (231111241400)the funding of Zhengzhou University。
文摘The increasingly severe energy crisis and environmental issues have raised higher requirements for grid-scale energy storage systems.Rechargeable batteries have enormous development prospects due to their flexibility and environmental protection. However, the traditional organic liquid-based batteries cannot meet our needs for future advanced batteries in terms of safety, energy density, and stability under extreme working conditions. In this case, we comprehensively summarize various advanced battery technologies to overcome the above problems.Firstly, we highlight the advantage of solid-state batteries compared to liquid electrolytes. Specifically, we focus on the advantages and challenges of solid-state lithium/sodium batteries and other types of solid-state batteries associated with the electrodes, solid electrolytes and the electrode/electrolyte interphase. Secondly, we discuss the environmentally friendly and safe liquid-state battery and its application prospect.Thirdly, the battery improvement strategy has been proposed to enhance the application of batteries under extreme conditions. Subsequently, we emphasize the importance of theoretical calculations and AI technology in promoting the development of battery technology. Finally, the current challenges and future directions of battery technology are summarized. The combination of in-depth failure mechanism analysis, advanced characterization techniques, economic commercialization and machine learning enables the rapid development of advanced battery technology for sustainable energy storage.
基金financially supported by the National Natural Science Foundation of China(22071137)。
文摘Activating MoS_(2) with atomic metal doping is promising to harvest desirable Pt-matched hydrogen evolution reaction(HER)catalytic performance.Herein,we developed an efficient method to access edgerich lattice-distorted MoS_(2) for highly efficient HER via in-situ sulphuration of atomic Co/Mo species that were well-dispersed in a formamide-derived N-doped carbonaceous(f-NC)substrate.Apart from others,pre-embedding Co/Mo species in f-NC controls the release of metal sources upon annealing in S vapor,grafting the as-made MoS_(2) with merits of short-range crystallinity,distorted lattices,rich defects,and more edges exposed.The content of atomic Co species embedded in MoS_(2) reaches up to 2.85 at.%,and its atomic dispersion has been systematically confirmed by using XRD,HRTEM,XPS,and XAS characterizations.The Co-doped MoS_(2) sample exhibits excellent HER activity,achieving overpotentials of 67 and155 m V at j=10 m A cm^(-2) in 1.0 M KOH and 0.5 M H_(2)SO_(4),respectively.Density functional theory simulations suggest that,compared with free-doping MoS_(2),the edged Co doping is responsible for the significantly improved HER activity.Our method,in addition to providing reliable Pt-matched HER catalysts,may also inspire the general synthesis of edge-rich metal-doped metal chalcogenide for a wide range of energy conversion applications.
基金supported by a grant(code #05K1501-01920) from ‘Center for Nanostructured Materials Technology’ under ‘21st Century Frontier R&D Programs’ of the Ministry of Science and Technology,Korea
文摘Phosphorus doped silicon-carbon composite particles were synthesized through a DC arc plasma torch.Silane(SiH4) and methane(CH4) were introduced into the reaction chamber as the precursor of silicon and carbon,respectively.Phosphine(PH3) was used as a phosphorus dopant gas.Characterization of synthesized particles were carried out by scanning electron microscopy(SEM),X-ray diffractometry(XRD),X-ray photoelectron spectroscopy(XPS) and bulk resistivity measurement.Electrochemical properties were investigated by cyclic test and electrochemical voltage spectroscopy(EVS).In the experimental range,phosphorus doped silicon-carbon composite electrode exhibits enhanced cycle performance than intrinsic silicon and phosphorus doped silicon.It can be explained that incorporation of carbon into silicon acts as a buffer matrix and phosphorus doping plays an important role to enhance the conductivity of the electrode,which leads to the improvement of the cycle performance of the cell.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea Government(MSIT)(NRF-2020R1A3B2079803),Republic of Korea.
文摘Lithium–sulfur batteries(LSBs)are regarded as promising candidates for the next-generation energy storage devices owing to their high-theoretical capacity(1675 mAh g^(−1))and affordable cost.However,several limitations of LSBs such as the lithium polysulfide shuttle,large volume expansion,and low electrical conductivity of sulfur need to be resolved for practical applications.To address these limitations,herein,a multidimensional architectured hybrid(Co@CNT/nG),where Co_(3)O_(4) nanoparticles are encapsulated into threedimensional(3D)porous N-doped reduced graphene oxide interconnected with carbon nanotube(CNT)branches,is synthesized through a simple pyrolysis method.The synergistic effect achieved through the homogeneously distributed and encapsulated Co_(3)O_(4) nanoparticles,the interconnected CNT branches,and the 3D hierarchical porous structure and N-doping of Co@CNT/nG significantly suppresses the shuttle effect of lithium polysulfides and enhances the conversion redox kinetics for the improved sulfur utilization.We validate this effect through various measurements including symmetric cells,Li_(2)S nucleation,shuttle currents,Tafel slopes,diffusion coefficients,and post-mortem analyses.Importantly,Co@CNT/nG-70S-based LSB cells achieve a high-specific capacity of 1193.1 mAh g^(−1) at 0.1 C and a low capacity decay rate of 0.030%per cycle for 700 cycles at 5 C,delivering a high areal capacity of 5.62 mAh cm^(−2) even with a loading of 6.5 mg cm^(−2).
基金supported by a grant from R&D Program of the Korea Railroad Research Institute,Republic of Korea。
文摘Lithium-sulfur(Li-S)batteries are receiving increasing attention as one of the potential next-generation batteries,owing to their high energy densities and low cost.However,practical Li-S batteries with high energy densities are extremely hindered by the sulfur loss,low Coulombic efficiency,and short cycling life originating from the polysulfide(LiPS)shuttle.In this study,two-dimensional(2D)ZnCo_(2)O_(4) microsheets fabricated by a facile hydrothermal process are employed to modify the separator,for improving the electrochemical performances of Li-S cells.The resulting 2D Zn Co_(2)O_(4)-coated separator features a coating thickness of approximately 10 lm,high ionic conductivity of 1.8 m S/cm,and low mass loading of 0.2 mg/cm^(2).This 2D ZnCo_(2)O_(4)-coated separator effectively inhibits Li PS shuttle by a strong chemical interaction with Li PS as well as promotes the redox kinetics by Zn CO2O4-coated layers,as determined by X-ray photoelectron spectroscopy analysis,self-discharge,time-dependent permeation test,Li symmetric cell test,and Li2S nucleation analyses.Consequently,the Li-S batteries based on the 2D Zn Co_(2)O_(4)-coated separator exhibit a high initial discharge capacity of 1292.2 m Ah/g at 0.1 C.Moreover,they exhibit excellent long cycle stability at 1 and 2 C with capacity retention of 84%and 86%even after800 cycles,corresponding to a capacity fading rate of 0.020%and 0.016%per cycle,respectively.Effectively,these Li-S cells with a high sulfur loading at 5.3 mg/cm^(2) and low electrolyte concentration of 9 l L/mg deliver a high discharge capacity of 4.99 m Ah/cm^(2) after 200 cycles at 0.1 C.
基金The support provided by the German Federal Ministry of Education and Research(BMBF)within the project“Benchbatt”(03XP0047B)is gratefully acknowledged.
文摘The solvent-free in situ polymerization technique has the potential to tailor-make conformal interfaces that are essential for developing durable and safe lithium metal polymer batteries(LMPBs).Hence,much attention has been given to the eco-friendly and rapid ultraviolet(UV)-induced in situ photopolymerization process to prepare solid-state polymer electrolytes.In this respect,an innovative method is proposed here to overcome the challenges of UV-induced photopolymerization(UV-curing)in the zones where UV-light cannot penetrate,especially in LMPBs where thick electrodes are used.The proposed frontal-inspired photopolymerization(FIPP)process is a diverged frontal-based technique that uses two classes(dual)of initiators to improve the slow reaction kinetics of allyl-based monomers/oligomers by at least 50%compared with the conventional UV-curing process.The possible reaction mechanism occurring in FIPP is demonstrated using density functional theory calculations and spectroscopic investigations.Indeed,the initiation mechanism identified for the FIPP relies on a photochemical pathway rather than an exothermic propagating front forms during the UV-irradiation step as the case with the classical frontal photopolymerization technique.Besides,the FIPP-based in situ cell fabrication using dual initiators is advantageous over both the sandwich cell assembly and conventional in situ photopolymerization in overcoming the limitations of mass transport and active material utilization in high energy and high power LMPBs that use thick electrodes.Furthermore,the LMPB cells fabricated using the in situ-FIPP process with high mass loading LiFePO_(4)electrodes(5.2 mg cm^(-2))demonstrate higher rate capability,and a 50%increase in specific capacity against a sandwich cell encouraging the use of this innovative process in large-scale solid-state battery production.
基金financially supported by the National Natural Science Foundation of China (No. 51771171, and 51971199)Education Department of Guangxi Zhuang Autonomous Region (No. 2019KY0021)the Natural Science Foundation of Guangxi Province (2019GXNSFBA185004, and 2018GXNSFAA281308)。
文摘Aluminum hydride(AlH3) is a binary metal hydride that contains more than 10.1 wt% of hydrogen and possesses a high volumetric hydrogen density of 148 kg H2 m^(-3).Pristine AlH3 can readily release hydrogen at a moderate temperature below 200℃.Such high hydrogen density and low desorption temperature make AlH3 one of most promising hydrogen storage media for mobile application.This review covers the research activity on the structures,synthesis,decomposition thermodynamics and kinetics,regeneration and application validation of AlH3 over the past decades.Finally,the future research directions of AlH3 as a hydrogen storage material will be revealed.
