Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temp...Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temperature(LT)operation.Therefore,a more comprehensive and systematic understanding of LIB behavior at LT is urgently required.This review article comprehensively reviews recent advancements in electrolyte engineering strategies aimed at improving the low-temperature operational capabilities of LIBs.The study methodically examines critical performance-limiting mechanisms through fundamental analysis of four primary challenges:insufficient ionic conductivity under cryogenic conditions,kinetically hindered charge transfer processes,Li+transport limitations across the solidelectrolyte interphase(SEI),and uncontrolled lithium dendrite growth.The work elaborates on innovative optimization approaches encompassing lithium salt molecular design with tailored dissociation characteristics,solvent matrix optimization through dielectric constant and viscosity regulation,interfacial engineering additives for constructing low-impedance SEI layers,and gel-polymer composite electrolyte systems.Notably,particular emphasis is placed on emerging machine learning-guided electrolyte formulation strategies that enable high-throughput virtual screening of constituent combinations and prediction of structure-property relationships.These artificial intelligence-assisted rational design frameworks demonstrate significant potential for accelerating the development of next-generation LT electrolytes by establishing quantitative composition-performance correlations through advanced data-driven methodologies.展开更多
The olivine-type lithium iron phosphate(LiFePO_(4))cathode material is promising and widely used as a high-performance lithium-ion battery cathode material in commercial batteries due to its low cost,environmental fri...The olivine-type lithium iron phosphate(LiFePO_(4))cathode material is promising and widely used as a high-performance lithium-ion battery cathode material in commercial batteries due to its low cost,environmental friendliness,and high safety.At present,LiFePO_(4)/C sec-ondary batteries are widely used for electronic products,automotive power batteries,and other occasion-related applications with good thermal stability,stable cycle performance,and low room-temperature self-discharge rate.However,LiFePO_(4)-based battery applications are seriously limited when they are operated in a cold climate.This outcome is due to a considerable decrease in Li+transport capabilities within the elec-trode,particularly leading to a dramatic decrease in the electrochemical capacity and power performance of the electrolyte.Therefore,the design of low-temperature electrolytes is important for the further commercial application of LiFePO_(4) batteries.This paper reviews the key factors for the poor low-temperature performance of LiFePO_(4)-based batteries and the research progress of low-temperature electrolytes.Spe-cial attention is paid to electrolyte components,including lithium salts,cosolvents,additives,and the development of new electrolytes.The factors affecting the anode are also analyzed.Finally,according to the current research progress,some viewpoints are summarized to provide suitable modification methods and research suggestions for improving the practicability of LiFePO_(4)/C commercial batteries at low temperat-ures in the future.展开更多
Lithium-ion batteries are widely recognized as prime candidates for energy storage devices.Ethylene carbonate(EC)has become a critical component in conventional commercial electrolytes due to its exceptional film-form...Lithium-ion batteries are widely recognized as prime candidates for energy storage devices.Ethylene carbonate(EC)has become a critical component in conventional commercial electrolytes due to its exceptional film-forming properties and high dielectric constant.However,the elevated freezing point,high viscosity,and strong solvation energy of EC significantly hinder the transport rate of Li^(+)and the desolvation process at low temperatures.This leads to substantial capacity loss and even lithium plating on graphite anodes.Herein,we have developed an efficient electrolyte system specifically designed for lowtemperature conditions,which consists of 1.0 M lithium bis(fluorosulfonyl)imide(LiFSI)in isoxazole(IZ)with fluorobenzene(FB)as an uncoordinated solvent and fluoroethylene carbonate(FEC)as a filmforming co-solvent.This system effectively lowers the desolvation energy of Li^(+)through dipole-dipole interactions.The weak solvation capability allows more anions to enter the solvation sheath,promoting the formation of contact ion pairs(CIPs)and aggregates(AGGs)that enhance the transport rate of Li^(+)while maintaining high ionic conductivity across a broad temperature range.Moreover,the formation of inorganic-dominant interfacial phases on the graphite anode,induced by fluoroethylene carbonate,significantly enhances the kinetics of Li^(+)transport.At a low temperature of-20℃,this electrolyte system achieves an impressive reversible capacity of 200.9 mAh g^(-1)in graphite half-cell,which is nearly three times that observed with conventional EC-based electrolytes,demonstrating excellent stability throughout its operation.展开更多
The poor oxidation stability of ether-based solvents has long been a major challenge limiting their practical application.To enhance the oxidative stability of ether-based electrolytes,the physicochemical properties o...The poor oxidation stability of ether-based solvents has long been a major challenge limiting their practical application.To enhance the oxidative stability of ether-based electrolytes,the physicochemical properties of various glycol dimethyl ethers are screened,and diglyme(G2)is selected as the sole solvent for the electrolyte.Lithium bis(fluorosulfonyl)imide(LiFSI),a highly dissociative salt,is used as the primary salt;while lithium nitrate(LiNO_(3))and lithium difluorophosphate(LiDFP),which have small ionic sizes and strong binding energies,are added as secondary salts.The resulting electrolyte can modulate the electric double layer structure by NO_(3)^(-) and DFP^(-) on the cathode side,leading to an increased Liþconcentration that is originally repelled by the cathode.Additionally,the oxidation stability of the electrolyte is improved and the formed electrode-electrolyte interphase is more uniform and stable,thereby enhancing the electrochemical performance of the cells.As a result,cells assembled with a total of 1 M ternary lithium salts in G2 solvent can operate at high voltage of 4.4 V.The LijjNCM811 cells maintain 80.2%capacity retention after 270 cycles at room temperature,with an average Coulombic efficiency of 99.5%,and exhibit 88.4%capacity retention after 200 cycles at -30℃.展开更多
Flexible zinc-ion batteries(FZIBs)have been acknowledged as a potential cornerstone for the future development of flexible energy storage,yet conventional FZIBs still encounter challenges,particularly concerning perfo...Flexible zinc-ion batteries(FZIBs)have been acknowledged as a potential cornerstone for the future development of flexible energy storage,yet conventional FZIBs still encounter challenges,particularly concerning performance failure at low temperatures.To address these challenges,a novel anti-freezing leather gel electrolyte(AFLGE-30)is designed,incorporating ethanol as a hydrogen bonding acceptor.The AFLGE-30 demonstrates exceptional frost resistance while maintaining favorable flexibility even at-30℃;accordingly,the battery can achieve a high specific capacity of about 70 m Ah/g.Cu//Zn battery exhibits remarkable stability at room temperature,retaining~96%efficiency after 120 plating/stripping cycles at1 m A/cm^(2).Concurrently,the Zn//Zn symmetric batteries demonstrate a lifespan of 4100 h at room temperature,which is attributed to the enhancement of Zn^(2+)deposition kinetics,restraining the formation of zinc dendrites.Furthermore,FZIBs exhibit minimal capacity loss even after bending,impacting,or burning.This work provides a promising strategy for designing low-temperature-resistant FZIBs.展开更多
Aqueous Zn-metal batteries(AZMBs)performance is hampered by freezing water at low temperatures,which hampers their multi-scenario application.Hydrogen bonds(HBs)play a pivotal role in water freezing,and proton transpo...Aqueous Zn-metal batteries(AZMBs)performance is hampered by freezing water at low temperatures,which hampers their multi-scenario application.Hydrogen bonds(HBs)play a pivotal role in water freezing,and proton transport is indispensable for the establishment of HBs.Here,the accelerated proton transport modulates the dynamic hydrogen bonding network of a Zn(BF4)2/EMIMBF4impregnated polyacrylamide/poly(vinyl alcohol)/xanthan gum dual network eutectic gel electrolyte(PPX-ILZSE)for lowtemperature AZMBs.The PPX-ILZSE forms more HBs,shorter HBs lifetimes,higher tetrahedral entropy,and faster desolvation processes,as demonstrated by experimental and theoretical calculations.This enhanced dynamic proton transport promotes rapid cycling of HBs formation-failure,and for polyaniline cathode(PANI)abundant redox sites of proton,confers excellent low temperature electrochemical performance to the Zn//PANI full cell.Specific capacities for 1000 and 5000 cycles at 1 and 5 A g^(-1)were149.8 and 128.4 m A h g^(-1)at room temperature,respectively.Furthermore,specific capacities of 131.1 mA hg^(-1)(92.4%capacity retention)and 0.0066%capacity decay per lap were achieved for 3000and 3500 laps at-30 and 40℃,respectively,at 0.5 A g^(-1).Furthermore,in-situ protective layer of ZnOHF nano-arrays on the Zn anode surface to eliminate dendrite growth and accelerate Zn-ions adsorption and charge transfer.展开更多
Aqueous zinc-ion batteries are regarded as the promising candidates for large-scale energy storage systems owing to low cost and high safety;however,their applications are restricted by their poor low-temperature perf...Aqueous zinc-ion batteries are regarded as the promising candidates for large-scale energy storage systems owing to low cost and high safety;however,their applications are restricted by their poor low-temperature performance.Herein,a low-temperature electrolyte for low-temperature aqueous zinc-ion batteries is designed by introducing low-polarity diglyme into an aqueous solution of Zn(ClO_(4))_(2).The diglyme disrupts the hydrogenbonding network of water and lowers the freezing point of the electrolyte to-105℃.The designed electrolyte achieves ionic conductivity up to16.18 mS cm^(-1)at-45℃.The diglyme and ClO_(4)^(-)reconfigure the solvated structure of Zn^(2+),which is more favorable for the desolvation of Zn^(2+)at low temperatures.In addition,the diglyme effectively suppresses the dendrites,hydrogen evolution reaction,and by-products of the zinc anode,improving the cycle stability of the battery.At-20℃,a Zn‖Zn symmetrical cell is cycled for 5200 h at 1 mA cm^(-2)and 1 mA h cm^(-2),and a Zn‖polyaniline battery achieves an ultra-long cycle life of 10000 times.This study sheds light on the future design of electrolytes with high ionic conductivity and easy desolvation at low temperatures for rechargeable batteries.展开更多
Aqueous alkali metal-ion batteries(AAMIBs)have been recognized as emerging electrochemical energy storage technologies for grid-scale applications owning to their intrinsic safety,cost-effectiveness,and environmental ...Aqueous alkali metal-ion batteries(AAMIBs)have been recognized as emerging electrochemical energy storage technologies for grid-scale applications owning to their intrinsic safety,cost-effectiveness,and environmental sustainability.However,the practical application of AAMIBs is still severely constrained by the tendency of aqueous electrolytes to freeze at low temperatures and decompose at high temperatures,limiting their operational temperature range.Considering the urgent need for energy systems with higher adaptability and resilience at various application scenarios,designing novel electrolytes via structure modulation has increasingly emerged as a feasible and economical strategy for the performance optimization of wide-temperature AAMIBs.In this review,the latest advancement of wide-temperature electrolytes for AAMIBs is systematically and comprehensively summarized.Specifically,the key challenges,failure mechanisms,correlations between hydrogen bond behaviors and physicochemical properties,and thermodynamic and kinetic interpretations in aqueous electrolytes are discussed firstly.Additionally,we offer forward-looking insights and innovative design principles for developing aqueous electrolytes capable of operating across a broad temperature range.This review is expected to provide some guidance and reference for the rational design and regulation of widetemperature electrolytes for AAMIBs and promote their future development.展开更多
Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density...Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density.However,their practical commercialization is hindered by critical challenges on the anode side,including dendrite growth and parasitic reactions at the anode/electrolyte interface.Recent studies highlight that rational electrolyte structure engineering offers an effective route to mitigate these issues and strengthen the electrochemical performance of the zinc metal anode.In this review,we systematically summarize state-of-the-art strategies for electrolyte optimization,with a particular focus on the zinc salts regulation,electrolyte additives,and the construction of novel electrolytes,while elucidating the underlying design principles.We further discuss the key structure–property relationships governing electrolyte behavior to provide guidance for the development of next-generation electrolytes.Finally,future perspectives on advanced electrolyte design are proposed.This review aims to serve as a comprehensive reference for researchers exploring high-performance electrolyte engineering in AZIBs.展开更多
This study focused on improving the cathode performance of Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.15)O_(3-δ)(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea_(0.6)Sr_(0.4)Co_(0...This study focused on improving the cathode performance of Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.15)O_(3-δ)(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.1)Mo_(0.05)O_(3-δ)(B S CNM_(0.05)),Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.05)Mo_(0.1)O_(3-δ)(BSCNM_(0.1)),and Ba_(0.6)Sr_(0.4)Co_(0.85)Mo_(0.15)O_(3-δ)(BSCM)—with Mo doping contents of 5mol%,10mol%,and15mol%,respectively,were successfully prepared using the sol-gel method.The effects of Mo doping on the crystal structure,conductivity,thermal expansion coefficient,oxygen reduction reaction(ORR)activity,and electrochemical performance were systematically evaluated using X-ray diffraction analysis,thermally induced characterization,electrochemical impedance spectroscopy,and single-cell performance tests.The results revealed that Mo doping could improve the conductivity of the materials,suppress their thermal expansion effects,and significantly improve the electrochemical performance.Surface chemical state analysis using X-ray photoelectron spectroscopy revealed that 5mol%Mo doping could facilitate a high adsorbed oxygen concentration leading to enhanced ORR activity in the materials.Density functional theory calculations confirmed that Mo doping promoted the ORR activity in the materials.At an operating temperature of 600℃,the BSCNM_(0.05)cathode material exhibited significantly enhanced electrochemical impedance characteristics,with a reduced area specific resistance of 0.048Ω·cm~2,which was lower than that of the undoped BSCN matrix material by 32.39%.At the same operating temperature,an anode-supported single cell using a BSCNM_(0.05)cathode achieved a peak power density of 1477 mW·cm^(-2),which was 30.71%,56.30%,and 171.50%higher than those of BSCN,BSCNM_(0.1),and B SCM,respectively.The improved ORR activity and electrochemical performance of BSCNM_(0.05)indicate that it can be used as a cathode material in low-temperature solid oxide fuel cells.展开更多
The pursuit of high energy density and sustainable energy storage devices has been the target of many researchers.However,safety issues such as the susceptibility of conventional liquid electrolytes to leakage and fla...The pursuit of high energy density and sustainable energy storage devices has been the target of many researchers.However,safety issues such as the susceptibility of conventional liquid electrolytes to leakage and flammability,as well as performance degradation due to uncontrollable dendrite growth in liquid electrolytes,have been limiting the further development of energy storage devices.In this regard,gel polymer electrolytes(GPEs)based on lignocellulosic(cellulose,hemicellulose,lignin)have attracted great interest due to their high thermal stability,excellent electrolyte wettability,and natural abundance.Therefore,in this critical review,a comprehensive overview of the current challenges faced by GPEs is presented,followed by a detailed description of the opportunities and advantages of lignocellulosic materials for the fabrication of GPEs for energy storage devices.Notably,the key properties and corresponding construction strategies of GPEs for energy storage are analyzed and discussed from the perspective of lignocellulose for the first time.Moreover,the future challenges and prospects of lignocellulose-mediated GPEs in energy storage applications are also critically reviewed and discussed.We sincerely hope this review will stimulate further research on lignocellulose-mediated GPEs in energy storage and provide meaningful directions for the strategy of designing advanced GPEs.展开更多
Chloride-based solid electrolytes are considered promising candidates for next-generation high-energy-density all-solid-state batteries(ASSBs).However,their relatively low oxidative decomposition threshold(~4.2 V vs.L...Chloride-based solid electrolytes are considered promising candidates for next-generation high-energy-density all-solid-state batteries(ASSBs).However,their relatively low oxidative decomposition threshold(~4.2 V vs.Li^(+)/Li)constrains their use in ultrahighvoltage systems(e.g.,4.8 V).In this work,ferroelectric Ba TiO_(3)(BTO)nanoparticles with optimized thickness of~50-100 nm were successfully coated onto Li_(2.5)Y_(0.5)Zr_(0.5)Cl_(6)(LYZC@5BTO)electrolytes using a time-efficient ball-milling process.The nanoparticle-induced interfacial ionic conduction enhancement mechanism contributed to the preservation of LYZC’s high ionic conductivity,which remained at 1.06 m S cm^(-1)for LYZC@5BTO.Furthermore,this surface electric field engineering strategy effectively mitigates the voltage-induced self-decomposition of chloride-based solid electrolytes,suppresses parasitic interfacial reactions with single-crystal NCM811(SCNCM811),and inhibits the irreversible phase transition of SCNCM811.Consequently,the cycling stability of LYZC under high-voltage conditions(4.8 V vs.Li+/Li)is significantly improved.Specifically,ASSB cells employing LYZC@5BTO exhibited a superior discharge capacity of 95.4 m Ah g^(-1)over 200 cycles at 1 C,way outperforming cell using pristine LYZC that only shows a capacity of 55.4 m Ah g^(-1).Furthermore,time-of-flight secondary ion mass spectrometry and X-ray photoelectron spectroscopy analysis revealed that Metal-O-Cl by-products from cumulative interfacial side reactions accounted for 6% of the surface species initially,rising to 26% after 200 cycles in pristine LYZC.In contrast,LYZC@5BTO limited this increase to only 14%,confirming the effectiveness of BTO in stabilizing the interfacial chemistry.This electric field modulation strategy offers a promising route toward the commercialization of high-voltage solid-state electrolytes and energy-dense ASSBs.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
Supercapacitors(SCs) are high-power energy storage devices with ultra-fast charge/discharge properties.SCs using concentrated aqueous-based electrolytes can work at low temperatures due to their intrinsic properties, ...Supercapacitors(SCs) are high-power energy storage devices with ultra-fast charge/discharge properties.SCs using concentrated aqueous-based electrolytes can work at low temperatures due to their intrinsic properties, such as higher freezing point depression(FPD) and robustness. Besides the traditional organic-and aqueous-based(salt-in-water) electrolytes used in SCs, water-in-salt(WISE) sodium perchlorate electrolytes offer high FPD, non-flammability, and low-toxicity conditions, allowing the fabrication of safer, environmentally friendly, and more robust devices. For the first time, this work reports a comprehensive study regarding WISE system’s charge-storage capabilities and physicochemical properties under low-temperature conditions(T < 0 ℃) using mesoporous carbon-based electrodes. The effect of temperature reduction on the electrolyte viscosity and electrical properties was investigated using different techniques and the in-situ(or operando) Raman spectroscopy under dynamic polarization conditions.The cell voltage, equivalent series resistance, and specific capacitance were investigated as a function of the temperature. The cell voltage(U) increased ~ 50%, while the specific capacitance decreased ~20%when the temperature was reduced from 25 ℃ to -10 ℃. As a result, the maximum specific energy(E = CU^(2)/2) increased ~ 100%. Therefore, low-temperature WISEs are promising candidates to improve the energy-storage characteristics in SCs.展开更多
This work reviews technologies that can be used to develop low-temperature solid oxide cells(LT-SOCs)and can be applied in fuel cells and electrolyzers operating at temperatures below 500℃,thus providing a more cost-...This work reviews technologies that can be used to develop low-temperature solid oxide cells(LT-SOCs)and can be applied in fuel cells and electrolyzers operating at temperatures below 500℃,thus providing a more cost-effective alternative than conventional high-temperature SOCs.Two routes showing potential to reduce the operating temperature of SOCs to below 500℃ are discussed.The first route is the principal way to enhance cell performance,namely,structure optimization.This technique includes the reduction of electrolyte thickness to the nanometer scale and the exploration of electrode structure with low polarization resistance.The other route is the development of novel protonconducting electrolyte materials,which is in the frontier of SOCs study.The fundamentals of proton conduction and the design principles of commonly used electrolyte materials are briefly explained.The most widely studied electrolyte materials for LT-SOCs,namely,perovskitetype BaCeO_(3) -and BaZrO_(3) -based oxides,and the effect of doping on the physical-chemical properties of these oxide materials are summarized.展开更多
With the increasing demand and striking upsurge in the price of lithium carbonate,sodium-ion batteries(SIBs)have gained significant attentions due to their abundance over lithium-ion batteries(LIBs).Some prototype SIB...With the increasing demand and striking upsurge in the price of lithium carbonate,sodium-ion batteries(SIBs)have gained significant attentions due to their abundance over lithium-ion batteries(LIBs).Some prototype SIBs have achieved great progress in terms of energy densities.Although SIBs show a relatively higher tolerance at the low temperature than LIBs due to the weaker cation–solvent interaction,the low-temperature performance of SIBs remains a critical challenge restricted by the electrolyte solidification and sluggish interphasial kinetics.In this review,we briefly cover the latest research progress in usable low-temperature electrolytes for SIBs.In the meantime,the mitigating mechanism and low-temperature performance of the electrolytes in different SIB configurations are also discussed.The merits and demerits of ether-based and carbonate-based electrolytes are compared to demonstrate their potential and limitations,thus providing application principles for ether-based and carbonate-based electrolytes at low temperatures to maximize their advantages.Furthermore,mitigation strategies for lowtemperature electrolytes are emphasized to guide the future electrolyte design.Finally,we provide some perspectives on the development of the low-temperature electrolytes for SIBs.展开更多
In the present study,high-quality apatite-type La9.33Ge6O26 powders are successfully synthesized by a facile moltensalt synthesis method（MSSM） at low temperatures,using Li Cl,Li Cl/Na Cl mixture（mass ratio 1：1） a...In the present study,high-quality apatite-type La9.33Ge6O26 powders are successfully synthesized by a facile moltensalt synthesis method（MSSM） at low temperatures,using Li Cl,Li Cl/Na Cl mixture（mass ratio 1：1） as molten salt,respectively.Experimental results indicate that the optimal mass ratio between reactant and molten salt is 1：2,and Li Cl/Na Cl mixed molten-salt is more beneficial for forming high-quality La9.33Ge6O26 powders than Li Cl individual molten-salt.Comparing with the conventional solid-state reaction method（SSRM）,the synthesis temperature of apatitetype La9.33Ge6O26 powders using the MSSM decreases more than 350℃,which can effectively avoid Ge loss in the preparation process of precursor powders.Furthermore,the powders obtained by the MSSM are homogeneous,nonagglomerated and well crystallized,which are very favorable for gaining dense pellets in the premise of avoiding Ge loss.On the basis of high-quality precursor powders,the dense and pure ceramic pellets of La（9.33）Ge6O（26） are gained at a low temperature of 1100℃ for 2 h,which exhibit higher conductivities（σ850℃（Li Cl）= 2.3 × 10^-2 S·cm^-1,σ850 ℃（Li Cl/Na Cl） = 4.9 × 10^-2 S·cm^-1） and lower activation energies（Ea（Li Cl）= 1.02 e V,Ea（Li Cl/Na Cl）= 0.99 e V） than that synthesized by the SSRM.展开更多
The effect of KOH electrolyte concentration on low-temperature electrochemical properties of LaNi5 alloy electrodes at 233 K was studied. The results indicated that the electrolyte concentration had great influence on...The effect of KOH electrolyte concentration on low-temperature electrochemical properties of LaNi5 alloy electrodes at 233 K was studied. The results indicated that the electrolyte concentration had great influence on discharge capacity and discharge voltage plateau of LaNi5 alloy electrode at 233 K, and the highest discharge capacity and discharge voltage plateau were both obtained at 6 mol/L KOH. When the KOH electrolyte concentration changed from 5 to 9 mol/L at 233 K, the high rate discharge ability （HRD） had the same change tendency as the diffusion coefficient, but the exchange current density did not change significantly, which implied that hydrogen diffusion was the control step at low temperature 233 K for discharge process of LaNi5 alloy electrode.展开更多
Lithium-ion batteries(LIBs)have monopolized energy storage markets in modern society.The reliable operation of LIBs at cold condition(<0°C),nevertheless,is inevitably hampered by the sluggish kinetics and para...Lithium-ion batteries(LIBs)have monopolized energy storage markets in modern society.The reliable operation of LIBs at cold condition(<0°C),nevertheless,is inevitably hampered by the sluggish kinetics and parasite reactions,which falls behind the increasing demands for portable electronics and electric vehicles.The electrolyte controls both Li+transport and interfacial reaction,dictating the low-temperature performance substantially.Therefore,the rational formulation of electrolytes is significant for realizing superior lowtemperature performance and broadening application niches of LIBs.Herein,we first discuss the kinetic limitations of low-temperature LIBs,highlighting the importance of electrolyte structure and interfacial chemistry.Then,the advancements for formulating subzero-temperature electrolyte are summarized with in-depth discussions about electrolyte formulation,solvation structure,interfacial chemistry,and low-temperature behaviors.Moreover,some opportunities for lithium metal batteries and the corresponding lowtemperature electrolyte are covered.Finally,the major challenges and future perspectives are outlined for low-temperature LIBs.展开更多
Hydrogel electrolytes hold great potential in flexible zinc ion supercapacitors(ZICs)due to their high conductivity,good safety,and flexibility.However,freezing of electrolytes at low temperature(subzero)leads to dras...Hydrogel electrolytes hold great potential in flexible zinc ion supercapacitors(ZICs)due to their high conductivity,good safety,and flexibility.However,freezing of electrolytes at low temperature(subzero)leads to drastic reduction in ionic conductivity and mechanical properties that deteriorates the performance of flexible ZICs.Besides,the mechanical fracture during arbitrary deformations significantly prunes out the lifespan of the flexible device.Herein,a Zn^(2+)and Li^(+)co-doped,polypyrrole-dopamine decorated Sb_(2)S_(3)incorporated,and polyvinyl alcohol/poly(N-(2-hydroxyethyl)acrylamide)double-network hydrogel electrolyte is constructed with favorable mechanical reliability,anti-freezing,and self-healing ability.In addition,it delivers ultra-high ionic conductivity of 8.6 and 3.7 S m^(-1)at 20 and−30°C,respectively,and displays excellent mechanical properties to withstand tensile stress of 1.85 MPa with tensile elongation of 760%,together with fracture energy of 5.14 MJ m^(-3).Notably,the fractured hydrogel electrolyte can recover itself after only 90 s of infrared illumination,while regaining 83%of its tensile strain and almost 100%of its ionic conductivity during−30–60°C.Moreover,ZICs coupled with this hydrogel electrolyte not only show a wide voltage window(up to 2 V),but also provide high energy density of 230 Wh kg^(-1)at power density of 500 W kg^(-1)with a capacity retention of 86.7%after 20,000 cycles under 20°C.Furthermore,the ZICs are able to retain excellent capacity even under various mechanical deformation at−30°C.This contribution will open up new insights into design of advanced wearable flexible electronics with environmental adaptability and long-life span.展开更多
基金the financial support from the Key Project of Shaanxi Provincial Natural Science Foundation-Key Project of Laboratory(2025SYS-SYSZD-117)the Natural Science Basic Research Program of Shaanxi(2025JCYBQN-125)+8 种基金Young Talent Fund of Xi'an Association for Science and Technology(0959202513002)the Key Industrial Chain Technology Research Program of Xi'an(24ZDCYJSGG0048)the Key Research and Development Program of Xianyang(L2023-ZDYF-SF-077)Postdoctoral Fellowship Program of CPSF(GZC20241442)Shaanxi Postdoctoral Science Foundation(2024BSHSDZZ070)Research Funds for the Interdisciplinary Projects,CHU(300104240913)the Fundamental Research Funds for the Central Universities,CHU(300102385739,300102384201,300102384103)the Scientific Innovation Practice Project of Postgraduate of Chang'an University(300103725063)the financial support from the Australian Research Council。
文摘Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temperature(LT)operation.Therefore,a more comprehensive and systematic understanding of LIB behavior at LT is urgently required.This review article comprehensively reviews recent advancements in electrolyte engineering strategies aimed at improving the low-temperature operational capabilities of LIBs.The study methodically examines critical performance-limiting mechanisms through fundamental analysis of four primary challenges:insufficient ionic conductivity under cryogenic conditions,kinetically hindered charge transfer processes,Li+transport limitations across the solidelectrolyte interphase(SEI),and uncontrolled lithium dendrite growth.The work elaborates on innovative optimization approaches encompassing lithium salt molecular design with tailored dissociation characteristics,solvent matrix optimization through dielectric constant and viscosity regulation,interfacial engineering additives for constructing low-impedance SEI layers,and gel-polymer composite electrolyte systems.Notably,particular emphasis is placed on emerging machine learning-guided electrolyte formulation strategies that enable high-throughput virtual screening of constituent combinations and prediction of structure-property relationships.These artificial intelligence-assisted rational design frameworks demonstrate significant potential for accelerating the development of next-generation LT electrolytes by establishing quantitative composition-performance correlations through advanced data-driven methodologies.
基金supported by the National Natural Science Foundation of China (No. 52102470)Guangxi Innovation Driven Development Project (No. AA17204100)
文摘The olivine-type lithium iron phosphate(LiFePO_(4))cathode material is promising and widely used as a high-performance lithium-ion battery cathode material in commercial batteries due to its low cost,environmental friendliness,and high safety.At present,LiFePO_(4)/C sec-ondary batteries are widely used for electronic products,automotive power batteries,and other occasion-related applications with good thermal stability,stable cycle performance,and low room-temperature self-discharge rate.However,LiFePO_(4)-based battery applications are seriously limited when they are operated in a cold climate.This outcome is due to a considerable decrease in Li+transport capabilities within the elec-trode,particularly leading to a dramatic decrease in the electrochemical capacity and power performance of the electrolyte.Therefore,the design of low-temperature electrolytes is important for the further commercial application of LiFePO_(4) batteries.This paper reviews the key factors for the poor low-temperature performance of LiFePO_(4)-based batteries and the research progress of low-temperature electrolytes.Spe-cial attention is paid to electrolyte components,including lithium salts,cosolvents,additives,and the development of new electrolytes.The factors affecting the anode are also analyzed.Finally,according to the current research progress,some viewpoints are summarized to provide suitable modification methods and research suggestions for improving the practicability of LiFePO_(4)/C commercial batteries at low temperat-ures in the future.
基金financial support from the Department of Science and Technology of Jilin Province(20240304104SF,20240304103SF)the Research and Innovation Fund of the Beihua University for the Graduate Student(Major Project 2023012)。
文摘Lithium-ion batteries are widely recognized as prime candidates for energy storage devices.Ethylene carbonate(EC)has become a critical component in conventional commercial electrolytes due to its exceptional film-forming properties and high dielectric constant.However,the elevated freezing point,high viscosity,and strong solvation energy of EC significantly hinder the transport rate of Li^(+)and the desolvation process at low temperatures.This leads to substantial capacity loss and even lithium plating on graphite anodes.Herein,we have developed an efficient electrolyte system specifically designed for lowtemperature conditions,which consists of 1.0 M lithium bis(fluorosulfonyl)imide(LiFSI)in isoxazole(IZ)with fluorobenzene(FB)as an uncoordinated solvent and fluoroethylene carbonate(FEC)as a filmforming co-solvent.This system effectively lowers the desolvation energy of Li^(+)through dipole-dipole interactions.The weak solvation capability allows more anions to enter the solvation sheath,promoting the formation of contact ion pairs(CIPs)and aggregates(AGGs)that enhance the transport rate of Li^(+)while maintaining high ionic conductivity across a broad temperature range.Moreover,the formation of inorganic-dominant interfacial phases on the graphite anode,induced by fluoroethylene carbonate,significantly enhances the kinetics of Li^(+)transport.At a low temperature of-20℃,this electrolyte system achieves an impressive reversible capacity of 200.9 mAh g^(-1)in graphite half-cell,which is nearly three times that observed with conventional EC-based electrolytes,demonstrating excellent stability throughout its operation.
文摘The poor oxidation stability of ether-based solvents has long been a major challenge limiting their practical application.To enhance the oxidative stability of ether-based electrolytes,the physicochemical properties of various glycol dimethyl ethers are screened,and diglyme(G2)is selected as the sole solvent for the electrolyte.Lithium bis(fluorosulfonyl)imide(LiFSI),a highly dissociative salt,is used as the primary salt;while lithium nitrate(LiNO_(3))and lithium difluorophosphate(LiDFP),which have small ionic sizes and strong binding energies,are added as secondary salts.The resulting electrolyte can modulate the electric double layer structure by NO_(3)^(-) and DFP^(-) on the cathode side,leading to an increased Liþconcentration that is originally repelled by the cathode.Additionally,the oxidation stability of the electrolyte is improved and the formed electrode-electrolyte interphase is more uniform and stable,thereby enhancing the electrochemical performance of the cells.As a result,cells assembled with a total of 1 M ternary lithium salts in G2 solvent can operate at high voltage of 4.4 V.The LijjNCM811 cells maintain 80.2%capacity retention after 270 cycles at room temperature,with an average Coulombic efficiency of 99.5%,and exhibit 88.4%capacity retention after 200 cycles at -30℃.
基金supported by the National Natural Science Foundation of China(Nos.22075139 and 62288102)。
文摘Flexible zinc-ion batteries(FZIBs)have been acknowledged as a potential cornerstone for the future development of flexible energy storage,yet conventional FZIBs still encounter challenges,particularly concerning performance failure at low temperatures.To address these challenges,a novel anti-freezing leather gel electrolyte(AFLGE-30)is designed,incorporating ethanol as a hydrogen bonding acceptor.The AFLGE-30 demonstrates exceptional frost resistance while maintaining favorable flexibility even at-30℃;accordingly,the battery can achieve a high specific capacity of about 70 m Ah/g.Cu//Zn battery exhibits remarkable stability at room temperature,retaining~96%efficiency after 120 plating/stripping cycles at1 m A/cm^(2).Concurrently,the Zn//Zn symmetric batteries demonstrate a lifespan of 4100 h at room temperature,which is attributed to the enhancement of Zn^(2+)deposition kinetics,restraining the formation of zinc dendrites.Furthermore,FZIBs exhibit minimal capacity loss even after bending,impacting,or burning.This work provides a promising strategy for designing low-temperature-resistant FZIBs.
基金supported by the National Natural Science Foundation of China(NSFC 52432002,52372041,and 52302087)China Postdoctoral Science Foundation(Grant No.2023 M740895)+1 种基金Heilongjiang Touyan Team Programthe Fundamental Research Funds for the Central Universities(Grant No.HIT.OCEF.2021003 and HIT.DZJJ.2025002)。
文摘Aqueous Zn-metal batteries(AZMBs)performance is hampered by freezing water at low temperatures,which hampers their multi-scenario application.Hydrogen bonds(HBs)play a pivotal role in water freezing,and proton transport is indispensable for the establishment of HBs.Here,the accelerated proton transport modulates the dynamic hydrogen bonding network of a Zn(BF4)2/EMIMBF4impregnated polyacrylamide/poly(vinyl alcohol)/xanthan gum dual network eutectic gel electrolyte(PPX-ILZSE)for lowtemperature AZMBs.The PPX-ILZSE forms more HBs,shorter HBs lifetimes,higher tetrahedral entropy,and faster desolvation processes,as demonstrated by experimental and theoretical calculations.This enhanced dynamic proton transport promotes rapid cycling of HBs formation-failure,and for polyaniline cathode(PANI)abundant redox sites of proton,confers excellent low temperature electrochemical performance to the Zn//PANI full cell.Specific capacities for 1000 and 5000 cycles at 1 and 5 A g^(-1)were149.8 and 128.4 m A h g^(-1)at room temperature,respectively.Furthermore,specific capacities of 131.1 mA hg^(-1)(92.4%capacity retention)and 0.0066%capacity decay per lap were achieved for 3000and 3500 laps at-30 and 40℃,respectively,at 0.5 A g^(-1).Furthermore,in-situ protective layer of ZnOHF nano-arrays on the Zn anode surface to eliminate dendrite growth and accelerate Zn-ions adsorption and charge transfer.
文摘Aqueous zinc-ion batteries are regarded as the promising candidates for large-scale energy storage systems owing to low cost and high safety;however,their applications are restricted by their poor low-temperature performance.Herein,a low-temperature electrolyte for low-temperature aqueous zinc-ion batteries is designed by introducing low-polarity diglyme into an aqueous solution of Zn(ClO_(4))_(2).The diglyme disrupts the hydrogenbonding network of water and lowers the freezing point of the electrolyte to-105℃.The designed electrolyte achieves ionic conductivity up to16.18 mS cm^(-1)at-45℃.The diglyme and ClO_(4)^(-)reconfigure the solvated structure of Zn^(2+),which is more favorable for the desolvation of Zn^(2+)at low temperatures.In addition,the diglyme effectively suppresses the dendrites,hydrogen evolution reaction,and by-products of the zinc anode,improving the cycle stability of the battery.At-20℃,a Zn‖Zn symmetrical cell is cycled for 5200 h at 1 mA cm^(-2)and 1 mA h cm^(-2),and a Zn‖polyaniline battery achieves an ultra-long cycle life of 10000 times.This study sheds light on the future design of electrolytes with high ionic conductivity and easy desolvation at low temperatures for rechargeable batteries.
基金supported by the National Natural Science Foundation of China(52002297)National Key R&D Program of China(2022VFB2404800)+1 种基金Wuhan Yellow Crane Talents Program,China Postdoctoral Science Foundation(No.2024M752495)the Postdoctoral Fellowship Program of CPSF(No.GZB20230552).
文摘Aqueous alkali metal-ion batteries(AAMIBs)have been recognized as emerging electrochemical energy storage technologies for grid-scale applications owning to their intrinsic safety,cost-effectiveness,and environmental sustainability.However,the practical application of AAMIBs is still severely constrained by the tendency of aqueous electrolytes to freeze at low temperatures and decompose at high temperatures,limiting their operational temperature range.Considering the urgent need for energy systems with higher adaptability and resilience at various application scenarios,designing novel electrolytes via structure modulation has increasingly emerged as a feasible and economical strategy for the performance optimization of wide-temperature AAMIBs.In this review,the latest advancement of wide-temperature electrolytes for AAMIBs is systematically and comprehensively summarized.Specifically,the key challenges,failure mechanisms,correlations between hydrogen bond behaviors and physicochemical properties,and thermodynamic and kinetic interpretations in aqueous electrolytes are discussed firstly.Additionally,we offer forward-looking insights and innovative design principles for developing aqueous electrolytes capable of operating across a broad temperature range.This review is expected to provide some guidance and reference for the rational design and regulation of widetemperature electrolytes for AAMIBs and promote their future development.
基金supported by the Natural Science Foundation of China(Nos.52125202,52202100,and U24A2065)the Natural Science Foundation of Jiangsu Province(BK20243016)Fundamental Research Funds for the Central Universities,China Postdoctoral Science Foundation(No.2024T171166).
文摘Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density.However,their practical commercialization is hindered by critical challenges on the anode side,including dendrite growth and parasitic reactions at the anode/electrolyte interface.Recent studies highlight that rational electrolyte structure engineering offers an effective route to mitigate these issues and strengthen the electrochemical performance of the zinc metal anode.In this review,we systematically summarize state-of-the-art strategies for electrolyte optimization,with a particular focus on the zinc salts regulation,electrolyte additives,and the construction of novel electrolytes,while elucidating the underlying design principles.We further discuss the key structure–property relationships governing electrolyte behavior to provide guidance for the development of next-generation electrolytes.Finally,future perspectives on advanced electrolyte design are proposed.This review aims to serve as a comprehensive reference for researchers exploring high-performance electrolyte engineering in AZIBs.
基金financially supported by the National Natural Science Foundation of China(No.22309067)the Open Project Program of the State Key Laboratory of Materials-Oriented Chemical Engineering,China(No.KL21-05)the Marine Equipment and Technology Institute,Jiangsu University of Science and Technology,China(No.XTCX202404)。
文摘This study focused on improving the cathode performance of Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.15)O_(3-δ)(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.1)Mo_(0.05)O_(3-δ)(B S CNM_(0.05)),Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.05)Mo_(0.1)O_(3-δ)(BSCNM_(0.1)),and Ba_(0.6)Sr_(0.4)Co_(0.85)Mo_(0.15)O_(3-δ)(BSCM)—with Mo doping contents of 5mol%,10mol%,and15mol%,respectively,were successfully prepared using the sol-gel method.The effects of Mo doping on the crystal structure,conductivity,thermal expansion coefficient,oxygen reduction reaction(ORR)activity,and electrochemical performance were systematically evaluated using X-ray diffraction analysis,thermally induced characterization,electrochemical impedance spectroscopy,and single-cell performance tests.The results revealed that Mo doping could improve the conductivity of the materials,suppress their thermal expansion effects,and significantly improve the electrochemical performance.Surface chemical state analysis using X-ray photoelectron spectroscopy revealed that 5mol%Mo doping could facilitate a high adsorbed oxygen concentration leading to enhanced ORR activity in the materials.Density functional theory calculations confirmed that Mo doping promoted the ORR activity in the materials.At an operating temperature of 600℃,the BSCNM_(0.05)cathode material exhibited significantly enhanced electrochemical impedance characteristics,with a reduced area specific resistance of 0.048Ω·cm~2,which was lower than that of the undoped BSCN matrix material by 32.39%.At the same operating temperature,an anode-supported single cell using a BSCNM_(0.05)cathode achieved a peak power density of 1477 mW·cm^(-2),which was 30.71%,56.30%,and 171.50%higher than those of BSCN,BSCNM_(0.1),and B SCM,respectively.The improved ORR activity and electrochemical performance of BSCNM_(0.05)indicate that it can be used as a cathode material in low-temperature solid oxide fuel cells.
基金supported by the National Natural Science Foundation of China(32501592,32271814,32301530,32471806)Young Elite Scientist Sponsorship Program by Cast(No.YESS20230242)+3 种基金Natural Science Foundation of Tianjin(23JCZDJC00630,24JCZDJC00630)the China Postdoctoral Science Foundation(2023M740563)Tianjin Enterprise Technology Commissioner Project(25YDTPJC00690)China Scholarship Council(202408120091,202408120105).
文摘The pursuit of high energy density and sustainable energy storage devices has been the target of many researchers.However,safety issues such as the susceptibility of conventional liquid electrolytes to leakage and flammability,as well as performance degradation due to uncontrollable dendrite growth in liquid electrolytes,have been limiting the further development of energy storage devices.In this regard,gel polymer electrolytes(GPEs)based on lignocellulosic(cellulose,hemicellulose,lignin)have attracted great interest due to their high thermal stability,excellent electrolyte wettability,and natural abundance.Therefore,in this critical review,a comprehensive overview of the current challenges faced by GPEs is presented,followed by a detailed description of the opportunities and advantages of lignocellulosic materials for the fabrication of GPEs for energy storage devices.Notably,the key properties and corresponding construction strategies of GPEs for energy storage are analyzed and discussed from the perspective of lignocellulose for the first time.Moreover,the future challenges and prospects of lignocellulose-mediated GPEs in energy storage applications are also critically reviewed and discussed.We sincerely hope this review will stimulate further research on lignocellulose-mediated GPEs in energy storage and provide meaningful directions for the strategy of designing advanced GPEs.
基金financially supported by Shenzhen Science and Technology Program(JCYJ20240813142900001)Guangdong Provincial Key Laboratory of New Energy Materials Service Safety。
文摘Chloride-based solid electrolytes are considered promising candidates for next-generation high-energy-density all-solid-state batteries(ASSBs).However,their relatively low oxidative decomposition threshold(~4.2 V vs.Li^(+)/Li)constrains their use in ultrahighvoltage systems(e.g.,4.8 V).In this work,ferroelectric Ba TiO_(3)(BTO)nanoparticles with optimized thickness of~50-100 nm were successfully coated onto Li_(2.5)Y_(0.5)Zr_(0.5)Cl_(6)(LYZC@5BTO)electrolytes using a time-efficient ball-milling process.The nanoparticle-induced interfacial ionic conduction enhancement mechanism contributed to the preservation of LYZC’s high ionic conductivity,which remained at 1.06 m S cm^(-1)for LYZC@5BTO.Furthermore,this surface electric field engineering strategy effectively mitigates the voltage-induced self-decomposition of chloride-based solid electrolytes,suppresses parasitic interfacial reactions with single-crystal NCM811(SCNCM811),and inhibits the irreversible phase transition of SCNCM811.Consequently,the cycling stability of LYZC under high-voltage conditions(4.8 V vs.Li+/Li)is significantly improved.Specifically,ASSB cells employing LYZC@5BTO exhibited a superior discharge capacity of 95.4 m Ah g^(-1)over 200 cycles at 1 C,way outperforming cell using pristine LYZC that only shows a capacity of 55.4 m Ah g^(-1).Furthermore,time-of-flight secondary ion mass spectrometry and X-ray photoelectron spectroscopy analysis revealed that Metal-O-Cl by-products from cumulative interfacial side reactions accounted for 6% of the surface species initially,rising to 26% after 200 cycles in pristine LYZC.In contrast,LYZC@5BTO limited this increase to only 14%,confirming the effectiveness of BTO in stabilizing the interfacial chemistry.This electric field modulation strategy offers a promising route toward the commercialization of high-voltage solid-state electrolytes and energy-dense ASSBs.
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the financial support from the Brazilian funding agencies CNPq(310544/2019-0),FAPESP(2014/02163-7&2017/11958-1)FAPEMIG(Financial support for the LMMA/UFVJM Laboratory)and CNPq(PQ-2 grant:Process 301095/2018-3)the support from Shell and the strategic importance of the support given by ANP(Brazil’s National Oil,Natural Gas,and Biofuels Agency)through the R&D levy regulation。
文摘Supercapacitors(SCs) are high-power energy storage devices with ultra-fast charge/discharge properties.SCs using concentrated aqueous-based electrolytes can work at low temperatures due to their intrinsic properties, such as higher freezing point depression(FPD) and robustness. Besides the traditional organic-and aqueous-based(salt-in-water) electrolytes used in SCs, water-in-salt(WISE) sodium perchlorate electrolytes offer high FPD, non-flammability, and low-toxicity conditions, allowing the fabrication of safer, environmentally friendly, and more robust devices. For the first time, this work reports a comprehensive study regarding WISE system’s charge-storage capabilities and physicochemical properties under low-temperature conditions(T < 0 ℃) using mesoporous carbon-based electrodes. The effect of temperature reduction on the electrolyte viscosity and electrical properties was investigated using different techniques and the in-situ(or operando) Raman spectroscopy under dynamic polarization conditions.The cell voltage, equivalent series resistance, and specific capacitance were investigated as a function of the temperature. The cell voltage(U) increased ~ 50%, while the specific capacitance decreased ~20%when the temperature was reduced from 25 ℃ to -10 ℃. As a result, the maximum specific energy(E = CU^(2)/2) increased ~ 100%. Therefore, low-temperature WISEs are promising candidates to improve the energy-storage characteristics in SCs.
文摘This work reviews technologies that can be used to develop low-temperature solid oxide cells(LT-SOCs)and can be applied in fuel cells and electrolyzers operating at temperatures below 500℃,thus providing a more cost-effective alternative than conventional high-temperature SOCs.Two routes showing potential to reduce the operating temperature of SOCs to below 500℃ are discussed.The first route is the principal way to enhance cell performance,namely,structure optimization.This technique includes the reduction of electrolyte thickness to the nanometer scale and the exploration of electrode structure with low polarization resistance.The other route is the development of novel protonconducting electrolyte materials,which is in the frontier of SOCs study.The fundamentals of proton conduction and the design principles of commonly used electrolyte materials are briefly explained.The most widely studied electrolyte materials for LT-SOCs,namely,perovskitetype BaCeO_(3) -and BaZrO_(3) -based oxides,and the effect of doping on the physical-chemical properties of these oxide materials are summarized.
基金funding support from the National Natural Science Foundation of China(52261135631,52103335)。
文摘With the increasing demand and striking upsurge in the price of lithium carbonate,sodium-ion batteries(SIBs)have gained significant attentions due to their abundance over lithium-ion batteries(LIBs).Some prototype SIBs have achieved great progress in terms of energy densities.Although SIBs show a relatively higher tolerance at the low temperature than LIBs due to the weaker cation–solvent interaction,the low-temperature performance of SIBs remains a critical challenge restricted by the electrolyte solidification and sluggish interphasial kinetics.In this review,we briefly cover the latest research progress in usable low-temperature electrolytes for SIBs.In the meantime,the mitigating mechanism and low-temperature performance of the electrolytes in different SIB configurations are also discussed.The merits and demerits of ether-based and carbonate-based electrolytes are compared to demonstrate their potential and limitations,thus providing application principles for ether-based and carbonate-based electrolytes at low temperatures to maximize their advantages.Furthermore,mitigation strategies for lowtemperature electrolytes are emphasized to guide the future electrolyte design.Finally,we provide some perspectives on the development of the low-temperature electrolytes for SIBs.
基金Project supported by the Natural Science Foundation of Shandong Province,China(Grant Nos.ZR2016FB16,ZR2015AQ010,and ZR2016AQ08)the Shandong University of Technology at Zibo and Zibo City Integration Development Project,China(Grant No.2016ZBXC205)
文摘In the present study,high-quality apatite-type La9.33Ge6O26 powders are successfully synthesized by a facile moltensalt synthesis method（MSSM） at low temperatures,using Li Cl,Li Cl/Na Cl mixture（mass ratio 1：1） as molten salt,respectively.Experimental results indicate that the optimal mass ratio between reactant and molten salt is 1：2,and Li Cl/Na Cl mixed molten-salt is more beneficial for forming high-quality La9.33Ge6O26 powders than Li Cl individual molten-salt.Comparing with the conventional solid-state reaction method（SSRM）,the synthesis temperature of apatitetype La9.33Ge6O26 powders using the MSSM decreases more than 350℃,which can effectively avoid Ge loss in the preparation process of precursor powders.Furthermore,the powders obtained by the MSSM are homogeneous,nonagglomerated and well crystallized,which are very favorable for gaining dense pellets in the premise of avoiding Ge loss.On the basis of high-quality precursor powders,the dense and pure ceramic pellets of La（9.33）Ge6O（26） are gained at a low temperature of 1100℃ for 2 h,which exhibit higher conductivities（σ850℃（Li Cl）= 2.3 × 10^-2 S·cm^-1,σ850 ℃（Li Cl/Na Cl） = 4.9 × 10^-2 S·cm^-1） and lower activation energies（Ea（Li Cl）= 1.02 e V,Ea（Li Cl/Na Cl）= 0.99 e V） than that synthesized by the SSRM.
基金the National Natural Science Foundation of China (NSFC 50571072)
文摘The effect of KOH electrolyte concentration on low-temperature electrochemical properties of LaNi5 alloy electrodes at 233 K was studied. The results indicated that the electrolyte concentration had great influence on discharge capacity and discharge voltage plateau of LaNi5 alloy electrode at 233 K, and the highest discharge capacity and discharge voltage plateau were both obtained at 6 mol/L KOH. When the KOH electrolyte concentration changed from 5 to 9 mol/L at 233 K, the high rate discharge ability （HRD） had the same change tendency as the diffusion coefficient, but the exchange current density did not change significantly, which implied that hydrogen diffusion was the control step at low temperature 233 K for discharge process of LaNi5 alloy electrode.
基金National Key Research and Development Program of China,Grant/Award Number:2022YFB2404800National Natural Science Foundation of China,Grant/Award Numbers:22008082,U1966214。
文摘Lithium-ion batteries(LIBs)have monopolized energy storage markets in modern society.The reliable operation of LIBs at cold condition(<0°C),nevertheless,is inevitably hampered by the sluggish kinetics and parasite reactions,which falls behind the increasing demands for portable electronics and electric vehicles.The electrolyte controls both Li+transport and interfacial reaction,dictating the low-temperature performance substantially.Therefore,the rational formulation of electrolytes is significant for realizing superior lowtemperature performance and broadening application niches of LIBs.Herein,we first discuss the kinetic limitations of low-temperature LIBs,highlighting the importance of electrolyte structure and interfacial chemistry.Then,the advancements for formulating subzero-temperature electrolyte are summarized with in-depth discussions about electrolyte formulation,solvation structure,interfacial chemistry,and low-temperature behaviors.Moreover,some opportunities for lithium metal batteries and the corresponding lowtemperature electrolyte are covered.Finally,the major challenges and future perspectives are outlined for low-temperature LIBs.
基金supported by the National Natural Science Foundation of China(52174247 and 22302066)“Hejian”Innovative Talent Project of Hunan Province(No.2022RC1088)+1 种基金the Hunan Provincial Natural Science Foundation(2023JJ40255)the Scientific Research Foundation of Hunan Provincial Education(22B0599 and 23A0442)。
文摘Hydrogel electrolytes hold great potential in flexible zinc ion supercapacitors(ZICs)due to their high conductivity,good safety,and flexibility.However,freezing of electrolytes at low temperature(subzero)leads to drastic reduction in ionic conductivity and mechanical properties that deteriorates the performance of flexible ZICs.Besides,the mechanical fracture during arbitrary deformations significantly prunes out the lifespan of the flexible device.Herein,a Zn^(2+)and Li^(+)co-doped,polypyrrole-dopamine decorated Sb_(2)S_(3)incorporated,and polyvinyl alcohol/poly(N-(2-hydroxyethyl)acrylamide)double-network hydrogel electrolyte is constructed with favorable mechanical reliability,anti-freezing,and self-healing ability.In addition,it delivers ultra-high ionic conductivity of 8.6 and 3.7 S m^(-1)at 20 and−30°C,respectively,and displays excellent mechanical properties to withstand tensile stress of 1.85 MPa with tensile elongation of 760%,together with fracture energy of 5.14 MJ m^(-3).Notably,the fractured hydrogel electrolyte can recover itself after only 90 s of infrared illumination,while regaining 83%of its tensile strain and almost 100%of its ionic conductivity during−30–60°C.Moreover,ZICs coupled with this hydrogel electrolyte not only show a wide voltage window(up to 2 V),but also provide high energy density of 230 Wh kg^(-1)at power density of 500 W kg^(-1)with a capacity retention of 86.7%after 20,000 cycles under 20°C.Furthermore,the ZICs are able to retain excellent capacity even under various mechanical deformation at−30°C.This contribution will open up new insights into design of advanced wearable flexible electronics with environmental adaptability and long-life span.
