Severe lithium dendrite growth and elevated thermal runaway risks pose significant hurdles for fast-charging lithium metal batteries(LMBs)This study reports a polydopamine-functionalized hydroxyapatite/aramid(PDA@HA)h...Severe lithium dendrite growth and elevated thermal runaway risks pose significant hurdles for fast-charging lithium metal batteries(LMBs)This study reports a polydopamine-functionalized hydroxyapatite/aramid(PDA@HA)hybrid nanofibers separator to synchronously improve th fast-charging LMB's stability and safety.(1)The separator's surface,enriched with lithiophilic carbonyl and hydroxyl groups,accelerates Li~+ion desolvation,while electrophilic imine groups impede anion movement.This dual mechanism optimizes the Li^(+)-ion flux distribution on th anode,mitigating dendrite formation.(2)The polar PDA modification layer fosters the development of a Li_(3)N/LiF-rich solid electrolyt interface,further enhancing Li anode stability.Consequently,Li//Li symmetric cells with PDA@HA separators exhibit extended cycle life in L plating/stripping tests:5000 h at 1 mA cm^(-2)and 700 h at 20 mA cm^(-2),respectively,outperforming PP separators(80 h and 8 h).In LiFePO_(4)(LFP,^(2.1)mg cm^(-2))//Li full cell evaluation,the PDA@HA separator enables stable operation for 11,000 cycles at 18.2C with 87%capacity retention,significantly outperforming existing fast-charging LMB counterparts in literature.At a high LFP loading of 15.5 mg cm^(-2),the cel maintains 137.6 mAh g^(-1)(2.13 mAh cm^(-2))over 250 cycles at 3C,achieving 98%capacity retention.Moreover,the PDA@HA separato increases threshold temperature for thermal runaway and reduces the exothermic rate,intensifying the battery's thermal safety.This research underscores the importance of functional separator design in improving Li metal anode reversibility,fast-charging performance,and therma safety of LMBs.展开更多
Weakly solvating electrolyte(WSE)demonstrates superior compatibility with lithium(Li)metal batteries(LMBs).However,its application in fast-charging high-voltage LMBs is challenging.Here,we propose a diluent modified W...Weakly solvating electrolyte(WSE)demonstrates superior compatibility with lithium(Li)metal batteries(LMBs).However,its application in fast-charging high-voltage LMBs is challenging.Here,we propose a diluent modified WSE for fast-charging high-voltage LMBs,which is formed by adding diluent of 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether(TTE)into the tetrahydropyran(THP)based WSE.A relatively loose solvation structure is formed due to the formation of weak hydrogen bond between TTE and THP,which accelerates the de-solvation kinetics of Li~+.Besides,more anions are involved in solvation structure in the presence of TTE,yielding inorganic-rich interphases with improved stability.Li(30μm)||Li Ni_(0.5)Co_(0.2)Mn_(0.3)O_(2)(4.1 mAh/cm^(2))batteries with the TTE modified WSE retain over 64%capacity retention after 175 cycles under high rate of 3 C and high-voltage of 4.5 V,much better than that with pure THP based WSE.This work points out that the combination of diluent with weakly solvating solvent is a promising approach to develop high performance electrolytes for fast-charging high-voltage LMBs.展开更多
Despite the growing interest in fast-cha rging solid-state lithium(Li)-metal batteries(SSLMBs),their practical implementation has yet to be achieved,primarily due to an incomplete understanding of the disparate and of...Despite the growing interest in fast-cha rging solid-state lithium(Li)-metal batteries(SSLMBs),their practical implementation has yet to be achieved,primarily due to an incomplete understanding of the disparate and often conflicting requirements of the bulk electrolyte and the electrode-electrolyte interphase.Here,we present a weakly coordinating cationic polymer electrolyte(WCPE)specifically designed to regulate the Li^(+)coordination structure,thereby enabling fast-charging SSLMBs.The WCPE comprises an imidazolium-based polycationic matrix combined with a succinonitrile(SN)-based highconcentration electrolyte.Unlike conventional neutral polymer matrices,the polycationic matrix in the WCPE competes with Li^(+)for interactions with SN,weakening the original coordination between SN and Li^(+).This modulation of SN-Li^(+)interaction improves both Li^(+)conductivity of the WCPE(σ_(Li^(+))=1.29mS cm^(-1))and redox kinetics at the electrode-electrolyte interphase.Consequently,SSLMB cells(comprising LiFePO_(4)cathodes and Li-metal anodes)with the WCPE achieve fast-charging capability(reaching over 80%state of charge within 10 min),outperforming those of previously reported polymer electrolytebased SSLMBs.展开更多
Na_(3)V_(2)(PO_(4))_(2)O_(2)F (VP) is recognized as a promising cathode material for sodium-ion batteries due to its stable structural framework and high specific capacity.Density functional theory (DFT) and finite el...Na_(3)V_(2)(PO_(4))_(2)O_(2)F (VP) is recognized as a promising cathode material for sodium-ion batteries due to its stable structural framework and high specific capacity.Density functional theory (DFT) and finite element simulations show that incorporating SO_(4)^(2-)into VP decreases its band gap,lowers the migration energy barrier,and ensures a uniform Na+concentration gradient and stress distribution during charge and discharge cycles.Consequently,the average Na+diffusion coefficient of Na_(3)V_(2)(PO_(4))_(1.95)(SO_(4))_(0.05)O_(2)F(VPS-1) is roughly double that of VP,leading to enhanced rate capability (80 C,75.5 mAh g^(-1)) and cycling stability (111.0 mAh g^(-1)capacity after 1000 cycles at 10 C current density) for VPS-1.VPS-1 exhibits outstanding fast-charging capabilities,achieving an 80%state of charge in just 8.1 min.The assembled VPS-1//SbSn/NPC full cell demonstrated stable cycling over 200 cycles at a high 5 C current,maintaining an average coulombic efficiency of 95.35%.展开更多
As one of the alloy-type lithium-ion electrodes,Bi has outstanding application prospects for large volume capacity(3800 mAh·cm^(-3))and high electronic conductivity(1.4×10^(7)S·m^(-1)).However,the fast-...As one of the alloy-type lithium-ion electrodes,Bi has outstanding application prospects for large volume capacity(3800 mAh·cm^(-3))and high electronic conductivity(1.4×10^(7)S·m^(-1)).However,the fast-charging performance is hindered by significant volume expansion(>218%)and a low rate of phase diffusion.To overcome these two problems,an N-doped carbon nanoflower coating layer was elaborately in-situ reconstructed on a multiple-wall Bi microsphere by hydrothermal methods and subsequent calcination in this study.The carbon nanoflowers greatly increase specific surface area(40.0 m^(2)·g^(-1))and alleviate the volume expansion(130%).In addition,the incorporation of N-doped carbon nanoflowers leads to a gradual enhancement in the Li adsorption energy of Bi during the process of lithium insertion and improves the electrical conductivity.Therefore,the contribution rate of pseudo-capacitance reached 87.5%at the scan rate of 0.8 mV·s^(-1),and the Li-ion diffusion coefficient(D_(Li^(+)))was calculated in the range of 10^(-10)to 10^(-12)cm^(2)·s^(-1).The Bi@CNFs anode provided a high specific volumetric capacity of 2117.0 mAh·cm^(-3)at 5C and a high capacity retention ratio of 93.2%after 800 cycles.The Bi@CNFs//LiFePO_(4)full cell also displayed a stable capacity of 113.9 mAh·g^(-1)and energy density of 296.1 Wh·kg^(-1)after 100 cycles with a Coulombic efficiency of 97.6%.The mechanism of fast-charging lithium storage was verified by distribution of relaxation time analysis and density functional theory calculation.This paper provides a new strategy to increase the pseudo-capacitance and reduce the volume expansion for the preparation of alloy-type fast-charging electrodes.展开更多
For the advancement of fast-charging sodium-ion batteries(SIBs),the synthesis of cutting-edge cathode materials with superior structural stability and enhanced Na+diffusion kinetics is imperative.Multiphase layered tr...For the advancement of fast-charging sodium-ion batteries(SIBs),the synthesis of cutting-edge cathode materials with superior structural stability and enhanced Na+diffusion kinetics is imperative.Multiphase layered transition metal oxides(LTMOs),which leverage the synergistic properties of two distinct monophasic LTMOs,have garnered significant attention;however,their efficacy under fast-charging conditions remains underexplored.In this study,we developed a high-throughput computational screening framework to identify optimal dopants that maximize the electrochemical performance of LTMOs.Specifically,we evaluated the efficacy of 32 dopants based on P2/O3-type Mn/Fe-based Na_(x)Mn_(0.5)Fe_(0.5)O_(2)(NMFO)cathode material.Multiphase LTMOs satisfying criteria for thermodynamic and structural stability,minimized phase transitions,and enhanced Na^(+)diffusion were systematically screened for their suitability in fast-charging applications.The analysis identified two dopants,Ti and Zr,which met all predefined screening criteria.Furthermore,we ranked and scored dopants based on their alignment with these criteria,establishing a comprehensive dopant performance database.These findings provide a robust foundation for experimental exploration and offer detailed guidelines for tailoring dopants to optimize fast-charging SIBs.展开更多
High-energy–density lithium-ion batteries(LIBs)that can be safely fast-charged are desirable for electric vehicles.However,sub-optimal lithiation potential and low capacity of commonly used LIBs anode cause safety is...High-energy–density lithium-ion batteries(LIBs)that can be safely fast-charged are desirable for electric vehicles.However,sub-optimal lithiation potential and low capacity of commonly used LIBs anode cause safety issues and low energy density.Here we hypothesize that a cobalt vanadate oxide,Co_(2)VO_(4),can be attractive anode material for fast-charging LIBs due to its high capacity(~1000 mAh g^(−1))and safe lithiation potential(~0.65 V vs.Li^(+)/Li).The Li+diffusion coefficient of Co2VO4 is evaluated by theoretical calculation to be as high as 3.15×10^(-10) cm^(2) s^(−1),proving Co_(2)VO_(4) a promising anode in fast-charging LIBs.A hexagonal porous Co2VO4 nanodisk(PCVO ND)structure is designed accordingly,featuring a high specific surface area of 74.57 m^(2) g^(−1) and numerous pores with a pore size of 14 nm.This unique structure succeeds in enhancing Li^(+) and electron transfer,leading to superior fast-charging performance than current commercial anodes.As a result,the PCVO ND shows a high initial reversible capacity of 911.0 mAh g^(−1) at 0.4 C,excellent fast-charging capacity(344.3 mAh g^(−1) at 10 C for 1000 cycles),outstanding long-term cycling stability(only 0.024% capacity loss per cycle at 10 C for 1000 cycles),confirming the commercial feasibility of PCVO ND in fast-charging LIBs.展开更多
Hybrid Na-ion capacitors(NICs)have received considerable interests owing to their low-cost,high-safety,and rapidly charging energy-storage characteristics.The NICs are composed of a capacitor-type cathode and a batter...Hybrid Na-ion capacitors(NICs)have received considerable interests owing to their low-cost,high-safety,and rapidly charging energy-storage characteristics.The NICs are composed of a capacitor-type cathode and a battery-type anode.The major challenge for NICs is to search for suitable electrode materials to overcome the sluggish diffusion of Na^(+)in the anode.Herein,ultrafine vanadium sulfide is encapsulated in carbon fiber(V_(3)S_(4)@CNF)as a self-supported electrode by electrospinning and in situ sulfurization.The carbon cladding and one-dimensional(ID)nanofiber network-like structure could alleviate the volume expansion of V_(3)S_(4)during Na^(+)de-/intercalation process.Consequently,the V_(3)S_(4)@CNF anode exhibited a pseudocapacitive sodium storage in terms of large Na^(+)-storage capacity(476 mAh·g^(-1)at 0.1A·g^(-1)),high-rate capability(290 mAh·g^(-1)at 20.0 A·g^(-1))and excellent cycling stability(95%capacity retention for1500 cycles at 2.0 A·g^(-1))in Na half-cells.By employing V_(3)S_(4)@CNF as the anode and the activated carbon(AC)cathode,the as-assembled NICs could deliver a high energy density of 110 Wh·kg^(-1)at a power density of200 W·kg^(-1).Even at a high power of 10,000 W·kg^(-1),the specific energy is still up to 42 Wh·kg^(-1).展开更多
With the ever-growing application of lithium-ion batteries(LIBs), their fast-charging technology has attracted great interests of scientists. However, growth of lithium dendrites during fast charge of the bat teries w...With the ever-growing application of lithium-ion batteries(LIBs), their fast-charging technology has attracted great interests of scientists. However, growth of lithium dendrites during fast charge of the bat teries with high energy density may pose great threats to the operation and cause serious safety issues Herein, we prepared a functional separator with an ultra-thin(20 nm) layer of Au nanoparticles deposited by evaporation coating method which could regulate growth direction and morphology of the lithium dendrites, owing to nearly zero overpotential of lithium meal nucleation on lithiated Au. Once the Li den drites are about to form on the graphite anode during fast charging(or lithiation), they plate predomi nantly on the Au deposited separator rather than on the graphite. Such selective deposition does no compromise the electrochemical performance of batteries under normal cycling. More importantly, i enables the better cycling stability of batteries at fast charge condition. The Li/Graphite cells with Au nanoparticles coated separator could cycle stably with a high areal capacity retention of 90.5% over 95 cycles at the current density of 0.72 m A cm^(-2). The functional separator provides an effective strategy to adjust lithium plating position at fast charge to ensure high safety of batteries without a compromise on the energy density of LIBs.展开更多
Silicon/carbon composites are promising alternatives to current graphite anodes in commercial lithiumion batteries(LIBs)because of their high capacity and excellent safety.Nevertheless,the unsatisfactory fastcharging ...Silicon/carbon composites are promising alternatives to current graphite anodes in commercial lithiumion batteries(LIBs)because of their high capacity and excellent safety.Nevertheless,the unsatisfactory fastcharging capability and cycle stability of Si/C composites caused by slow charge transport capability and huge volume change under industrial electrode conditions severely hamper their development.Here,a novel Si/C anode was fabricated by homogeneously depositing amorphous C-Si nanolayers on graphite(C-Si@graphite).C-Si nanolayers with uniformly dispersed sub-nanometer Si particles in 3D carbon skeleton significantly boost electron and Li-ion transport and efficiently relieve Si's agglomeration and volume change.As a result,the tailored C-Si@graphite electrodes show an excellent rate capacity(760.3 mAh·g^(-1)at 5.0C)and long cycle life of over 1000 cycles at 1.0C and800 cycles at 2.0C under industrial electrode conditions.In addition,the assembled full cells(C-Si@graphite,anode;Li[Ni_(0.8)Co_(0.1)Mn_(0.1)]O_(2),cathode)present superior fastcharging capability(240.4 Wh·kg^(-1),charging for16.2 min,3.0C)and long cycle life(80.7%capacity retention after 500 cycles at 1.0C),demonstrating the massive potential of C-Si@graphite for practical application.展开更多
Fast-charging and low temperature operation are of vital importance for the further development of lithium-ion batteries(LIBs),which is hindered by the utilization of conventional carbonate-based electrolytes due to t...Fast-charging and low temperature operation are of vital importance for the further development of lithium-ion batteries(LIBs),which is hindered by the utilization of conventional carbonate-based electrolytes due to their slow kinetics,narrow operating temperature and voltage range.Herein,an acetonitrile(AN)-based localized high-concentration electrolyte(LHCE)is proposed to retain liquid state and high ionic conductivity at ultra-low temperatures while possessing high oxidation stability.We originally reveal the excellent thermal shielding effect of non-solvating diluent to prevent the aggregation of Li^(+) solvates as temperature drops,maintaining the merits of fast Li transport and facile desolvation as at room temperature,which bestows the graphite electrode with remarkable low temperature performance(264 mA h g^(-1) at-20 C).Remarkably,an extremely high capacity retention of 97%is achieved for high-voltage high-energy graphite||NCM batteries after 250 cycles at-20 C,and a high capacity of 110 mA h g^(-1)(71%of its room-temperature capacity)is retained at-30°C.The study unveils the key role of the non-solvating diluents and provides instructive guidance in designing electrolytes towards fast-charging and low temperature LIBs.展开更多
Dendrite growth of zinc(Zn)anode at high current density severely affects the fast-charging performance of aqueous zinc metal batteries(AZMBs).While interfacial modification strategies can optimize Zn per formance,cha...Dendrite growth of zinc(Zn)anode at high current density severely affects the fast-charging performance of aqueous zinc metal batteries(AZMBs).While interfacial modification strategies can optimize Zn per formance,challenges such as complicated preparation processes,excessive layer thicknesses,and high voltage hysteresis should be addressed.Herein,we utilize a cost-effective liquid fluorosiloxane,(3,3,3trifluoropropyl)trimethoxysilane,for scalable modification of Zn foil via drop-casting at room tempera ture,resulting in an ultra-thin interphase layer of only 20 nm.The Si-O-Zn bonds formed between flu orosiloxane and Zn ensure interfacial stability,and the Si-O-Si bonds between fluorosiloxane molecule help to homogenize the electric field distribution.Additionally,the abundant highly electronegative flu orine atoms on the anode surface act as zincophilic sites,promoting the uniform deposition of Zn^(2+)Thus,the modified Zn foil(SiFO-Zn)exhibits excellent dendrite suppression,reduced voltage hysteresis and prolonged cycle life at ultra-high current density(40 mA/cm^(2)),achieving a cumulative areal capac ity of 12.9 Ah/cm^(2).Further,the full cell assembled with 10μm-thick Si FO-Zn anode and MnO_(2)cathode achieves 2600 cycles at 5 A/g with minimal capacity degradation,and a large-size(22.5 cm^(-2))pouch cel powers the light-emitting diode even after reverse bending,demonstrating the potential of AZMBs fo fast-charging flexible devices.展开更多
Lithium-ion batteries(LIBs)with the“double-high”characteristics of high energy density and high power density are in urgent demand for facilitating the development of advanced portable electronics.However,the lithiu...Lithium-ion batteries(LIBs)with the“double-high”characteristics of high energy density and high power density are in urgent demand for facilitating the development of advanced portable electronics.However,the lithium ion(Li+)-storage performance of the most commercialized lithium cobalt oxide(LiCoO_(2),LCO)cathodes is still far from satisfactory in terms of high-voltage and fast-charging capabilities for reaching the double-high target.Herein,we systematically summarize and discuss high-voltage and fast-charging LCO cathodes,covering in depth the key fundamental challenges,latest advancements in modification strategies,and future perspectives in this field.Comprehensive and elaborated discussions are first presented on key fundamental challenges related to structural degradation,interfacial instability,the inhomogeneity reactions,and sluggish interfacial kinetics.We provide an instructive summary of deep insights into promising modification strategies and underlying mechanisms,categorized into element doping(Li-site,cobalt-/oxygen-site,and multi-site doping)for improved Li+diffusivity and bulkstructure stability;surface coating(dielectrics,ionic/electronic conductors,and their combination)for surface stability and conductivity;nanosizing;combinations of these strategies;and other strategies(i.e.,optimization of the electrolyte,binder,tortuosity of electrodes,charging protocols,and prelithiation methods).Finally,forward-looking perspectives and promising directions are sketched out and insightfully elucidated,providing constructive suggestions and instructions for designing and realizing high-voltage and fast-charging LCO cathodes for next-generation double-high LIBs.展开更多
Adopting the metalized plastic current collector(MPCC)enhances the safety and specific energy density of lithium-ion batteries(LIBs)but sacrifices the rate capability.The reduced rate capability is customarily ascribe...Adopting the metalized plastic current collector(MPCC)enhances the safety and specific energy density of lithium-ion batteries(LIBs)but sacrifices the rate capability.The reduced rate capability is customarily ascribed to the lower electronic conductivity of MPCC as compared with the metal ones(e.g.,Al and Cu)due to the less metal usage.Here,we demonstrate that the interfacial contact between the current collector(CC)and the active-material layer,rather than the electronic conductivity of CC,accounts for the rate performance of the cells.By introducing a thin carbon coating(~300 nm)onto the surface of MPCC(e.g.,1μm thick aluminum deposited on both sides of 10μm polyethylene terephthalate(PET)film,Al-PET),we reduced the contact resistance between MPCC and cathode materials.Using the carbon-coated Al-PET(C@Al-PET)as CC,the 6.0-Ah graphite/LiCoO_(2)pouch cell delivers significantly improved fast-charge capability and cycling stability,which are identified as the homogenized potential distribution and electrode utilization with multiphysical field simulations.Most importantly,the cell with C@Al-PET CC could still pass the harsh impact test,promising its applications in high-rate LIBs with superior safety.展开更多
Lithium(Li)metal anodes(LMAs)have garnered significant attention due to their exceptionally high theoretical capacity and low redox potentials.However,the uncontrolled growth of Li dendrites and substantial volume exp...Lithium(Li)metal anodes(LMAs)have garnered significant attention due to their exceptionally high theoretical capacity and low redox potentials.However,the uncontrolled growth of Li dendrites and substantial volume expansion severely undermine their cycling stability,particularly at elevated current densities.Herein,we develop a lithiophilic 3D Li host by incorporating ZnO/ZnSe heterostructures onto brass fibers(ZnO/ZnSe@Brass),designed to enhance the fast-charging capabilities of Li metal batteries.This hierarchical structure effectively mitigates volume expansion and reduces local current density during lithiation.The uniformly distributed ZnO/ZnSe functions as a lithiophilic skin for the Li anode,facilitating smooth and dense Li deposition.Notably,the in situ formed solid electrolyte interphase,enriched with Li_(2)Se and Li_(2)O,provides high ionic conductivity and superior mechanical strength,thereby accelerating ion transport and charge transfer kinetics.Benefiting from the synergistic effects of the ZnO/ZnSe@Brass host,the resulting Li symmetric cell exhibits robust cycling performance exceeding 10,000 cycles(20 mA cm^(−2)/1 mA h cm^(−2))and supports fast charging rates at an ultra-high current density of 80 mA cm^(−2).When paired with LiFePO4,the full-cell demonstrates excellent cycle life(>500 cycles at 2 C)and outstanding rate performance.This finding of ZnO/ZnSe@Brass as a Li host sheds light on the design of advanced LMAs for fast-charging Li metal batteries.展开更多
The safe,flexible,and environment-friendly Zn-ion batteries have aroused great interests nowadays.Nevertheless,flagrant Zn dendrite uncontrollably grows in liquid electrolytes due to insufficient surface protection,wh...The safe,flexible,and environment-friendly Zn-ion batteries have aroused great interests nowadays.Nevertheless,flagrant Zn dendrite uncontrollably grows in liquid electrolytes due to insufficient surface protection,which severely impedes the future applications of Zn-ion batteries especially at high current densities.Gel electrolytes are emerging to tackle this issue,yet the required high modulus for inhibiting dendrite growth as well as concurrent poor interfacial contact with roughened Zn electrodes are not easily reconcilable to regulate the fragile Zn/Zn^(2+) interface.Here we demonstrate,such a conflict may be defeated by using a mechanoadaptive cellulose nanofibril-based morphing gel electrolyte(MorphGE),which synergizes bulk compliance for optimizing interfacial contact as well as high modulus for suppressing dendrite formation.Moreover,by anchoring desolvated Zn^(2+) on cellulose nanofibrils,the side reactions which induce dendrite formation are also significantly reduced.As a result,the MorphGE-based symmetrical Zn-ion battery demonstrated outstanding stability for more than 100 h at the high current density of 10 mA·cm^(−2) and areal capacity of 10 mA·h·cm^(−2),and the corresponding Zn-ion battery delivered a prominent specific capacity of 100 mA·h·g^(−1) for more than 500 cycles at 20 C.The present example of engineering the mechanoadaptivity of gel electrolytes will shed light on a new pathway for designing highly safe and flexible energy storage devices.展开更多
Fast-charging is highly demanded for applications requiring short charging time.However,fast-charging triggers serious problems,leading to decline in charge acceptance and energy efficiency,accelerated capacity degrad...Fast-charging is highly demanded for applications requiring short charging time.However,fast-charging triggers serious problems,leading to decline in charge acceptance and energy efficiency,accelerated capacity degradation,and safety risk.In this work,a three-electrode coin cell with a Li metal reference electrode is designed to individually record the potential of two electrodes,and measure the impedance of each electrode by using a power-optimized graphite-LiNi0.80Co0.15Al0.05O2 electrode couple.It is shown that regardless of the state-of-charge the Li-ion cell's impedance is contributed predominantly by the cathode,and that the cathode's impedance is dominated by the charge-transfer resistance.In consistence with the impedance results,polarization of the Li-ion cell is dominated by the cathode.It is surprised to find that no Li plating occurs on the graphite anode even if the charging rate is increased to 10 C(1 C=1.30 mA cm^−2).The results of this work indicate that low overall impedance with a high cathode-to-anode impedance ratio is the key to enabling safe fast-charging,and that fast-charging Li-ion batteries without Li plating on the graphite anode is possible if the cathode and graphite anode are optimistically engineered.展开更多
The development of deeply cyclable lithium metal batteries with fast-charging capability offers a promising solution to relieve the“range anxiety”in driving electric vehicles.Conventional lithium metal anodes suffer...The development of deeply cyclable lithium metal batteries with fast-charging capability offers a promising solution to relieve the“range anxiety”in driving electric vehicles.Conventional lithium metal anodes suffered from low operating current densities and shallow charge/discharge depths,owing to the intrinsic dendrite growth governed by Sand’s law.Herein,we come up with a novel design of heavy-duty lithium metal anode fabricated by partially infusing the three-dimensional(3D)porous graphene aerogel with molten Li.Both electroanalytical measurements and simulations show that the unique electrode architecture brings notable advantages in mediating smooth Li plating/stripping,including reduced local current density,inhibited dendrite growth,buffered volume fluctuation,as well as more efficient Li utilization.Consequently,a remarkable cycling performance in symmetric cells for over 400 cycles(800 h)with an ultrahigh cycling capacity of 15 mAh·cm^(−2) at 15 mA·cm^(−2) is achieved,which,to our best knowledge,has been never seen in literature.LiFePO4 full cells demonstrate a superb rate capability up to 10 C and a prolonged cycling of 1,600 cycles at 2 C with the per-cycle capacity decay of only 0.023%.This study paves the way for the ultimate deployment of lithium metal batteries in real-world applications that require fast charging and deep cycling.展开更多
The sluggish lithium-ion(Li-ion)transport kinetics in graphite anode hinders its application in fast-charging Li-ion batteries(LIBs).Here,we develop an ionpumping interphase(IPI)on graphdiyne(GDY)/graphite heterojunct...The sluggish lithium-ion(Li-ion)transport kinetics in graphite anode hinders its application in fast-charging Li-ion batteries(LIBs).Here,we develop an ionpumping interphase(IPI)on graphdiyne(GDY)/graphite heterojunction anodes to boost the ionic transport kinetics and enable high-performance,fast-charging LIBs.The IPI changed the ion solvation/desolvation environment by covalent/non-covalent interactions with Li ions or solvents to optimize solid-electrolyte interphase(SEI)and regulate Li-ion transport behavior.We studied the in situ growth of few-layer GDY on graphite surface(GDY/graphite)as the IPI and found that the strong interaction between GDY and Li ions enabled surface-induced modification of the ion solvation behavior and surface-assisted desolvation effect to accelerate the Li-ion desolvation process.A functional anion-derived SEI layer with improved Li-ion conductivity was created.Together with the generated built-in electric field at GDY/graphite hetero-interface self-pumping Li ions to intercalate into the graphite,the Li-ion transport kinetics was significantly enhanced to effectively eliminate Li plating and large voltage polarization of the graphite anodes.A fast Li intercalation in GDY/graphite without Li oversaturation at the edge of the graphite was directly observed.The superior performance with high capacity(139.2 mA h g^(-1))and long lifespan(1650 cycles)under extremely fast-charging conditions(20 C,1 C=372 mA g^(-1))was achieved on GDY/graphite anodes.Even at low temperatures(-20℃),a specific capacity of 128.4 mA h g^(-1) was achieved with a capacity retention of 80%after 500 cycles at a 2 C rate.展开更多
SiO-based materials represent a promising class of anodes for lithium-ion batteries(LIBs),with a high theoretical capacity and appropriate and safe Li-insertion potential.However,SiO experiences a large volume change ...SiO-based materials represent a promising class of anodes for lithium-ion batteries(LIBs),with a high theoretical capacity and appropriate and safe Li-insertion potential.However,SiO experiences a large volume change during the electrochemical reaction,low Li diffusivity,and low electron conductivity,resulting in degradation and low rate capability for LIBs.Here,we report on the rapid crafting of SiO–Sn_(2)Fe@C composites via a one-step plasma milling process,leading to an alloy of Sn and Fe and in turn refining SiO and Sn_(2)Fe into nanoparticles that are well dispersed in a nanosized,few-layer graphene matrix.The Sn and Fe nanoparticles generated during the first Li-insertion process form a stable network to improve Li diffusivity and electron conductivity.As an anode mate-rial,the SiO–Sn_(2)Fe@C composite manifests high reversible capacities,superior cycling stability,and excellent rate capability.The capacity retention is found to be as high as 95%and 84%at the 100th and 300th cycles under 0.3 C.During rate capability testing at 3,6,and 11 C,the capacity retentions are 71%,60%,and 50%,respectively.This study highlights that this simple,one-step plasma milling strategy can further improve SiO-based anode materials for high-performance LIBs.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.52202328,52372099,52271222)the Shanghai Sailing Program(22YF1455500)。
文摘Severe lithium dendrite growth and elevated thermal runaway risks pose significant hurdles for fast-charging lithium metal batteries(LMBs)This study reports a polydopamine-functionalized hydroxyapatite/aramid(PDA@HA)hybrid nanofibers separator to synchronously improve th fast-charging LMB's stability and safety.(1)The separator's surface,enriched with lithiophilic carbonyl and hydroxyl groups,accelerates Li~+ion desolvation,while electrophilic imine groups impede anion movement.This dual mechanism optimizes the Li^(+)-ion flux distribution on th anode,mitigating dendrite formation.(2)The polar PDA modification layer fosters the development of a Li_(3)N/LiF-rich solid electrolyt interface,further enhancing Li anode stability.Consequently,Li//Li symmetric cells with PDA@HA separators exhibit extended cycle life in L plating/stripping tests:5000 h at 1 mA cm^(-2)and 700 h at 20 mA cm^(-2),respectively,outperforming PP separators(80 h and 8 h).In LiFePO_(4)(LFP,^(2.1)mg cm^(-2))//Li full cell evaluation,the PDA@HA separator enables stable operation for 11,000 cycles at 18.2C with 87%capacity retention,significantly outperforming existing fast-charging LMB counterparts in literature.At a high LFP loading of 15.5 mg cm^(-2),the cel maintains 137.6 mAh g^(-1)(2.13 mAh cm^(-2))over 250 cycles at 3C,achieving 98%capacity retention.Moreover,the PDA@HA separato increases threshold temperature for thermal runaway and reduces the exothermic rate,intensifying the battery's thermal safety.This research underscores the importance of functional separator design in improving Li metal anode reversibility,fast-charging performance,and therma safety of LMBs.
基金supported by Hengyang City,Hunan Province Science and Technology Innovation Project(No.202250045319)the National Natural Science Foundation of China(Nos.11375084,21808125)the Scientific Research Planning Project of Jilin Provincial Education Department(No.JJKH20241249KJ)。
文摘Weakly solvating electrolyte(WSE)demonstrates superior compatibility with lithium(Li)metal batteries(LMBs).However,its application in fast-charging high-voltage LMBs is challenging.Here,we propose a diluent modified WSE for fast-charging high-voltage LMBs,which is formed by adding diluent of 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether(TTE)into the tetrahydropyran(THP)based WSE.A relatively loose solvation structure is formed due to the formation of weak hydrogen bond between TTE and THP,which accelerates the de-solvation kinetics of Li~+.Besides,more anions are involved in solvation structure in the presence of TTE,yielding inorganic-rich interphases with improved stability.Li(30μm)||Li Ni_(0.5)Co_(0.2)Mn_(0.3)O_(2)(4.1 mAh/cm^(2))batteries with the TTE modified WSE retain over 64%capacity retention after 175 cycles under high rate of 3 C and high-voltage of 4.5 V,much better than that with pure THP based WSE.This work points out that the combination of diluent with weakly solvating solvent is a promising approach to develop high performance electrolytes for fast-charging high-voltage LMBs.
基金supported by the Basic Science Research Program(RS-2024-00344021,RS-2023-00261543,and RS-202300257666)through the National Research Foundation of Korea(NRF),the National Research Council of Science(000)Korea Institute for Advancement of Technology(KIAT)grant funded by the Korea Government(MOTIE)(RS-2024-00420590,HRD Program for Industrial Innovation)The computational resources were provided by KITSI(KSC-2024-CRE-0143)。
文摘Despite the growing interest in fast-cha rging solid-state lithium(Li)-metal batteries(SSLMBs),their practical implementation has yet to be achieved,primarily due to an incomplete understanding of the disparate and often conflicting requirements of the bulk electrolyte and the electrode-electrolyte interphase.Here,we present a weakly coordinating cationic polymer electrolyte(WCPE)specifically designed to regulate the Li^(+)coordination structure,thereby enabling fast-charging SSLMBs.The WCPE comprises an imidazolium-based polycationic matrix combined with a succinonitrile(SN)-based highconcentration electrolyte.Unlike conventional neutral polymer matrices,the polycationic matrix in the WCPE competes with Li^(+)for interactions with SN,weakening the original coordination between SN and Li^(+).This modulation of SN-Li^(+)interaction improves both Li^(+)conductivity of the WCPE(σ_(Li^(+))=1.29mS cm^(-1))and redox kinetics at the electrode-electrolyte interphase.Consequently,SSLMB cells(comprising LiFePO_(4)cathodes and Li-metal anodes)with the WCPE achieve fast-charging capability(reaching over 80%state of charge within 10 min),outperforming those of previously reported polymer electrolytebased SSLMBs.
基金National Natural Science Foundation of China (52372224 and 52072299)Major Project of Shaanxi Coal Joint Fund of Shaanxi Provincial Science and Technology Department (2019JLZ-07)。
文摘Na_(3)V_(2)(PO_(4))_(2)O_(2)F (VP) is recognized as a promising cathode material for sodium-ion batteries due to its stable structural framework and high specific capacity.Density functional theory (DFT) and finite element simulations show that incorporating SO_(4)^(2-)into VP decreases its band gap,lowers the migration energy barrier,and ensures a uniform Na+concentration gradient and stress distribution during charge and discharge cycles.Consequently,the average Na+diffusion coefficient of Na_(3)V_(2)(PO_(4))_(1.95)(SO_(4))_(0.05)O_(2)F(VPS-1) is roughly double that of VP,leading to enhanced rate capability (80 C,75.5 mAh g^(-1)) and cycling stability (111.0 mAh g^(-1)capacity after 1000 cycles at 10 C current density) for VPS-1.VPS-1 exhibits outstanding fast-charging capabilities,achieving an 80%state of charge in just 8.1 min.The assembled VPS-1//SbSn/NPC full cell demonstrated stable cycling over 200 cycles at a high 5 C current,maintaining an average coulombic efficiency of 95.35%.
基金supported by the project of the National Natural Science Foundation of China(NSFC,Nos.5216040127,52164048 and U1802256)Central Guidance for Local Science and Technology Development Funds(No.202107AB110011)the Analysis and Test Funds of Kunming University of Science and Technology(No.2021M0202230188).
文摘As one of the alloy-type lithium-ion electrodes,Bi has outstanding application prospects for large volume capacity(3800 mAh·cm^(-3))and high electronic conductivity(1.4×10^(7)S·m^(-1)).However,the fast-charging performance is hindered by significant volume expansion(>218%)and a low rate of phase diffusion.To overcome these two problems,an N-doped carbon nanoflower coating layer was elaborately in-situ reconstructed on a multiple-wall Bi microsphere by hydrothermal methods and subsequent calcination in this study.The carbon nanoflowers greatly increase specific surface area(40.0 m^(2)·g^(-1))and alleviate the volume expansion(130%).In addition,the incorporation of N-doped carbon nanoflowers leads to a gradual enhancement in the Li adsorption energy of Bi during the process of lithium insertion and improves the electrical conductivity.Therefore,the contribution rate of pseudo-capacitance reached 87.5%at the scan rate of 0.8 mV·s^(-1),and the Li-ion diffusion coefficient(D_(Li^(+)))was calculated in the range of 10^(-10)to 10^(-12)cm^(2)·s^(-1).The Bi@CNFs anode provided a high specific volumetric capacity of 2117.0 mAh·cm^(-3)at 5C and a high capacity retention ratio of 93.2%after 800 cycles.The Bi@CNFs//LiFePO_(4)full cell also displayed a stable capacity of 113.9 mAh·g^(-1)and energy density of 296.1 Wh·kg^(-1)after 100 cycles with a Coulombic efficiency of 97.6%.The mechanism of fast-charging lithium storage was verified by distribution of relaxation time analysis and density functional theory calculation.This paper provides a new strategy to increase the pseudo-capacitance and reduce the volume expansion for the preparation of alloy-type fast-charging electrodes.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.2022R1F1A1074339)。
文摘For the advancement of fast-charging sodium-ion batteries(SIBs),the synthesis of cutting-edge cathode materials with superior structural stability and enhanced Na+diffusion kinetics is imperative.Multiphase layered transition metal oxides(LTMOs),which leverage the synergistic properties of two distinct monophasic LTMOs,have garnered significant attention;however,their efficacy under fast-charging conditions remains underexplored.In this study,we developed a high-throughput computational screening framework to identify optimal dopants that maximize the electrochemical performance of LTMOs.Specifically,we evaluated the efficacy of 32 dopants based on P2/O3-type Mn/Fe-based Na_(x)Mn_(0.5)Fe_(0.5)O_(2)(NMFO)cathode material.Multiphase LTMOs satisfying criteria for thermodynamic and structural stability,minimized phase transitions,and enhanced Na^(+)diffusion were systematically screened for their suitability in fast-charging applications.The analysis identified two dopants,Ti and Zr,which met all predefined screening criteria.Furthermore,we ranked and scored dopants based on their alignment with these criteria,establishing a comprehensive dopant performance database.These findings provide a robust foundation for experimental exploration and offer detailed guidelines for tailoring dopants to optimize fast-charging SIBs.
基金supported by the National Key Research and Development Project(2018YFE0124800)the National Nature Science Foundation of China(51702157,51873086,51673096).
文摘High-energy–density lithium-ion batteries(LIBs)that can be safely fast-charged are desirable for electric vehicles.However,sub-optimal lithiation potential and low capacity of commonly used LIBs anode cause safety issues and low energy density.Here we hypothesize that a cobalt vanadate oxide,Co_(2)VO_(4),can be attractive anode material for fast-charging LIBs due to its high capacity(~1000 mAh g^(−1))and safe lithiation potential(~0.65 V vs.Li^(+)/Li).The Li+diffusion coefficient of Co2VO4 is evaluated by theoretical calculation to be as high as 3.15×10^(-10) cm^(2) s^(−1),proving Co_(2)VO_(4) a promising anode in fast-charging LIBs.A hexagonal porous Co2VO4 nanodisk(PCVO ND)structure is designed accordingly,featuring a high specific surface area of 74.57 m^(2) g^(−1) and numerous pores with a pore size of 14 nm.This unique structure succeeds in enhancing Li^(+) and electron transfer,leading to superior fast-charging performance than current commercial anodes.As a result,the PCVO ND shows a high initial reversible capacity of 911.0 mAh g^(−1) at 0.4 C,excellent fast-charging capacity(344.3 mAh g^(−1) at 10 C for 1000 cycles),outstanding long-term cycling stability(only 0.024% capacity loss per cycle at 10 C for 1000 cycles),confirming the commercial feasibility of PCVO ND in fast-charging LIBs.
基金financially supported by the National Natural Science Foundation of China(No.22279122)Zhejiang Provincial Natural Science Foundation of China(No.LZ22B030004)the Foundation of State Key Laboratory of Coal Conversion(No.J22-23-909)。
文摘Hybrid Na-ion capacitors(NICs)have received considerable interests owing to their low-cost,high-safety,and rapidly charging energy-storage characteristics.The NICs are composed of a capacitor-type cathode and a battery-type anode.The major challenge for NICs is to search for suitable electrode materials to overcome the sluggish diffusion of Na^(+)in the anode.Herein,ultrafine vanadium sulfide is encapsulated in carbon fiber(V_(3)S_(4)@CNF)as a self-supported electrode by electrospinning and in situ sulfurization.The carbon cladding and one-dimensional(ID)nanofiber network-like structure could alleviate the volume expansion of V_(3)S_(4)during Na^(+)de-/intercalation process.Consequently,the V_(3)S_(4)@CNF anode exhibited a pseudocapacitive sodium storage in terms of large Na^(+)-storage capacity(476 mAh·g^(-1)at 0.1A·g^(-1)),high-rate capability(290 mAh·g^(-1)at 20.0 A·g^(-1))and excellent cycling stability(95%capacity retention for1500 cycles at 2.0 A·g^(-1))in Na half-cells.By employing V_(3)S_(4)@CNF as the anode and the activated carbon(AC)cathode,the as-assembled NICs could deliver a high energy density of 110 Wh·kg^(-1)at a power density of200 W·kg^(-1).Even at a high power of 10,000 W·kg^(-1),the specific energy is still up to 42 Wh·kg^(-1).
基金supported by the National Key Research and Development Program(2019YFC0810703)the National Natural Science Foundation of China(22071133)the China Postdoctoral Science Foundation(2020M680581)。
文摘With the ever-growing application of lithium-ion batteries(LIBs), their fast-charging technology has attracted great interests of scientists. However, growth of lithium dendrites during fast charge of the bat teries with high energy density may pose great threats to the operation and cause serious safety issues Herein, we prepared a functional separator with an ultra-thin(20 nm) layer of Au nanoparticles deposited by evaporation coating method which could regulate growth direction and morphology of the lithium dendrites, owing to nearly zero overpotential of lithium meal nucleation on lithiated Au. Once the Li den drites are about to form on the graphite anode during fast charging(or lithiation), they plate predomi nantly on the Au deposited separator rather than on the graphite. Such selective deposition does no compromise the electrochemical performance of batteries under normal cycling. More importantly, i enables the better cycling stability of batteries at fast charge condition. The Li/Graphite cells with Au nanoparticles coated separator could cycle stably with a high areal capacity retention of 90.5% over 95 cycles at the current density of 0.72 m A cm^(-2). The functional separator provides an effective strategy to adjust lithium plating position at fast charge to ensure high safety of batteries without a compromise on the energy density of LIBs.
基金financially supported by Guangdong Basic and Applied Basic Research Foundation (No.2020A1515110762)。
文摘Silicon/carbon composites are promising alternatives to current graphite anodes in commercial lithiumion batteries(LIBs)because of their high capacity and excellent safety.Nevertheless,the unsatisfactory fastcharging capability and cycle stability of Si/C composites caused by slow charge transport capability and huge volume change under industrial electrode conditions severely hamper their development.Here,a novel Si/C anode was fabricated by homogeneously depositing amorphous C-Si nanolayers on graphite(C-Si@graphite).C-Si nanolayers with uniformly dispersed sub-nanometer Si particles in 3D carbon skeleton significantly boost electron and Li-ion transport and efficiently relieve Si's agglomeration and volume change.As a result,the tailored C-Si@graphite electrodes show an excellent rate capacity(760.3 mAh·g^(-1)at 5.0C)and long cycle life of over 1000 cycles at 1.0C and800 cycles at 2.0C under industrial electrode conditions.In addition,the assembled full cells(C-Si@graphite,anode;Li[Ni_(0.8)Co_(0.1)Mn_(0.1)]O_(2),cathode)present superior fastcharging capability(240.4 Wh·kg^(-1),charging for16.2 min,3.0C)and long cycle life(80.7%capacity retention after 500 cycles at 1.0C),demonstrating the massive potential of C-Si@graphite for practical application.
基金supported by the National Natural Science Foundation of China (No.92372123)the Natural Science Foundation of Guangdong Province (No.2022B1515020005)the Department of Science and Technology of Guangdong Province (No.2020B0101030005)
文摘Fast-charging and low temperature operation are of vital importance for the further development of lithium-ion batteries(LIBs),which is hindered by the utilization of conventional carbonate-based electrolytes due to their slow kinetics,narrow operating temperature and voltage range.Herein,an acetonitrile(AN)-based localized high-concentration electrolyte(LHCE)is proposed to retain liquid state and high ionic conductivity at ultra-low temperatures while possessing high oxidation stability.We originally reveal the excellent thermal shielding effect of non-solvating diluent to prevent the aggregation of Li^(+) solvates as temperature drops,maintaining the merits of fast Li transport and facile desolvation as at room temperature,which bestows the graphite electrode with remarkable low temperature performance(264 mA h g^(-1) at-20 C).Remarkably,an extremely high capacity retention of 97%is achieved for high-voltage high-energy graphite||NCM batteries after 250 cycles at-20 C,and a high capacity of 110 mA h g^(-1)(71%of its room-temperature capacity)is retained at-30°C.The study unveils the key role of the non-solvating diluents and provides instructive guidance in designing electrolytes towards fast-charging and low temperature LIBs.
基金supported by the National Natural Science Foundation of China(Nos.22075048,52201201)Shaanxi Yanchang Petroleum Co.,Ltd.(No.18529),Yiwu Research Institute of Fudan University(No.20-1-06)+2 种基金the Shanghai International Collaboration Research Project(No.19520713900)the State Key Laboratory of Molecular Engineering of Polymers(Fudan University,No.K2024-36)the State Key Lab of Advanced Metals and Materials(No.2022Z-11)。
文摘Dendrite growth of zinc(Zn)anode at high current density severely affects the fast-charging performance of aqueous zinc metal batteries(AZMBs).While interfacial modification strategies can optimize Zn per formance,challenges such as complicated preparation processes,excessive layer thicknesses,and high voltage hysteresis should be addressed.Herein,we utilize a cost-effective liquid fluorosiloxane,(3,3,3trifluoropropyl)trimethoxysilane,for scalable modification of Zn foil via drop-casting at room tempera ture,resulting in an ultra-thin interphase layer of only 20 nm.The Si-O-Zn bonds formed between flu orosiloxane and Zn ensure interfacial stability,and the Si-O-Si bonds between fluorosiloxane molecule help to homogenize the electric field distribution.Additionally,the abundant highly electronegative flu orine atoms on the anode surface act as zincophilic sites,promoting the uniform deposition of Zn^(2+)Thus,the modified Zn foil(SiFO-Zn)exhibits excellent dendrite suppression,reduced voltage hysteresis and prolonged cycle life at ultra-high current density(40 mA/cm^(2)),achieving a cumulative areal capac ity of 12.9 Ah/cm^(2).Further,the full cell assembled with 10μm-thick Si FO-Zn anode and MnO_(2)cathode achieves 2600 cycles at 5 A/g with minimal capacity degradation,and a large-size(22.5 cm^(-2))pouch cel powers the light-emitting diode even after reverse bending,demonstrating the potential of AZMBs fo fast-charging flexible devices.
基金supported by the National Key Research and Development Program of China(2022YFA1504100)the National Natural Science Foundation of China(22125903,51872283,and 22005298)+4 种基金Dalian Innovation Support Plan for High Level Talents(2019RT09)Dalian National Laboratory For Clean Energy(DNL),Chinese Academy of Sciences(CAS),DNL Cooperation Fund,CAS(DNL202016 and DNL202019)Dalian Institute of Chemical Physics(DICP I2020032)Exploratory Research Project of Yanchang Petroleum International Limited and DICP(yc-hw-2022ky-01)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL Fund 2021002 and 2021009).
文摘Lithium-ion batteries(LIBs)with the“double-high”characteristics of high energy density and high power density are in urgent demand for facilitating the development of advanced portable electronics.However,the lithium ion(Li+)-storage performance of the most commercialized lithium cobalt oxide(LiCoO_(2),LCO)cathodes is still far from satisfactory in terms of high-voltage and fast-charging capabilities for reaching the double-high target.Herein,we systematically summarize and discuss high-voltage and fast-charging LCO cathodes,covering in depth the key fundamental challenges,latest advancements in modification strategies,and future perspectives in this field.Comprehensive and elaborated discussions are first presented on key fundamental challenges related to structural degradation,interfacial instability,the inhomogeneity reactions,and sluggish interfacial kinetics.We provide an instructive summary of deep insights into promising modification strategies and underlying mechanisms,categorized into element doping(Li-site,cobalt-/oxygen-site,and multi-site doping)for improved Li+diffusivity and bulkstructure stability;surface coating(dielectrics,ionic/electronic conductors,and their combination)for surface stability and conductivity;nanosizing;combinations of these strategies;and other strategies(i.e.,optimization of the electrolyte,binder,tortuosity of electrodes,charging protocols,and prelithiation methods).Finally,forward-looking perspectives and promising directions are sketched out and insightfully elucidated,providing constructive suggestions and instructions for designing and realizing high-voltage and fast-charging LCO cathodes for next-generation double-high LIBs.
基金support of the National Key R&D Program of China(2022YFB3803500)Zhejiang Rouzhen Technology Corp.,Ltd.,and OPPO Mobile Telecommunications Corp.,Ltd.
文摘Adopting the metalized plastic current collector(MPCC)enhances the safety and specific energy density of lithium-ion batteries(LIBs)but sacrifices the rate capability.The reduced rate capability is customarily ascribed to the lower electronic conductivity of MPCC as compared with the metal ones(e.g.,Al and Cu)due to the less metal usage.Here,we demonstrate that the interfacial contact between the current collector(CC)and the active-material layer,rather than the electronic conductivity of CC,accounts for the rate performance of the cells.By introducing a thin carbon coating(~300 nm)onto the surface of MPCC(e.g.,1μm thick aluminum deposited on both sides of 10μm polyethylene terephthalate(PET)film,Al-PET),we reduced the contact resistance between MPCC and cathode materials.Using the carbon-coated Al-PET(C@Al-PET)as CC,the 6.0-Ah graphite/LiCoO_(2)pouch cell delivers significantly improved fast-charge capability and cycling stability,which are identified as the homogenized potential distribution and electrode utilization with multiphysical field simulations.Most importantly,the cell with C@Al-PET CC could still pass the harsh impact test,promising its applications in high-rate LIBs with superior safety.
基金supported by the National Natural Science Foundation of China(U22A20118)Natural Science Foundation of Fujian Province(2023J01400)Award Program for Fujian Minjiang Scholar Professorship。
文摘Lithium(Li)metal anodes(LMAs)have garnered significant attention due to their exceptionally high theoretical capacity and low redox potentials.However,the uncontrolled growth of Li dendrites and substantial volume expansion severely undermine their cycling stability,particularly at elevated current densities.Herein,we develop a lithiophilic 3D Li host by incorporating ZnO/ZnSe heterostructures onto brass fibers(ZnO/ZnSe@Brass),designed to enhance the fast-charging capabilities of Li metal batteries.This hierarchical structure effectively mitigates volume expansion and reduces local current density during lithiation.The uniformly distributed ZnO/ZnSe functions as a lithiophilic skin for the Li anode,facilitating smooth and dense Li deposition.Notably,the in situ formed solid electrolyte interphase,enriched with Li_(2)Se and Li_(2)O,provides high ionic conductivity and superior mechanical strength,thereby accelerating ion transport and charge transfer kinetics.Benefiting from the synergistic effects of the ZnO/ZnSe@Brass host,the resulting Li symmetric cell exhibits robust cycling performance exceeding 10,000 cycles(20 mA cm^(−2)/1 mA h cm^(−2))and supports fast charging rates at an ultra-high current density of 80 mA cm^(−2).When paired with LiFePO4,the full-cell demonstrates excellent cycle life(>500 cycles at 2 C)and outstanding rate performance.This finding of ZnO/ZnSe@Brass as a Li host sheds light on the design of advanced LMAs for fast-charging Li metal batteries.
基金the National Science Foundation of China(NSFC)(Nos.51903041,21991123,and 51873035)Natural Science Foundation of Shanghai(No.19ZR1470700)“Qimingxing Plan”(No.19QA1400200).
文摘The safe,flexible,and environment-friendly Zn-ion batteries have aroused great interests nowadays.Nevertheless,flagrant Zn dendrite uncontrollably grows in liquid electrolytes due to insufficient surface protection,which severely impedes the future applications of Zn-ion batteries especially at high current densities.Gel electrolytes are emerging to tackle this issue,yet the required high modulus for inhibiting dendrite growth as well as concurrent poor interfacial contact with roughened Zn electrodes are not easily reconcilable to regulate the fragile Zn/Zn^(2+) interface.Here we demonstrate,such a conflict may be defeated by using a mechanoadaptive cellulose nanofibril-based morphing gel electrolyte(MorphGE),which synergizes bulk compliance for optimizing interfacial contact as well as high modulus for suppressing dendrite formation.Moreover,by anchoring desolvated Zn^(2+) on cellulose nanofibrils,the side reactions which induce dendrite formation are also significantly reduced.As a result,the MorphGE-based symmetrical Zn-ion battery demonstrated outstanding stability for more than 100 h at the high current density of 10 mA·cm^(−2) and areal capacity of 10 mA·h·cm^(−2),and the corresponding Zn-ion battery delivered a prominent specific capacity of 100 mA·h·g^(−1) for more than 500 cycles at 20 C.The present example of engineering the mechanoadaptivity of gel electrolytes will shed light on a new pathway for designing highly safe and flexible energy storage devices.
基金Funding information Army Research Laboratory,Grant/Award Number:N/A
文摘Fast-charging is highly demanded for applications requiring short charging time.However,fast-charging triggers serious problems,leading to decline in charge acceptance and energy efficiency,accelerated capacity degradation,and safety risk.In this work,a three-electrode coin cell with a Li metal reference electrode is designed to individually record the potential of two electrodes,and measure the impedance of each electrode by using a power-optimized graphite-LiNi0.80Co0.15Al0.05O2 electrode couple.It is shown that regardless of the state-of-charge the Li-ion cell's impedance is contributed predominantly by the cathode,and that the cathode's impedance is dominated by the charge-transfer resistance.In consistence with the impedance results,polarization of the Li-ion cell is dominated by the cathode.It is surprised to find that no Li plating occurs on the graphite anode even if the charging rate is increased to 10 C(1 C=1.30 mA cm^−2).The results of this work indicate that low overall impedance with a high cathode-to-anode impedance ratio is the key to enabling safe fast-charging,and that fast-charging Li-ion batteries without Li plating on the graphite anode is possible if the cathode and graphite anode are optimistically engineered.
基金financially supported by the National Natural Science Foundation of China(Nos.22075193 and 22072101)the Natural Science Foundation of Jiangsu Province(No.BK20211306)+2 种基金the Key Technology Initiative of Suzhou Municipal Science and Technology Bureau(No.SYG201934)Six Talent Peaks Project in Jiangsu Province(No.TD-XCL-006)the support from the Honorary Professor Program of Jiangsu Province and Priority Academic Program Development(PAPD)of Jiangsu Higher Education Institutions.
文摘The development of deeply cyclable lithium metal batteries with fast-charging capability offers a promising solution to relieve the“range anxiety”in driving electric vehicles.Conventional lithium metal anodes suffered from low operating current densities and shallow charge/discharge depths,owing to the intrinsic dendrite growth governed by Sand’s law.Herein,we come up with a novel design of heavy-duty lithium metal anode fabricated by partially infusing the three-dimensional(3D)porous graphene aerogel with molten Li.Both electroanalytical measurements and simulations show that the unique electrode architecture brings notable advantages in mediating smooth Li plating/stripping,including reduced local current density,inhibited dendrite growth,buffered volume fluctuation,as well as more efficient Li utilization.Consequently,a remarkable cycling performance in symmetric cells for over 400 cycles(800 h)with an ultrahigh cycling capacity of 15 mAh·cm^(−2) at 15 mA·cm^(−2) is achieved,which,to our best knowledge,has been never seen in literature.LiFePO4 full cells demonstrate a superb rate capability up to 10 C and a prolonged cycling of 1,600 cycles at 2 C with the per-cycle capacity decay of only 0.023%.This study paves the way for the ultimate deployment of lithium metal batteries in real-world applications that require fast charging and deep cycling.
基金the National Nature Science Foundation of China(grant nos.52072222 and 22279073)the National Key Research and Development Project of China(grant no.2022YFA1200044)+2 种基金the Taishan Scholar Project of Shandong Province of China(grant no.62460082061017)the Natural Science Foundation of Shandong Province(grant no.ZR2022ZD35)the National Nature Science Foundation of China(grant nos.21790050 and 21790051).
文摘The sluggish lithium-ion(Li-ion)transport kinetics in graphite anode hinders its application in fast-charging Li-ion batteries(LIBs).Here,we develop an ionpumping interphase(IPI)on graphdiyne(GDY)/graphite heterojunction anodes to boost the ionic transport kinetics and enable high-performance,fast-charging LIBs.The IPI changed the ion solvation/desolvation environment by covalent/non-covalent interactions with Li ions or solvents to optimize solid-electrolyte interphase(SEI)and regulate Li-ion transport behavior.We studied the in situ growth of few-layer GDY on graphite surface(GDY/graphite)as the IPI and found that the strong interaction between GDY and Li ions enabled surface-induced modification of the ion solvation behavior and surface-assisted desolvation effect to accelerate the Li-ion desolvation process.A functional anion-derived SEI layer with improved Li-ion conductivity was created.Together with the generated built-in electric field at GDY/graphite hetero-interface self-pumping Li ions to intercalate into the graphite,the Li-ion transport kinetics was significantly enhanced to effectively eliminate Li plating and large voltage polarization of the graphite anodes.A fast Li intercalation in GDY/graphite without Li oversaturation at the edge of the graphite was directly observed.The superior performance with high capacity(139.2 mA h g^(-1))and long lifespan(1650 cycles)under extremely fast-charging conditions(20 C,1 C=372 mA g^(-1))was achieved on GDY/graphite anodes.Even at low temperatures(-20℃),a specific capacity of 128.4 mA h g^(-1) was achieved with a capacity retention of 80%after 500 cycles at a 2 C rate.
基金This work was supported by the National Natural Science Foundation of China(grant numbers 52001124,52071144,51831009,and 51621001).
文摘SiO-based materials represent a promising class of anodes for lithium-ion batteries(LIBs),with a high theoretical capacity and appropriate and safe Li-insertion potential.However,SiO experiences a large volume change during the electrochemical reaction,low Li diffusivity,and low electron conductivity,resulting in degradation and low rate capability for LIBs.Here,we report on the rapid crafting of SiO–Sn_(2)Fe@C composites via a one-step plasma milling process,leading to an alloy of Sn and Fe and in turn refining SiO and Sn_(2)Fe into nanoparticles that are well dispersed in a nanosized,few-layer graphene matrix.The Sn and Fe nanoparticles generated during the first Li-insertion process form a stable network to improve Li diffusivity and electron conductivity.As an anode mate-rial,the SiO–Sn_(2)Fe@C composite manifests high reversible capacities,superior cycling stability,and excellent rate capability.The capacity retention is found to be as high as 95%and 84%at the 100th and 300th cycles under 0.3 C.During rate capability testing at 3,6,and 11 C,the capacity retentions are 71%,60%,and 50%,respectively.This study highlights that this simple,one-step plasma milling strategy can further improve SiO-based anode materials for high-performance LIBs.
