Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and l...Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and long-range electric vehicles.However,technical barriers such as dendrite growth and poor Li plating/stripping reversibility severely hinder the practical application of LMBs.However,lithium nitrate(LiNO_(3))is found to be able to stabilize the Li/electrolyte interface and has been used to address the above challenges.To date,considerable research efforts have been devoted toward understanding the roles of LiNO_(3) in regulating the surface properties of Li anodes and toward the development of many effective strategies.These research efforts are partially mentioned in some articles on LMBs and yet have not been reviewed systematically.To fill this gap,we discuss the recent advances in fundamental and technological research on LiNO_(3) and its derivatives for improving the performances of LMBs,particularly for Li-sulfur(S),Li-oxygen(O),and Li-Li-containing transition-metal oxide(LTMO)batteries,as well as LiNO_(3)-containing recipes for precursors in battery materials and interphase fabrication.This review pays attention to the effects of LiNO_(3) in lithium-based batteries,aiming to provide scientific guidance for the optimization of electrode/electrolyte interfaces and enrich the design of advanced LMBs.展开更多
Solid-state lithium(Li)batteries are hailed as the nextgeneration energy storage technology,garnering significant attention for their potential high energy density and safety.Particularly when using Li-rich manganese ...Solid-state lithium(Li)batteries are hailed as the nextgeneration energy storage technology,garnering significant attention for their potential high energy density and safety.Particularly when using Li-rich manganese layered oxide(LRMO)as cathodes(theoretical capacity exceeding250 mAh/g),energy densities over 600 Wh/kg can be theoretically achieved[1,2].展开更多
Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving...Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving the overall performance of CPEs due to their difficulty in achieving robust electrochemical and mechanical interfaces simultaneously.Here,by regulating the surface charge characteristics of halloysite nanotube(HNT),we propose a concept of lithium-ion dynamic interface(Li^(+)-DI)engineering in nano-charged CPE(NCCPE).Results show that the surface charge characteristics of HNTs fundamentally change the Li^(+)-DI,and thereof the mechanical and ion-conduction behaviors of the NCCPEs.Particularly,the HNTs with positively charged surface(HNTs+)lead to a higher Li^(+)transference number(0.86)than that of HNTs-(0.73),but a lower toughness(102.13 MJ m^(-3)for HNTs+and 159.69 MJ m^(-3)for HNTs-).Meanwhile,a strong interface compatibilization effect by Li^(+)is observed for especially the HNTs+-involved Li^(+)-DI,which improves the toughness by 2000%compared with the control.Moreover,HNTs+are more effective to weaken the Li^(+)-solvation strength and facilitate the formation of Li F-rich solid-electrolyte interphase of Li metal compared to HNTs-.The resultant Li|NCCPE|LiFePO4cell delivers a capacity of 144.9 m Ah g^(-1)after 400 cycles at 0.5 C and a capacity retention of 78.6%.This study provides deep insights into understanding the roles of surface charges of nanofillers in regulating the mechanical and electrochemical interfaces in ASSLMBs.展开更多
Driven by the increasing demand for high-energy-density batteries in electric vehicles and portable electronics,lithium metal batteries have made significant breakthroughs[1–3].While critical challenges associated wi...Driven by the increasing demand for high-energy-density batteries in electric vehicles and portable electronics,lithium metal batteries have made significant breakthroughs[1–3].While critical challenges associated with lithium metal anodes in liquid electrolytes(e.g.,dendrite growth,interface instability)have hindered commercialization[4–6],solid electrolyte systems have shown promise in mitigating these issues.Among these,solid polymer electrolytes(SPEs)have emerged as a viable solution for enabling stable quasisolid-state lithium metal batteries[7–9].展开更多
In order to explore the reduction pathways of zinc oxide in LiCl molten salt and the optimal process,experiments were conducted in an alumina crucible using metallic lithium as the reducing agent and lithium chloride ...In order to explore the reduction pathways of zinc oxide in LiCl molten salt and the optimal process,experiments were conducted in an alumina crucible using metallic lithium as the reducing agent and lithium chloride molten salt as the reaction medium at 923 K.The study assessed the effects of lithium thermochemical reduction and electrolytic reduction of ZnO.The volatilization behavior of metal oxides in molten salts,the equivalent of a reducing agent,reduction time,amount of molten salt,stirring time,and the method of reduction feed were investigated for their impacts on the reduction yield and product composition.X-ray powder diffraction(XRD)analysis of the products showed that lithium reduction of ZnO not only produced metallic Zn but also formed a LiZn alloy.Electrolytic reduction can be used to obtain the metallic Zn product by controlling the potential below-2.2 V(vs Ag/Ag^(+)).Moreover,sintered oxides and higher electrode potentials could enhance the efficiency of electrolysis.Under the optimal reaction conditions determined experimentally,the lithium reduction experiment achieved a yield of 77.2%after a 12-h test,and the electrolytic reduction reached a yield of 85.4%after a 6-h test.展开更多
Herein,3‑aminopropyltriethoxysilane(APTES)was used to modify F‑containing silica slag(SS)by simple grafting and served as a multifunctional barrier layer.The amino group(—NH2)in the amino‑modified SS(NH2‑SS)forms lig...Herein,3‑aminopropyltriethoxysilane(APTES)was used to modify F‑containing silica slag(SS)by simple grafting and served as a multifunctional barrier layer.The amino group(—NH2)in the amino‑modified SS(NH2‑SS)forms ligand bonds or hydrogen bonds with sulfur ions in lithium polysulfides(LiPSs),thus inhibiting the shuttle effect.Electrochemical analyses demonstrated that lithium‑sulfur(Li‑S)batteries employing the NH2‑SS interlayer exhibited discharge specific capacities of 1048 and 789 mAh·g^(-1) at 0.2C and 2C,respectively,and even at 4C,the initial discharge specific capacity remained at 590 mAh·g^(-1),outperforming the Li‑S battery with unmodified SS as the interlayer.展开更多
The sulfation and decomposition process has proven effective in selectively extracting lithium from lepidolite.It is essential to clarify the thermochemical behavior and kinetic parameters of decomposition reactions.A...The sulfation and decomposition process has proven effective in selectively extracting lithium from lepidolite.It is essential to clarify the thermochemical behavior and kinetic parameters of decomposition reactions.Accordingly,comprehensive kinetic study by employing thermalgravimetric analysis at various heating rates was presented in this paper.Two main weight loss regions were observed during heating.The initial region corresponded to the dehydration of crystal water,whereas the subsequent region with overlapping peaks involved complex decomposition reactions.The overlapping peaks were separated into two individual reaction peaks and the activation energy of each peak was calculated using isoconversional kinetics methods.The activation energy of peak 1 exhibited a continual increase as the reaction conversion progressed,while that of peak 2 steadily decreased.The optimal kinetic models,identified as belonging to the random nucleation and subsequent growth category,provided valuable insights into the mechanism of the decomposition reactions.Furthermore,the adjustment factor was introduced to reconstruct the kinetic mechanism models,and the reconstructed models described the kinetic mechanism model more accurately for the decomposition reactions.This study enhanced the understanding of the thermochemical behavior and kinetic parameters of the lepidolite sulfation product decomposition reactions,further providing theoretical basis for promoting the selective extraction of lithium.展开更多
Lithium-sulfur(Li-S)batteries require efficient catalysts to accelerate polysulfide conversion and mitigate the shuttle effect.However,the rational design of catalysts remains challenging due to the lack of a systemat...Lithium-sulfur(Li-S)batteries require efficient catalysts to accelerate polysulfide conversion and mitigate the shuttle effect.However,the rational design of catalysts remains challenging due to the lack of a systematic strategy that rationally optimizes electronic structures and mesoscale transport properties.In this work,we propose an autogenously transformed CoWO_(4)/WO_(2) heterojunction catalyst,integrating a strong polysulfide-adsorbing intercalation catalyst with a metallic-phase promoter for enhanced activity.CoWO_(4) effectively captures polysulfides,while the CoWO_(4)/WO_(2) interface facilitates their S-S bond activation on heterogenous catalytic sites.Benefiting from its directional intercalation channels,CoWO_(4) not only serves as a dynamic Li-ion reservoir but also provides continuous and direct pathways for rapid Li-ion transport.Such synergistic interactions across the heterojunction interfaces enhance the catalytic activity of the composite.As a result,the CoWO_(4)/WO_(2) heterostructure demonstrates significantly enhanced catalytic performance,delivering a high capacity of 1262 mAh g^(−1) at 0.1 C.Furthermore,its rate capability and high sulfur loading performance are markedly improved,surpassing the limitations of its single-component counterparts.This study provides new insights into the catalytic mechanisms governing Li-S chemistry and offers a promising strategy for the rational design of high-performance Li-S battery catalysts.展开更多
Polyethylene oxide(PEO)-based solid polymer electrolytes(SPEs)have long faced limitations due to low ionic conductivity at ambient temperature and poor interfacial stability with lithium metal anodes.Here,we present a...Polyethylene oxide(PEO)-based solid polymer electrolytes(SPEs)have long faced limitations due to low ionic conductivity at ambient temperature and poor interfacial stability with lithium metal anodes.Here,we present a structural engineering strategy to address these challenges through shear-induced crystallization of concentrated PEO-LiTFSI solutions,which self-assemble into flower-like spherulites with radially aligned lamellar crystals.This unique structure creates continuous Li^(+)transport highways through densely packed crystalline domains,achieving a record-high ionic conductivity of 1.70×10^(-4) S/cm at 25℃ for pristine PEO-based systems.Strategic incorporation of lithium montmorillonite(MMTli,10 wt%)further optimizes the composite electrolyte,balancing high ionic conductivity(1.47×10^(-4) S/cm)with enhanced electrochemical stability(4.99 V vs.Li^(+)/Li),elevated Li^(+)transference number(0.62),and mechanical robustness.The composite electrolyte enables stable Li plating/stripping over 800 h in symmetric Li||Li cells and powers LiFePO_(4)||Li solid-state batteries with 82%capacity retention after 200 cycles at 0.2 C under ambient conditions.This work pioneers a scalable processing paradigm for crystalline polymer electrolytes,offering new insights into ion transport mechanisms and validating clay minerals as multifunctional additives for next-generation energy storage systems.展开更多
In-situ poly(1,3-dioxolane)(PDOL)-based electrolyte has received extensive attention in the research of lithium metal batteries due to its high stability to lithium anode and simple processing.However,it is still face...In-situ poly(1,3-dioxolane)(PDOL)-based electrolyte has received extensive attention in the research of lithium metal batteries due to its high stability to lithium anode and simple processing.However,it is still faced with defects such as low intrinsic ionic conductivity,a narrow electrochemical window,and poor thermal stability.A crosslinking and fluorination molecular design strategy toward PDOL is proposed to tackle the issues above.The amorphous crosslinked structure effectively improves ionic conductivity by inhibiting long-chain crystallization.Especially,the antioxidant–CF_(3)groups,stable crosslinked structure,and reduced terminal hydroxyl groups significantly enhance the electrochemical oxidation stability with a superb high-voltage window of 4.7 V.In addition,the designed electrolyte also exhibits obviously improved thermal stability with no deformation at 120°C for 5 min.Furthermore,the semi-solid NCM811||Li batteries exhibit a favourable capacity retention of 88.8%after 150 cycles at 0.5 C.Even assembled with NCM622 cathode working at 4.5 V,the semi-solid batteries can still show a satisfactory capacity retention of 85.3%after 100 cycles at 0.5 C.Also,a 0.1 Ah NCM811||Li pouch cell with active materials loading of 9 mg/cm2 demonstrates satisfactory cycling stability and working ability,which shows promising practical application prospects.展开更多
To ease the scarcity of lithium(Li)resource and cut down on environmental pollution,an efficient,selective,inexpensive and sustainable Li recycling process from waste batteries is needed,which is yet to be achieved.He...To ease the scarcity of lithium(Li)resource and cut down on environmental pollution,an efficient,selective,inexpensive and sustainable Li recycling process from waste batteries is needed,which is yet to be achieved.Here,we report a low-potential photoelectrochemical(PEC)system that selectively and efficiently extracts Li metals from multi-cation electrolytes under 1 sun illumination.Based on the difference of redox potential,we can get rid of the disturbance of other cations(i.e.,Fe,Co and Ni ions)by a bias-free PEC device to realize the extraction of high-purity Li metals on a coplanar Si-based photocathode-TiO_(2) photoanode tandem device at 2 V of applied bias(far less than the redox potentials of Li^(+)/Li).In such system,the extraction rate of Li metals(purity>99.5%)exceeds 1.35 g h^(-1)m^(-2)with 90%of Faradaic efficiency.Long-term experiments,different electrode/electrolyte tests,and various price assessments further demonstrate the stability,compatibility and economy of PEC extraction system,enabling a solar-driven pathway for the recycling of critical metal resources.展开更多
High-nickel cathode,LiNi0.8Co0.1Mn0.1O_(2)(NCM811),and sulfide-solid electrolyte are a promising combination for all-solid-state lithium batteries(ASSLBs).However,this combination faces the issue of interfacial instab...High-nickel cathode,LiNi0.8Co0.1Mn0.1O_(2)(NCM811),and sulfide-solid electrolyte are a promising combination for all-solid-state lithium batteries(ASSLBs).However,this combination faces the issue of interfacial instability between the cathode and electrolyte.Given the surface alkalinity of NCM811,we propose a strategy to construct a solid-polymer-electrolyte(SPE)interphase on NCM811 surface by leveraging the surface alkaline residues to nucleophilically initiate the in-situ ring-opening polymerization of cyclic organic molecules.As a proof-of-concept,this study demonstrates that the ring-opening copolymerization of 1,3-dioxolane and maleic anhydride produces a homogeneous,compact,and conformal SPE layer on NCM811 surface to prevent the cathode from contact and reaction with Li6PS5Cl solid-state electrolyte.Consequently,the SPE-modified-NCM811 in ASSLBs exhibits high capacities of 193.5 mA h g^(-1) at 0.2 C,160.9 mA h g^(-1) at 2.0 C and 112.3 mA h g^(-1) at 10 C,and particularly,excellent long-term cycling stabilities over 11000 cycles with a 71.95%capacity retention at 10 C at 25℃,as well as a remained capacity of 117.9 mA h g^(-1) after 8000 cycles at 30 C at 60℃,showing a great application prospect.This study provides a new route for creating electrochemically and structurally stable solid-solid interfaces for ASSLBs.展开更多
The practical application of lithium metal batteries(LMBs)requires electrolytes that simultaneously ensure high safety and interfacial stability.Although locally concentrated ionic liquid electrolytes(LCILEs)exhibit e...The practical application of lithium metal batteries(LMBs)requires electrolytes that simultaneously ensure high safety and interfacial stability.Although locally concentrated ionic liquid electrolytes(LCILEs)exhibit exceptional electrochemical stability and compatibility with electrode electrolyte interfaces(EEIs),two major challenges persist:(i)safety risks caused by excessive low-flash-point diluents,and(ii)insufficient understanding of how diluents modulate solvation structures.Herein,we introduce a low-diluent-content LCILE system composed of lithium bis(fluorosulfonyl)imide(LiFSI)salt,N-methyl-N-propyl-pyrrolidinium bis(fluorosulfonyl)imide(Pyr_(13)FSI)ionic liquid,and trifluoromethanesulfonate(TFS)diluent.The TFS diluent strengthens ion-ion interactions by lowering the dielectric constant of the electrolyte,resulting in the formation of a unique nanometric anion aggregates(N-AGGs)reinforced solvation structure.These large anionic clusters exhibit accelerated redox decomposition kinetics,facilitating the rapid formation of a thin,dense,and low-impedance EEI.Consequently,the Li/LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)coin cell achieves 87.8%capacity retention over 300 cycles at 4.3 V,while a practical 1.4 Ah Li/NCM622 pouch cell retains 84.5%capacity after 80 cycles at 4.5 V.Furthermore,the electrolyte demonstrates exceptional safety,and 2 Ah Li metal pouch cells successfully pass rigorous nail penetration tests without any ignition or explosion.This work not only provides a design strategy for intrinsically safe and high-performance electrolytes but also highlights the critical role of anion cluster decomposition kinetics in shaping EEI formation.展开更多
Structural instability and sluggish lithium-ion(Li+) kinetics of spinel NiCo_(2)O_(4) anodes severely hinder their applications in high-energy-density lithium-ion batteries.Mesocrystalline structures exhibit promising...Structural instability and sluggish lithium-ion(Li+) kinetics of spinel NiCo_(2)O_(4) anodes severely hinder their applications in high-energy-density lithium-ion batteries.Mesocrystalline structures exhibit promising potential in balancing structural stability and enhancing reaction kinetics.However,their controlled synthesis mechanisms remain elusive.Herein,a substrate interface engineering strategy is developed to achieve controllable synthesis of mesocrystalline and polycrystalline NiCo_(2)O_(4) nanorods.Remarkably,mesocrystalline NiCo_(2)O_(4) exhibits a high capacity retention rate of 85.7% after 500 cycles at 2 A/g,attributed to its porous structure facilitating Li^(+) transport kinetics and unique stress-buffering effect validated by ex-situ TEM.Theoretical calculations and interfacial chemical analysis reveal that substratecrystal surface engineering regulates the nucleation-growth pathways:Acid-treated nickel foam enables epitaxial growth via lattice matching,acting as a low-interfacial-energy template to reduce nucleation barriers and promote low-temperature oriented crystallization.In contrast,carbon cloth requires hightemperature thermal activation to overcome surface diffusion barriers induced by elevated interfacial energy.This substrate-driven crystallization kinetic modulation overcomes the limitations of random nucleation in conventional hydrothermal synthesis.The established substrate-crystal interfacial interaction model not only clarifies the kinetic essence of crystal orientation regulation but also provides a universal theoretical framework for lattice-matching design and mesostructural optimization of advanced electrode materials.展开更多
Crystallized lithium fluoride(LiF)melts at 848℃ upon heating,and evaporates subsequently at a remarkably high temperature of 1673℃,characterizing its excellent thermally stability as one of the most representative m...Crystallized lithium fluoride(LiF)melts at 848℃ upon heating,and evaporates subsequently at a remarkably high temperature of 1673℃,characterizing its excellent thermally stability as one of the most representative metal halides.The marriage between Li F and rechargeable batteries dates back to early activities related to the electrochemical properties of lithium metal(Li°)negative electrodes,in which the nonaqueous electrolytes containing fluorinated salts were generally employed,e.g.,lithium tetrafluoroborate(LiBF_(4)),lithium hexafluoroarsenate(LiAsF_(6)),lithium trifluoromethanesulfonate(CF_(3)SO_(3)Li)[1].展开更多
Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and of...Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.展开更多
Photonic neural networks(PNNs)of sufficiently large physical dimensions and high operation accuracies are envisaged as ideal candidates for breaking the major bottlenecks in the current artificial intelligence archite...Photonic neural networks(PNNs)of sufficiently large physical dimensions and high operation accuracies are envisaged as ideal candidates for breaking the major bottlenecks in the current artificial intelligence architectures in terms of latency,energy efficiency,and computational power.To achieve this vision,it is of vital importance to scale up the PNNs while simultaneously reducing the high demand on the dimensions required by them.The underlying cause of this strategy is the enormous gap between the scales of photonic and electronic integrated circuits.Here,we demonstrate monolithically integrated optical convolutional processors on thin film lithium niobate(TFLN)that harness inherent parallelism in photonics to enable large-scale programmable convolution kernels and,in turn,greatly reduce the dimensions required by subsequent fully connected layers.Experimental validation achieves high classification accuracies of 96%(86%)on the MNIST(Fashion-MNIST)dataset and 84.6%on the AG News dataset while dramatically reducing the required subsequent fully connected layer dimensions to 196×10(from 784×10)and 175×4(from 800×4),respectively.Furthermore,our devices can be driven by commercial field-programmable gate array systems;a unique advantage in addition to their scalable channel number and kernel size.Our architecture provides a solution to build practical machine learning photonic devices.展开更多
Anode-free lithium-metal batteries(AFLMBs)offer high energy density.However,lithium dendrite growth and interfacial instability remain critical obstacles to their commercialization.Here,lithiophilic nanosized(∼5 nm)L...Anode-free lithium-metal batteries(AFLMBs)offer high energy density.However,lithium dendrite growth and interfacial instability remain critical obstacles to their commercialization.Here,lithiophilic nanosized(∼5 nm)LixSn combined with an inorganic-rich@polymer dual-layer structure was constructed on a Cu current collector,prepared via a galvanostatic process using a dual-lithium salt electrolyte in a Cu||Cu configuration.The polymer outer layer,initiated by LixSn,reinforces the solid electrolyte interphase(SEI),providing mechanical robustness and enabling stable cycling in an ether-based electrolyte.Furthermore,the Sn and LixSn particle sizes can be effectively tuned by adjusting the galvanostatic discharge current.The nanosized LixSn significantly lowers the nucleation overpotential and creates abundant lithiophilic nucleation sites,resulting in uniform,dense Li plating/stripping.The modified Cu collector demonstrates superior performance in ether-based electrolytes,achieving over 92%capacity retention after 100 cycles at a current density of 1.5 mA cm^(−2)and an area capacity of 1.1 mAh cm^(−2).This work provides a simple,eco-friendly,and scalable approach for fabricating high-performance anode-free current collectors for AFLMBs.展开更多
Traditional pyrometallurgy and hydrometallurgy processes primarily focus on the recovery of valuable metals(Co,Ni,etc.)from spent lithium-ion batteries.However,these methods are not economical for recycling cheap LiFe...Traditional pyrometallurgy and hydrometallurgy processes primarily focus on the recovery of valuable metals(Co,Ni,etc.)from spent lithium-ion batteries.However,these methods are not economical for recycling cheap LiFePO_(4).Herein,a synergistic thermal-decomposition and electric-drive strategy is proposed to recover the whole spent LiFePO_(4)electrode by in-situ recovering the inactive lithium(dead lithium and trapped interlayer lithium).Firstly,the organic components in the dense solid electrolyte interface(SEI)are effectively decomposed through thermal-decomposition processing,exposing the dead lithium encapsulated within the SEI and recovering the electron channels between the dead lithium and graphite.Leveraging the difference between the Gibbs free energy of the dead lithium and graphite as the driving force facilitates the dead lithium inserting into the anode.Then,fully utilizing the remaining discharge capacity of the spent LiFePO_(4)cell,the inactive lithium is reinserted into LiFePO_(4)lattice during the electric-drive process.Consequently,the reactivated lithium content increases by more than 16%,reaching a capacity of 134.2 mA h g^(-1)compared to 115.2 mA h g^(-1)from degraded LiFePO_(4),allowing for effective participation in the subsequent cycling.This work provides new perspectives on highly profitable cycles with low energy and material consumption and a low carbon footprint.展开更多
The widespread application of solid-state polymer electrolytes(SPEs)is impeded due to their limited ionic conductivity,narrow electrochemical window and lithium dendrite problem.In this work,Mg-metal-organic framework...The widespread application of solid-state polymer electrolytes(SPEs)is impeded due to their limited ionic conductivity,narrow electrochemical window and lithium dendrite problem.In this work,Mg-metal-organic frameworks(MOF)is incorporated into a polyethylene oxide(PEO)-based polymer solid electrolyte,leading to the insitu formation of LiF and other compounds at the electrolyte interface.This modification significantly improves lithium-ion transport capabilities and regulates lithium deposition behavior,suppressing the formation of lithium dendrites.展开更多
基金supported by the Yunnan Fundamental Research Projects(Grant Nos.202401AU070163 and 202501AT070298)the Yunnan Engineering Research Center Innovation Ability Construction and Enhancement Projects(Grant No.2023-XMDJ-00617107)+5 种基金the University Service Key Industry Project of Yunnan Province(Grant No.FWCY-ZD2024005)the Expert Workstation Support Project of Yunnan Province(Grant No.202405AF140069)the Scientific Research Foundation of Kunming University of Science and Technology(Grant No.20220122)the Analysis and Test Foundation of Kunming University of Science and Technology(Grant No.2023T20220122)the Natural Science Foundation of Inner Mongolia Autonomous Region of China(Grant No.2025QN02057)the Ordos City Strategic Pioneering Science and Technology Special Program for New Energy(Grant No.DC2400003365).
文摘Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and long-range electric vehicles.However,technical barriers such as dendrite growth and poor Li plating/stripping reversibility severely hinder the practical application of LMBs.However,lithium nitrate(LiNO_(3))is found to be able to stabilize the Li/electrolyte interface and has been used to address the above challenges.To date,considerable research efforts have been devoted toward understanding the roles of LiNO_(3) in regulating the surface properties of Li anodes and toward the development of many effective strategies.These research efforts are partially mentioned in some articles on LMBs and yet have not been reviewed systematically.To fill this gap,we discuss the recent advances in fundamental and technological research on LiNO_(3) and its derivatives for improving the performances of LMBs,particularly for Li-sulfur(S),Li-oxygen(O),and Li-Li-containing transition-metal oxide(LTMO)batteries,as well as LiNO_(3)-containing recipes for precursors in battery materials and interphase fabrication.This review pays attention to the effects of LiNO_(3) in lithium-based batteries,aiming to provide scientific guidance for the optimization of electrode/electrolyte interfaces and enrich the design of advanced LMBs.
基金supported by the National Natural Science Foundation of China(No.22479021).
文摘Solid-state lithium(Li)batteries are hailed as the nextgeneration energy storage technology,garnering significant attention for their potential high energy density and safety.Particularly when using Li-rich manganese layered oxide(LRMO)as cathodes(theoretical capacity exceeding250 mAh/g),energy densities over 600 Wh/kg can be theoretically achieved[1,2].
基金the financial support from the National Natural Science Foundation of China(52203123 and 52473248)State Key Laboratory of Polymer Materials Engineering(sklpme2024-2-04)+1 种基金the Fundamental Research Funds for the Central Universitiessponsored by the Double First-Class Construction Funds of Sichuan University。
文摘Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving the overall performance of CPEs due to their difficulty in achieving robust electrochemical and mechanical interfaces simultaneously.Here,by regulating the surface charge characteristics of halloysite nanotube(HNT),we propose a concept of lithium-ion dynamic interface(Li^(+)-DI)engineering in nano-charged CPE(NCCPE).Results show that the surface charge characteristics of HNTs fundamentally change the Li^(+)-DI,and thereof the mechanical and ion-conduction behaviors of the NCCPEs.Particularly,the HNTs with positively charged surface(HNTs+)lead to a higher Li^(+)transference number(0.86)than that of HNTs-(0.73),but a lower toughness(102.13 MJ m^(-3)for HNTs+and 159.69 MJ m^(-3)for HNTs-).Meanwhile,a strong interface compatibilization effect by Li^(+)is observed for especially the HNTs+-involved Li^(+)-DI,which improves the toughness by 2000%compared with the control.Moreover,HNTs+are more effective to weaken the Li^(+)-solvation strength and facilitate the formation of Li F-rich solid-electrolyte interphase of Li metal compared to HNTs-.The resultant Li|NCCPE|LiFePO4cell delivers a capacity of 144.9 m Ah g^(-1)after 400 cycles at 0.5 C and a capacity retention of 78.6%.This study provides deep insights into understanding the roles of surface charges of nanofillers in regulating the mechanical and electrochemical interfaces in ASSLMBs.
基金supported by the National Natural Science Foundation of China(22279028,21975063,22421001)the Natural Science Foundation of Hebei Province(B2021205019)the 333 Project of Hebei Province(C20231106)。
文摘Driven by the increasing demand for high-energy-density batteries in electric vehicles and portable electronics,lithium metal batteries have made significant breakthroughs[1–3].While critical challenges associated with lithium metal anodes in liquid electrolytes(e.g.,dendrite growth,interface instability)have hindered commercialization[4–6],solid electrolyte systems have shown promise in mitigating these issues.Among these,solid polymer electrolytes(SPEs)have emerged as a viable solution for enabling stable quasisolid-state lithium metal batteries[7–9].
文摘In order to explore the reduction pathways of zinc oxide in LiCl molten salt and the optimal process,experiments were conducted in an alumina crucible using metallic lithium as the reducing agent and lithium chloride molten salt as the reaction medium at 923 K.The study assessed the effects of lithium thermochemical reduction and electrolytic reduction of ZnO.The volatilization behavior of metal oxides in molten salts,the equivalent of a reducing agent,reduction time,amount of molten salt,stirring time,and the method of reduction feed were investigated for their impacts on the reduction yield and product composition.X-ray powder diffraction(XRD)analysis of the products showed that lithium reduction of ZnO not only produced metallic Zn but also formed a LiZn alloy.Electrolytic reduction can be used to obtain the metallic Zn product by controlling the potential below-2.2 V(vs Ag/Ag^(+)).Moreover,sintered oxides and higher electrode potentials could enhance the efficiency of electrolysis.Under the optimal reaction conditions determined experimentally,the lithium reduction experiment achieved a yield of 77.2%after a 12-h test,and the electrolytic reduction reached a yield of 85.4%after a 6-h test.
文摘Herein,3‑aminopropyltriethoxysilane(APTES)was used to modify F‑containing silica slag(SS)by simple grafting and served as a multifunctional barrier layer.The amino group(—NH2)in the amino‑modified SS(NH2‑SS)forms ligand bonds or hydrogen bonds with sulfur ions in lithium polysulfides(LiPSs),thus inhibiting the shuttle effect.Electrochemical analyses demonstrated that lithium‑sulfur(Li‑S)batteries employing the NH2‑SS interlayer exhibited discharge specific capacities of 1048 and 789 mAh·g^(-1) at 0.2C and 2C,respectively,and even at 4C,the initial discharge specific capacity remained at 590 mAh·g^(-1),outperforming the Li‑S battery with unmodified SS as the interlayer.
基金financially supported by the National Natural Science Foundation of China(Nos.52034002 and U2202254)the Fundamental Research Funds for the Central Universities,China(No.FRF-TT-19-001)。
文摘The sulfation and decomposition process has proven effective in selectively extracting lithium from lepidolite.It is essential to clarify the thermochemical behavior and kinetic parameters of decomposition reactions.Accordingly,comprehensive kinetic study by employing thermalgravimetric analysis at various heating rates was presented in this paper.Two main weight loss regions were observed during heating.The initial region corresponded to the dehydration of crystal water,whereas the subsequent region with overlapping peaks involved complex decomposition reactions.The overlapping peaks were separated into two individual reaction peaks and the activation energy of each peak was calculated using isoconversional kinetics methods.The activation energy of peak 1 exhibited a continual increase as the reaction conversion progressed,while that of peak 2 steadily decreased.The optimal kinetic models,identified as belonging to the random nucleation and subsequent growth category,provided valuable insights into the mechanism of the decomposition reactions.Furthermore,the adjustment factor was introduced to reconstruct the kinetic mechanism models,and the reconstructed models described the kinetic mechanism model more accurately for the decomposition reactions.This study enhanced the understanding of the thermochemical behavior and kinetic parameters of the lepidolite sulfation product decomposition reactions,further providing theoretical basis for promoting the selective extraction of lithium.
基金support of the National Natural Science Foundation of China(22075131 and 22078265)the Shaanxi Fundamental Science Research Project for Mathematics and Physics under Grants(No.22JSZ005)the State-Key Laboratory of Multiphase Complex Systems(No.MPCS-2021-A).
文摘Lithium-sulfur(Li-S)batteries require efficient catalysts to accelerate polysulfide conversion and mitigate the shuttle effect.However,the rational design of catalysts remains challenging due to the lack of a systematic strategy that rationally optimizes electronic structures and mesoscale transport properties.In this work,we propose an autogenously transformed CoWO_(4)/WO_(2) heterojunction catalyst,integrating a strong polysulfide-adsorbing intercalation catalyst with a metallic-phase promoter for enhanced activity.CoWO_(4) effectively captures polysulfides,while the CoWO_(4)/WO_(2) interface facilitates their S-S bond activation on heterogenous catalytic sites.Benefiting from its directional intercalation channels,CoWO_(4) not only serves as a dynamic Li-ion reservoir but also provides continuous and direct pathways for rapid Li-ion transport.Such synergistic interactions across the heterojunction interfaces enhance the catalytic activity of the composite.As a result,the CoWO_(4)/WO_(2) heterostructure demonstrates significantly enhanced catalytic performance,delivering a high capacity of 1262 mAh g^(−1) at 0.1 C.Furthermore,its rate capability and high sulfur loading performance are markedly improved,surpassing the limitations of its single-component counterparts.This study provides new insights into the catalytic mechanisms governing Li-S chemistry and offers a promising strategy for the rational design of high-performance Li-S battery catalysts.
基金supported by the National Natural Science Foundation of China(No.42272044)the High-performance Computing Platform of China University of Geosciences Beijing。
文摘Polyethylene oxide(PEO)-based solid polymer electrolytes(SPEs)have long faced limitations due to low ionic conductivity at ambient temperature and poor interfacial stability with lithium metal anodes.Here,we present a structural engineering strategy to address these challenges through shear-induced crystallization of concentrated PEO-LiTFSI solutions,which self-assemble into flower-like spherulites with radially aligned lamellar crystals.This unique structure creates continuous Li^(+)transport highways through densely packed crystalline domains,achieving a record-high ionic conductivity of 1.70×10^(-4) S/cm at 25℃ for pristine PEO-based systems.Strategic incorporation of lithium montmorillonite(MMTli,10 wt%)further optimizes the composite electrolyte,balancing high ionic conductivity(1.47×10^(-4) S/cm)with enhanced electrochemical stability(4.99 V vs.Li^(+)/Li),elevated Li^(+)transference number(0.62),and mechanical robustness.The composite electrolyte enables stable Li plating/stripping over 800 h in symmetric Li||Li cells and powers LiFePO_(4)||Li solid-state batteries with 82%capacity retention after 200 cycles at 0.2 C under ambient conditions.This work pioneers a scalable processing paradigm for crystalline polymer electrolytes,offering new insights into ion transport mechanisms and validating clay minerals as multifunctional additives for next-generation energy storage systems.
基金the financial support from the National Natural Science Foundation of China (No. 52072390)the National High-Level Talents Special Support Program (Leading Talent of Technological Innovation)+2 种基金the China Postdoctoral Science Foundation (No. 2023M743648)the Young Scientists Fund of the National Natural Science Foundation of China (No. 52302330)the support from the Shanghai Emperor of Cleaning Hi-Tech Co.,LTD
文摘In-situ poly(1,3-dioxolane)(PDOL)-based electrolyte has received extensive attention in the research of lithium metal batteries due to its high stability to lithium anode and simple processing.However,it is still faced with defects such as low intrinsic ionic conductivity,a narrow electrochemical window,and poor thermal stability.A crosslinking and fluorination molecular design strategy toward PDOL is proposed to tackle the issues above.The amorphous crosslinked structure effectively improves ionic conductivity by inhibiting long-chain crystallization.Especially,the antioxidant–CF_(3)groups,stable crosslinked structure,and reduced terminal hydroxyl groups significantly enhance the electrochemical oxidation stability with a superb high-voltage window of 4.7 V.In addition,the designed electrolyte also exhibits obviously improved thermal stability with no deformation at 120°C for 5 min.Furthermore,the semi-solid NCM811||Li batteries exhibit a favourable capacity retention of 88.8%after 150 cycles at 0.5 C.Even assembled with NCM622 cathode working at 4.5 V,the semi-solid batteries can still show a satisfactory capacity retention of 85.3%after 100 cycles at 0.5 C.Also,a 0.1 Ah NCM811||Li pouch cell with active materials loading of 9 mg/cm2 demonstrates satisfactory cycling stability and working ability,which shows promising practical application prospects.
基金the National Natural Science Foundation of China(22479047,22409058)the Outstanding Youth Scientist Foundation of Hunan Province(2022JJ10023)the Provincial Natural Science Foundation of Guangdong(2023A1515011745)for financial support of this research。
文摘To ease the scarcity of lithium(Li)resource and cut down on environmental pollution,an efficient,selective,inexpensive and sustainable Li recycling process from waste batteries is needed,which is yet to be achieved.Here,we report a low-potential photoelectrochemical(PEC)system that selectively and efficiently extracts Li metals from multi-cation electrolytes under 1 sun illumination.Based on the difference of redox potential,we can get rid of the disturbance of other cations(i.e.,Fe,Co and Ni ions)by a bias-free PEC device to realize the extraction of high-purity Li metals on a coplanar Si-based photocathode-TiO_(2) photoanode tandem device at 2 V of applied bias(far less than the redox potentials of Li^(+)/Li).In such system,the extraction rate of Li metals(purity>99.5%)exceeds 1.35 g h^(-1)m^(-2)with 90%of Faradaic efficiency.Long-term experiments,different electrode/electrolyte tests,and various price assessments further demonstrate the stability,compatibility and economy of PEC extraction system,enabling a solar-driven pathway for the recycling of critical metal resources.
基金supported by the National Key R&D Program of China(2021YFB3800300).
文摘High-nickel cathode,LiNi0.8Co0.1Mn0.1O_(2)(NCM811),and sulfide-solid electrolyte are a promising combination for all-solid-state lithium batteries(ASSLBs).However,this combination faces the issue of interfacial instability between the cathode and electrolyte.Given the surface alkalinity of NCM811,we propose a strategy to construct a solid-polymer-electrolyte(SPE)interphase on NCM811 surface by leveraging the surface alkaline residues to nucleophilically initiate the in-situ ring-opening polymerization of cyclic organic molecules.As a proof-of-concept,this study demonstrates that the ring-opening copolymerization of 1,3-dioxolane and maleic anhydride produces a homogeneous,compact,and conformal SPE layer on NCM811 surface to prevent the cathode from contact and reaction with Li6PS5Cl solid-state electrolyte.Consequently,the SPE-modified-NCM811 in ASSLBs exhibits high capacities of 193.5 mA h g^(-1) at 0.2 C,160.9 mA h g^(-1) at 2.0 C and 112.3 mA h g^(-1) at 10 C,and particularly,excellent long-term cycling stabilities over 11000 cycles with a 71.95%capacity retention at 10 C at 25℃,as well as a remained capacity of 117.9 mA h g^(-1) after 8000 cycles at 30 C at 60℃,showing a great application prospect.This study provides a new route for creating electrochemically and structurally stable solid-solid interfaces for ASSLBs.
基金supported by the National Key R&D Program of China(Grant No.2022YFE0207300)the National Natural Science Foundation of China(Grant Nos.22179142 and 22075314)+1 种基金Jiangsu Provincial Science and Technology Program(Grant No.BG 2024020).XPSWAXS and TOF-SIMS characterizations were supported by Nano-X(Vacuum Interconnected Nanotech Workstation,Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences(SINANO),Suzhou 215123,China)。
文摘The practical application of lithium metal batteries(LMBs)requires electrolytes that simultaneously ensure high safety and interfacial stability.Although locally concentrated ionic liquid electrolytes(LCILEs)exhibit exceptional electrochemical stability and compatibility with electrode electrolyte interfaces(EEIs),two major challenges persist:(i)safety risks caused by excessive low-flash-point diluents,and(ii)insufficient understanding of how diluents modulate solvation structures.Herein,we introduce a low-diluent-content LCILE system composed of lithium bis(fluorosulfonyl)imide(LiFSI)salt,N-methyl-N-propyl-pyrrolidinium bis(fluorosulfonyl)imide(Pyr_(13)FSI)ionic liquid,and trifluoromethanesulfonate(TFS)diluent.The TFS diluent strengthens ion-ion interactions by lowering the dielectric constant of the electrolyte,resulting in the formation of a unique nanometric anion aggregates(N-AGGs)reinforced solvation structure.These large anionic clusters exhibit accelerated redox decomposition kinetics,facilitating the rapid formation of a thin,dense,and low-impedance EEI.Consequently,the Li/LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)coin cell achieves 87.8%capacity retention over 300 cycles at 4.3 V,while a practical 1.4 Ah Li/NCM622 pouch cell retains 84.5%capacity after 80 cycles at 4.5 V.Furthermore,the electrolyte demonstrates exceptional safety,and 2 Ah Li metal pouch cells successfully pass rigorous nail penetration tests without any ignition or explosion.This work not only provides a design strategy for intrinsically safe and high-performance electrolytes but also highlights the critical role of anion cluster decomposition kinetics in shaping EEI formation.
基金financially supported by the National Nature Science Foundation of China (No.52401273)Science and Technology Department of Henan (Nos.242102241007,252102320178 and 252102321067)Training Program for Young Backbone Teachers in Higher Education Institutions in Henan Province (No.2024GGJS101)。
文摘Structural instability and sluggish lithium-ion(Li+) kinetics of spinel NiCo_(2)O_(4) anodes severely hinder their applications in high-energy-density lithium-ion batteries.Mesocrystalline structures exhibit promising potential in balancing structural stability and enhancing reaction kinetics.However,their controlled synthesis mechanisms remain elusive.Herein,a substrate interface engineering strategy is developed to achieve controllable synthesis of mesocrystalline and polycrystalline NiCo_(2)O_(4) nanorods.Remarkably,mesocrystalline NiCo_(2)O_(4) exhibits a high capacity retention rate of 85.7% after 500 cycles at 2 A/g,attributed to its porous structure facilitating Li^(+) transport kinetics and unique stress-buffering effect validated by ex-situ TEM.Theoretical calculations and interfacial chemical analysis reveal that substratecrystal surface engineering regulates the nucleation-growth pathways:Acid-treated nickel foam enables epitaxial growth via lattice matching,acting as a low-interfacial-energy template to reduce nucleation barriers and promote low-temperature oriented crystallization.In contrast,carbon cloth requires hightemperature thermal activation to overcome surface diffusion barriers induced by elevated interfacial energy.This substrate-driven crystallization kinetic modulation overcomes the limitations of random nucleation in conventional hydrothermal synthesis.The established substrate-crystal interfacial interaction model not only clarifies the kinetic essence of crystal orientation regulation but also provides a universal theoretical framework for lattice-matching design and mesostructural optimization of advanced electrode materials.
文摘Crystallized lithium fluoride(LiF)melts at 848℃ upon heating,and evaporates subsequently at a remarkably high temperature of 1673℃,characterizing its excellent thermally stability as one of the most representative metal halides.The marriage between Li F and rechargeable batteries dates back to early activities related to the electrochemical properties of lithium metal(Li°)negative electrodes,in which the nonaqueous electrolytes containing fluorinated salts were generally employed,e.g.,lithium tetrafluoroborate(LiBF_(4)),lithium hexafluoroarsenate(LiAsF_(6)),lithium trifluoromethanesulfonate(CF_(3)SO_(3)Li)[1].
基金supported by Basic Science Research Program(Priority Research Institute)through the NRF of Korea funded by the Ministry of Education(2021R1A6A1A10039823)by the Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Ministry of Education(2020R1A6C101B194)。
文摘Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.
基金supported by the National Natural Science Foundation of China (Grant Nos.12192251,12334014,62335019,12134001,1230441812474378)+1 种基金the Quantum Science and Technology National Science and Technology Major Project(Grant No.2021ZD0301403)the Shanghai Municipal Science and Technology Major Project (Grant No.2019SHZDZX01)。
文摘Photonic neural networks(PNNs)of sufficiently large physical dimensions and high operation accuracies are envisaged as ideal candidates for breaking the major bottlenecks in the current artificial intelligence architectures in terms of latency,energy efficiency,and computational power.To achieve this vision,it is of vital importance to scale up the PNNs while simultaneously reducing the high demand on the dimensions required by them.The underlying cause of this strategy is the enormous gap between the scales of photonic and electronic integrated circuits.Here,we demonstrate monolithically integrated optical convolutional processors on thin film lithium niobate(TFLN)that harness inherent parallelism in photonics to enable large-scale programmable convolution kernels and,in turn,greatly reduce the dimensions required by subsequent fully connected layers.Experimental validation achieves high classification accuracies of 96%(86%)on the MNIST(Fashion-MNIST)dataset and 84.6%on the AG News dataset while dramatically reducing the required subsequent fully connected layer dimensions to 196×10(from 784×10)and 175×4(from 800×4),respectively.Furthermore,our devices can be driven by commercial field-programmable gate array systems;a unique advantage in addition to their scalable channel number and kernel size.Our architecture provides a solution to build practical machine learning photonic devices.
基金supported by the National Research Foundation of Korea (NRF) grant funded by the Korean Government (MSIT)(No. 2020R1A5A1019131)supported by a Korea Institute of Energy Technology Evaluation and Planning (KETEP)grant funded by the Korean government (MOTIE)(RS-2022-KP002703, Sector coupling energy industry advancement manpower training program)+1 种基金supported by the Korea Institute of Energy Technology Evaluation and Planning(KETEP)the Ministry of Trade,Industry&Energy(MOTIE) of the Republic of Korea (RS-2024-00469587)
文摘Anode-free lithium-metal batteries(AFLMBs)offer high energy density.However,lithium dendrite growth and interfacial instability remain critical obstacles to their commercialization.Here,lithiophilic nanosized(∼5 nm)LixSn combined with an inorganic-rich@polymer dual-layer structure was constructed on a Cu current collector,prepared via a galvanostatic process using a dual-lithium salt electrolyte in a Cu||Cu configuration.The polymer outer layer,initiated by LixSn,reinforces the solid electrolyte interphase(SEI),providing mechanical robustness and enabling stable cycling in an ether-based electrolyte.Furthermore,the Sn and LixSn particle sizes can be effectively tuned by adjusting the galvanostatic discharge current.The nanosized LixSn significantly lowers the nucleation overpotential and creates abundant lithiophilic nucleation sites,resulting in uniform,dense Li plating/stripping.The modified Cu collector demonstrates superior performance in ether-based electrolytes,achieving over 92%capacity retention after 100 cycles at a current density of 1.5 mA cm^(−2)and an area capacity of 1.1 mAh cm^(−2).This work provides a simple,eco-friendly,and scalable approach for fabricating high-performance anode-free current collectors for AFLMBs.
基金supported by the Key Technologies R&D Program of Xiamen(No.3502Z20231057)the Natural Science Foundation of Fujian Province,China(No.2024J011210,No.2021J011214,No.2021J01685)+5 种基金the High-Level Talent Start-Up Foundation of Xiamen Institute of Technology for financial support(No.YKJ23017R)the Industry Leading Key Projects of Fujian Province(No.2022H0057)the Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang(2020R01002)the Fujian Young and Middle-aged Teachers Teacher Education Research Project(Science and Technology)(No.JAT200461)2023 Xiamen Overseas Students Scientific Research Project(Start-up)the National Natural Science Foundation of China(No.21975212,No.22101242,No.52002352,No.52071295)。
文摘Traditional pyrometallurgy and hydrometallurgy processes primarily focus on the recovery of valuable metals(Co,Ni,etc.)from spent lithium-ion batteries.However,these methods are not economical for recycling cheap LiFePO_(4).Herein,a synergistic thermal-decomposition and electric-drive strategy is proposed to recover the whole spent LiFePO_(4)electrode by in-situ recovering the inactive lithium(dead lithium and trapped interlayer lithium).Firstly,the organic components in the dense solid electrolyte interface(SEI)are effectively decomposed through thermal-decomposition processing,exposing the dead lithium encapsulated within the SEI and recovering the electron channels between the dead lithium and graphite.Leveraging the difference between the Gibbs free energy of the dead lithium and graphite as the driving force facilitates the dead lithium inserting into the anode.Then,fully utilizing the remaining discharge capacity of the spent LiFePO_(4)cell,the inactive lithium is reinserted into LiFePO_(4)lattice during the electric-drive process.Consequently,the reactivated lithium content increases by more than 16%,reaching a capacity of 134.2 mA h g^(-1)compared to 115.2 mA h g^(-1)from degraded LiFePO_(4),allowing for effective participation in the subsequent cycling.This work provides new perspectives on highly profitable cycles with low energy and material consumption and a low carbon footprint.
基金supported by the National Natural Science Foundation of China(Nos.52374302 and 51874099)the Natural Science Foundation of Fujian Province’s Key Project(No.2021J02031)+1 种基金support from the open fund from Academy of Carbon Neutrality of Fujian Normal University(No.TZH_(2)022-06)We also thank the Undergraduate Training Programs for Innovation and Entrepreneurship(No.cxx1-2024363)。
文摘The widespread application of solid-state polymer electrolytes(SPEs)is impeded due to their limited ionic conductivity,narrow electrochemical window and lithium dendrite problem.In this work,Mg-metal-organic frameworks(MOF)is incorporated into a polyethylene oxide(PEO)-based polymer solid electrolyte,leading to the insitu formation of LiF and other compounds at the electrolyte interface.This modification significantly improves lithium-ion transport capabilities and regulates lithium deposition behavior,suppressing the formation of lithium dendrites.
