A carbonate-based electrolyte containing a self-synthesized trimethylsilyl-benzenesulfonate(TMSBS)multifunctional additive is developed to enhance the all-climate performance of pouch NaNi_(0.33)Fe_(0.33)Mn_(0.33)O_(2...A carbonate-based electrolyte containing a self-synthesized trimethylsilyl-benzenesulfonate(TMSBS)multifunctional additive is developed to enhance the all-climate performance of pouch NaNi_(0.33)Fe_(0.33)Mn_(0.33)O_(2)(NFM)/hard carbon(HC)sodium-ion batteries(SIBs)over a wide range from−30 to 60℃.The pouch cells exhibit an 18.1%increase in capacity retention after 250 cycles at room temperature and an 11.3%increase after 240 cycles at 45℃.The low-temperature discharging of different rates at−30℃and the cycling at−10℃demonstrate the adaptability of TMSBS-containing electrolytes at low temperatures.Compared to traditional commercial electrolytes,this electrolyte can prevent excessive dissolution of interfacial films of two electrodes,purify undesirable substances of electrolyte composition,and optimize electrode interfaces and solvation structure.In addition,based on the gas analysis in the cyclic process at 45℃and the storage at 60℃by employing both in-situ and non-in-situ techniques,it reveals that TMSBS can suppress the side reactions of gas evolution,thereby ensuring the safety of SIBs.This work presents a practical strategy for upgrading commercial SIBs and highlights the importance of rational electrolyte design for practical applications.展开更多
In the investigation of the next-generation battery anode,Li metal has attracted increasing attention owing to its ultrahigh specific capacity and low reduction potential.However,its low columbic efficiency,limited cy...In the investigation of the next-generation battery anode,Li metal has attracted increasing attention owing to its ultrahigh specific capacity and low reduction potential.However,its low columbic efficiency,limited cycling life,and serious safety hazards have hindered the practical application of rechargeable Li metal batteries.Although several strategies have been proposed to enhance the electrochemical performance of Li metal anodes,most are centered around ether-based electrolytes,which are volatile and do not provide a sufficiently large voltage window.Therefore,we aimed to attain stable Li deposition/stripping in a commercial carbonate-based electrolyte.Herein,we have successfully synthesized hydrogen titanate(HTO)nanowire arrays decorated with homogenous Ag nanoparticles(NPs)(Ag@HTO)via simple hydrothermal and silver mirror reactions.The 3 D cross-linked array structure with Ag NPs provides preferable nucleation sites for uniform Li deposition,and most importantly,when assembled with the commercial LiNi_(0.5)Co0.2Mn_(0.3)O_(2) cathode material,the Ag@HTO could maintain a capacity retention ratio of 81.2% at 1 C after 200 cycles,however the pristine Ti foil failed to do so after only 60 cycles.Our research therefore reveals a new way of designing current collectors paired with commercial high voltage cathodes that can create high energy density Li metal batteries.展开更多
Nowadays,lithium-ion capacitors(LICs) have become a type of important electrochemical energy storage devices due to their high power and long cycle life characteristics with fast response time.As one of the essential ...Nowadays,lithium-ion capacitors(LICs) have become a type of important electrochemical energy storage devices due to their high power and long cycle life characteristics with fast response time.As one of the essential components of LICs,the electrolytes not only provide the anions and cations required during charge and discharge processes,but also supply the liquid environment for ions to migrate between anodes and cathodes in LIC cells.It is well accepted that propylene carbonate(PC) cannot be used as a single solvent for Li-ion electrolyte due to the failure to form stable SEI film on graphite surface.In this work,the compatibility of PC-based electrolyte with commercial soft carbon anode and activated carbon cathode has been validated by using the laminated pouch LIC cells.The effects of additives on the electrochemical properties of PC-based LICs have been systematically investigated.Ethylene sulfite(ES) was proved to be an effective additive to promote capacity retention at high C-rate,which is superior to vinylene carbonate and fluoroethylene carbonate.The addition of 5 wt% ES plays an important role in reducing internal resistance,as well as improving electrochemical stability and low-temperature performances.This study is expected to be beneficial to explore robust electrolyte/additive combinations for LICs to reduce the internal resistance and to improve the lowtemperature performances.展开更多
Density functional theory is used to investigate the complexes structures and properties of poly(vinyl ethylene carbonate)(PVEC/LiTFSI)and poly(vinylene carbonate)(PVCA/LiDFOB)electrolytes containing five-membered rin...Density functional theory is used to investigate the complexes structures and properties of poly(vinyl ethylene carbonate)(PVEC/LiTFSI)and poly(vinylene carbonate)(PVCA/LiDFOB)electrolytes containing five-membered ring carbonate groups under the polymer/Li^(+)model and the polymer/lithium salt model.In addition,the calculated and experimental values of the oxidation potentials of the two electrolytes were compared,and the reasons for the differences in the oxidation potentials of the two electrolytes are elucidated.The calculation results show that the PVEC/LiTFSI has more free ion structures and diverse coordination structures compared to PVCA/LiDFOB electrolyte.This provides a reasonable theoretical explanation for its higher ionic conductivity and lower cation mobility number.The PVEC/LiTFSI electrolyte has a lower oxidation potential compared to the PVCA/LiDFOB electrolyte,which is attributed to the proton transfer that occurs during its oxidation.展开更多
With the increasing demand for high energy density energy storage device,Li metal has received intensive attention for its ultrahigh capacity and the lowest redox potential.LiNO_(3)is widely used as electrolyte additi...With the increasing demand for high energy density energy storage device,Li metal has received intensive attention for its ultrahigh capacity and the lowest redox potential.LiNO_(3)is widely used as electrolyte additive for ether electrolyte,which can improve the cycle performance of Li metal anode.Compared to ethers,carbonates are more suitable for Li metal batteries with high voltage cathode because they have a wider electrochemical window.However,LiNO_(3)performs poor solubility in carbonate electrolyte,restricting its application in high voltage Li battery.Herein,we presented a facile method to introduce abundant LiNO_(3)additive to carbonate electrolyte system by introducing LiNO_(3)-PAN es as the interlayer of the cell.LiNO_(3)-PAN es is in sufficient contact with the electrolyte so that it can continuously releases LiNO_(3)to assist the formation of Li_(2)N_(2)O_(2)-rich single nitrogenous component SEI layer on Li surface.With the help of LiNO_(3)-PAN es,Li metal anode shows excellent cycle stability even at a high current density of 4mA/cm^(2),so that the cycle performance of the full cells was significantly improved,whether in the anode-free Cu||LFP cell or the Li||NCM622 cell.展开更多
Ethylene carbonate(EC)is widely used in lithium-ion batteries due to its optimal overall performance with satisfactory conductivity,relatively stable solid electrolyte interphase(SEI),and wide electrochemical window.E...Ethylene carbonate(EC)is widely used in lithium-ion batteries due to its optimal overall performance with satisfactory conductivity,relatively stable solid electrolyte interphase(SEI),and wide electrochemical window.EC is also the most widely used electrolyte solvent in sodium ion batteries.However,compared to lithium metal,sodium metal(Na)shows higher activity and reacts violently with EC-based electrolyte(NaPF_(6)as solute),which leads to the failure of sodium metal batteries(SMBs).Herein,we reveal the electrochemical instability mechanism of EC on sodium metal battery,and find that the com-bination of EC and NaPF_(6) is electrically reduced in sodium metal anode during charging,resulting in the reduction of the first coulombic efficiency,and the continuous consumption of electrolyte leads to the cell failure.To address the above issues,an additive modified linear carbonate-based electrolyte is provided as a substitute for EC based electrolytes.Specifically,ethyl methyl carbonate(EMC)and dimethyl carbon-ate(DMC)as solvents and fluoroethylene carbonate(FEC)as SEI-forming additive have been identified as the optimal solvent for NaFP_(6)based electrolyte and used in Na_(4)Fe_(3)(PO_(4))_(2)(P_(2)O_(7))/Na batteries.The batter-ies exhibit excellent capacity retention rate of about 80%over 1000 cycles at a cut-off voltage of 4.3 V.展开更多
The low lithium transference number of conventional dual-ion polymer electrolytes will lead to concentration polarization and lithium dendrite growth,thereby affecting the safety and cycling performance of lithium bat...The low lithium transference number of conventional dual-ion polymer electrolytes will lead to concentration polarization and lithium dendrite growth,thereby affecting the safety and cycling performance of lithium batteries.Herein,we report a flame-retardant polycarbonate-based single-ion conducting polymer electrolyte(PAGEC-B/PFN).Due to the immobilization of anions within the polycarbonate crosslinking network,PAGEC-B/PFN exhibits a high lithium transference number(0.86),which is beneficial for alleviating concentration polarization and suppressing the growth of lithium dendrite.With the assistance of the TEP flame retardant and FEC,as well as LiNO_(3) additives,PAGEC-B/PFN exhibits excellent flame retardancy,high ionic conductivity,and outstanding interfacial compatibility with the lithium metal anode.As expected,PAGEC-B/PFN achieves a high critical current density of up to 2.0 mA cm^(-2)and stable cycling of Li‖Li cell for over 2200 h.Meanwhile,LFP‖PAGEC-B/PFN‖Li cell delivers a specific capacity of 147.8 mA h g^(-1)at 0.5 C and exhibits excellent cycling performance over 600 cycles.This work provides a strategy for designing solid-state lithium batteries with high safety and high performance.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
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
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
Halide solid-state electrolytes have gained significant attention in recent years due to their high ionic conductivity,making them promising candidates for future all-solid-state batteries.Recent studies have identifi...Halide solid-state electrolytes have gained significant attention in recent years due to their high ionic conductivity,making them promising candidates for future all-solid-state batteries.Recent studies have identified numerous crystal structures with the Li_(3)MX_(6)composition,although many remain unexplored across various chemical systems.In this research,we developed a comprehensive method to examine all conceivable space groups and structures within theLi-M-X system,where M includes In,Ga,and La,and X includes F,Cl,Br,and 1.Our findings revealed two metastable structures:Li_(3)InF_(6)with P3c1 symmetry and Li_(3)InI_(6)with C2/c symmetry,exhibiting ionic conductivities of 0.55 and 2.18mS/cm at 300K,respectively.Notably,the trigonal symmetry of Li3InF6 demonstrates that high ionic conductivities are not limited to monoclinic structures but can also be achieved with trigonal symmetries.The electrochemical stability windows,mechanical properties,and reaction energies of these materials with known cathodes suggest their potential for use in all-solid-state batteries.Additionally,we predicted the stability of novel materials,including Li_(5)InCl_(9),Li_(5)InBr_(9),Li_(5)InI_(8),LiIn_(2)Cl_(9),LiIn_(2)Br_(9),and LiIn_(2)Ig_(9).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
Lithium-mediated nitrogen reduction reaction(LMNRR)is a promising route for sustainable ammonia synthesis,but the generation of excessive solid electrolyte interphase(SEI)severely limits its efficiency.Here,we tackle ...Lithium-mediated nitrogen reduction reaction(LMNRR)is a promising route for sustainable ammonia synthesis,but the generation of excessive solid electrolyte interphase(SEI)severely limits its efficiency.Here,we tackle this challenge by introducing n-hexane as an electrolyte additive to weaken LiClO4 ionization,achieving minimized dissociation via squeezed solvation shells with compact ion pairs.Molecular dynamics simulations and experimental characterizations reveal that n-hexane enriches anion coordination around Li+,endowing the electrolyte with robust anti-reduction capability.This suppresses SEI overgrowth,reduces interfacial resistance,and accelerates N2 diffusion.Consequently,a thinner,inorganic-rich SEI is formed,enabling high nitrogen flux and rapid active Li3N generation kinetics.Consequently,the proof-of-concept system achieves unprecedentedly high Faradaic efficiency of 53.8%±8.2%at 10 mA cm^(−2)and NH3 yield rate of 88.57±9.5 nmol s^(−1)cm^(−2)under ambient conditions,making a giant step further toward industrializing the electrochemical ammonia production.展开更多
With the global push for energy conservation and the rapid development of low-power,flexible and wearable optical displays,the demand for electrochromic technology has surged.Gel polymer electrolytes(GPEs),a crucial c...With the global push for energy conservation and the rapid development of low-power,flexible and wearable optical displays,the demand for electrochromic technology has surged.Gel polymer electrolytes(GPEs),a crucial component of electrochromic devices(ECDs),show great promise in applications.This is attributed to their efficient ion-transport capabilities,excellent mechanical properties and strong adhesion.All of these characteristics are conducive to enhancing the safety of the devices,streamlining the packaging process,significantly improving the electrochromic performance of ECDs and boosting their commercial application potential.This review provides a comprehensive overview of GPEs for ECDs,focusing on their basic designs,functional modifications and practical applications.Firstly,this review outlines the fundamental design of GPEs for ECDs,encompassing key performance index,classification,gelation mechanism and preparation methods.Building on this foundation,it provides an in-depth discussion of functionalized GPEs developed to enhance device performance or expand functionality,including electrochromic,temperature-responsive,photo-responsive and stretchable self-healing GPE.Furthermore,the integration of GPEs into various ECD applications,including smart windows,displays,energy storage devices and wearable electronic,are summarized to highlight the advantages that the design of GPEs brings to the practical application of ECDs.Finally,based on the summary of GPEs employed for ECDs,the challenges and development expectations in this direction were indicated.展开更多
With the escalating demand for safe,sustainable,and high-performance energy storage systems,hydrogel electrolytes have emerged as promising alternatives to conventional liquid electrolytes in zinc-ion batteries.By int...With the escalating demand for safe,sustainable,and high-performance energy storage systems,hydrogel electrolytes have emerged as promising alternatives to conventional liquid electrolytes in zinc-ion batteries.By integrating the high ionic conductivity of liquid electrolytes with the mechanical robustness of solid frameworks,hydrogel electrolytes offer distinct advantages in suppressing zinc dendrite formation,enhancing interfacial stability,and enabling reliable operation under extreme environmental conditions.This review systematically summarizes the fundamental characteristics and design criteria of hydrogel electrolytes,including mechanical flexibility,ionic transport capabilities,and environmental adaptability.It further explores various compositional design strategies involving natural polymers,synthetic polymers,and composite systems,as well as the incorporation of electrolyte salts and functional additives.In addition,recent advances in functional optimization,such as anti-freezing properties,self-healing abilities,thermal responsiveness,and biocompatibility,are comprehensively discussed.Finally,the review outlines the current challenges and proposes potential directions for future research.展开更多
Succinonitrile(SN)-based polymer plastic crystal electrolytes(PPCEs)are regarded as promising candidates for lithium metal batteries but suffer from serious side reactions with Li metal.Herein,we propose a multi-dimen...Succinonitrile(SN)-based polymer plastic crystal electrolytes(PPCEs)are regarded as promising candidates for lithium metal batteries but suffer from serious side reactions with Li metal.Herein,we propose a multi-dimensional optimization strategy to alleviate the side reactions between SN and Li metal,and develop a highly stable poly-vinylethylene carbonate-based PPCE(PPCE-VEC).Moreover,we identify the intrinsic factors of multi-dimensional polymer structures on the electrolyte stability by three typical classes of polyesters.The PPCE-VEC constructed by in situ polymerization exhibits much better stability than poly-vinylene carbonate-based PPCE(PPCE-VCA)and poly-trifluoroethyl acrylate-based PPCE(PPCE-TFA),which is verified by its fewer SN-decomposition species in X-ray photoelectron spectroscopy(XPS)and outstanding full cell performance.The PPCE-VEC-enabled LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)full cell achieve 73.7%capacity retention after 1400 cycles,which outperforms PPCE-VCA-and PPCE-TFA-enabled full cells(61.9%and 46.9%).Spectral analysis and theoretical calculation reveal that the high solvation ability of the carbonyl site,flexible polymer chain,and homogeneous electrolyte phase of PPCE-VEC are favorable to maximizing competition coordination with Li^(+)to weaken the Li^(+)–SN binding and shape an anion-rich solvation structure.This optimized polymer-involved Li^(+)solvation enhances SN stability and facilitates the formation of B/F enriched solid-electrolyte interphase(SEI),thus significantly improving PPCE stability.展开更多
Aqueous zinc-ion batteries(AZIBs)hold great promise for next-generation energy storage but face challenges such as Zn dendrite growth,side reactions,and limited performance at low temperatures.Here,we propose an elect...Aqueous zinc-ion batteries(AZIBs)hold great promise for next-generation energy storage but face challenges such as Zn dendrite growth,side reactions,and limited performance at low temperatures.Here,we propose an electrolyte design strategy that reconstructs the hydrogenbond network through the synergistic effect of glycerol(GL)and methylsulfonamide(MSA),enabling the formation of a(100)-oriented Zn anode.This design significantly broadens the operating current and temperature windows of AZIBs.As a result,Zn||Zn symmetric cells exhibit remarkable cycling stability,achieving 4,000 h at 1 mA cm^(-2)and 600 h at 40 mA cm^(-2)(both at 1 mAh cm^(-2)capacity);even at-20℃,Zn||Zn symmetric cells deliver ultra-stable cycling for over 5,400 h.Furthermore,Zn||VO_(2)full cells retain 77.3%of their capacity after 2,000 cycles at 30°C with a current density of 0.5 A g^(-1)and 85.4%capacity retention after 2,000 cycles at-20°C and 0.25 A g^(-1).These results demonstrate a robust pathway for enhancing the practicality and low-temperature adaptability of AZIBs.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
In the realm of large-scale power system energy storage,sodium-based batteries represent a cost-effective post-lithium energy storage technology,making inorganic solid-state sodium batteries(ISSSB)a critical branch of...In the realm of large-scale power system energy storage,sodium-based batteries represent a cost-effective post-lithium energy storage technology,making inorganic solid-state sodium batteries(ISSSB)a critical branch of this development.Inorganic solid-state electrolytes(ISSEs)are the core components of sodium batteries;however,they face significant challenges such as insufficient ionic conductivity,interfacial instability,and dendrite growth,all of which severely hinder practical application.This review critically assesses experimental protocols and theoretical frameworks related to mainstream ISSEs and systematizes optimization strategies aimed at overcoming these challenges.Leveraging integrated insights from both experimental and computational studies,the review first categorizes and summarizes the primary types of ISSEs,namely oxide-,sulfide-,and halide-based electrolytes.It then details interfacial optimization strategies focused on addressing three core interfacial issues:ion transport barriers resulting from mechanical incompatibility,side reactions stemming from electrochemical mismatch,and dendrite formation.Finally,the review advocates prioritizing in-depth research that integrates experimental and theoretical approaches to establish a closed-loop methodology encompassing predictive design,multiscale investigation,mechanistic exploration,and high-throughput automated experimentation,with feedback-driven refinement.This work serves as a comprehensive reference and systematic roadmap for future research on solid-state electrolytes(SSEs).展开更多
The low ionic conductivity and poor mechanical strength of polyethylene oxide(PEO)-based electrolytes severely restrict their practical application.To address this problem,this work designs a scalable,high-strength(24...The low ionic conductivity and poor mechanical strength of polyethylene oxide(PEO)-based electrolytes severely restrict their practical application.To address this problem,this work designs a scalable,high-strength(24.3 MPa)bicontinuous porous poly(m-phthaloyl-m-phenylenediamine)(PMIA)membrane integrated into PEO/LiTFSI(PL),thus forming a PMIA/PEO/LiTFSI(PPL)composite electrolyte.Compared to the PL electrolyte,the PPL electrolyte reinforced by a bicontinuous porous PMIA membrane exhibits significantly enhanced mechanical strength,reaching 13.4 MPa.In addition,the amide groups on PMIA strongly coordinate with LiTFSI and form hydrogen bonds with PEO,promoting Li salt dissociation and reducing the Li^(+)migration barrier.This creates efficient,fast Li^(+)transport channels at the PMIA/PL interfaces,effectively promoting the uniform Li^(+)deposition and minimizing lithium dendrite formation.The PPL electrolyte achieves high ionic conductivity(1×10^(−4)S cm^(−1)at 30°C)and Li^(+)transference number(tLi^(+)=0.43).The assembled LiFePO_(4)/Li battery demonstrates excellent cycling stability,retaining 80%capacity after 2000 cycles at 2 C,while the Li/Li symmetric cell operates stably for over 900 h at 0.3 mA cm^(−2).Therefore,the scalable porous PMIA membrane effectively enhances both the mechanical strength and Li^(+)transport in PEO-based electrolytes,offering a viable strategy for their commercial-scale implementation.展开更多
基金supported by the Scientific Research Innovation Project of Graduate School of South China Normal University。
文摘A carbonate-based electrolyte containing a self-synthesized trimethylsilyl-benzenesulfonate(TMSBS)multifunctional additive is developed to enhance the all-climate performance of pouch NaNi_(0.33)Fe_(0.33)Mn_(0.33)O_(2)(NFM)/hard carbon(HC)sodium-ion batteries(SIBs)over a wide range from−30 to 60℃.The pouch cells exhibit an 18.1%increase in capacity retention after 250 cycles at room temperature and an 11.3%increase after 240 cycles at 45℃.The low-temperature discharging of different rates at−30℃and the cycling at−10℃demonstrate the adaptability of TMSBS-containing electrolytes at low temperatures.Compared to traditional commercial electrolytes,this electrolyte can prevent excessive dissolution of interfacial films of two electrodes,purify undesirable substances of electrolyte composition,and optimize electrode interfaces and solvation structure.In addition,based on the gas analysis in the cyclic process at 45℃and the storage at 60℃by employing both in-situ and non-in-situ techniques,it reveals that TMSBS can suppress the side reactions of gas evolution,thereby ensuring the safety of SIBs.This work presents a practical strategy for upgrading commercial SIBs and highlights the importance of rational electrolyte design for practical applications.
基金supported by the National Natural Science Foundation of China(Nos.2127318,21621091,and 21875195)the National Key Research and Development Program of China(No.2017YFB0102000)the Fundamental Research Funds for the Central Universities(No.20720190040)。
文摘In the investigation of the next-generation battery anode,Li metal has attracted increasing attention owing to its ultrahigh specific capacity and low reduction potential.However,its low columbic efficiency,limited cycling life,and serious safety hazards have hindered the practical application of rechargeable Li metal batteries.Although several strategies have been proposed to enhance the electrochemical performance of Li metal anodes,most are centered around ether-based electrolytes,which are volatile and do not provide a sufficiently large voltage window.Therefore,we aimed to attain stable Li deposition/stripping in a commercial carbonate-based electrolyte.Herein,we have successfully synthesized hydrogen titanate(HTO)nanowire arrays decorated with homogenous Ag nanoparticles(NPs)(Ag@HTO)via simple hydrothermal and silver mirror reactions.The 3 D cross-linked array structure with Ag NPs provides preferable nucleation sites for uniform Li deposition,and most importantly,when assembled with the commercial LiNi_(0.5)Co0.2Mn_(0.3)O_(2) cathode material,the Ag@HTO could maintain a capacity retention ratio of 81.2% at 1 C after 200 cycles,however the pristine Ti foil failed to do so after only 60 cycles.Our research therefore reveals a new way of designing current collectors paired with commercial high voltage cathodes that can create high energy density Li metal batteries.
基金the National Natural Science Foundation of China(Nos.52077207,51822706,51777200 and 51772127)Beijing Natural Science Foundation(No.JQ19012)Dalian National Laboratory for Clean Energy Cooperation Fund,the CAS(No.DNL201912)。
文摘Nowadays,lithium-ion capacitors(LICs) have become a type of important electrochemical energy storage devices due to their high power and long cycle life characteristics with fast response time.As one of the essential components of LICs,the electrolytes not only provide the anions and cations required during charge and discharge processes,but also supply the liquid environment for ions to migrate between anodes and cathodes in LIC cells.It is well accepted that propylene carbonate(PC) cannot be used as a single solvent for Li-ion electrolyte due to the failure to form stable SEI film on graphite surface.In this work,the compatibility of PC-based electrolyte with commercial soft carbon anode and activated carbon cathode has been validated by using the laminated pouch LIC cells.The effects of additives on the electrochemical properties of PC-based LICs have been systematically investigated.Ethylene sulfite(ES) was proved to be an effective additive to promote capacity retention at high C-rate,which is superior to vinylene carbonate and fluoroethylene carbonate.The addition of 5 wt% ES plays an important role in reducing internal resistance,as well as improving electrochemical stability and low-temperature performances.This study is expected to be beneficial to explore robust electrolyte/additive combinations for LICs to reduce the internal resistance and to improve the lowtemperature performances.
文摘Density functional theory is used to investigate the complexes structures and properties of poly(vinyl ethylene carbonate)(PVEC/LiTFSI)and poly(vinylene carbonate)(PVCA/LiDFOB)electrolytes containing five-membered ring carbonate groups under the polymer/Li^(+)model and the polymer/lithium salt model.In addition,the calculated and experimental values of the oxidation potentials of the two electrolytes were compared,and the reasons for the differences in the oxidation potentials of the two electrolytes are elucidated.The calculation results show that the PVEC/LiTFSI has more free ion structures and diverse coordination structures compared to PVCA/LiDFOB electrolyte.This provides a reasonable theoretical explanation for its higher ionic conductivity and lower cation mobility number.The PVEC/LiTFSI electrolyte has a lower oxidation potential compared to the PVCA/LiDFOB electrolyte,which is attributed to the proton transfer that occurs during its oxidation.
基金supported by the National Key R&D Program of China(No.2022YFB2402600)National Natural Science Foundation of China(No.22279166)+1 种基金Basic and Applied Basic Research Foundation of Guangdong Province-Regional joint fund project(No.2022B1515120019)the Fundamental Research Funds for the Central Universities,Sun Yat-Sen University(Nos.22qntd0101 and 22dfx01).
文摘With the increasing demand for high energy density energy storage device,Li metal has received intensive attention for its ultrahigh capacity and the lowest redox potential.LiNO_(3)is widely used as electrolyte additive for ether electrolyte,which can improve the cycle performance of Li metal anode.Compared to ethers,carbonates are more suitable for Li metal batteries with high voltage cathode because they have a wider electrochemical window.However,LiNO_(3)performs poor solubility in carbonate electrolyte,restricting its application in high voltage Li battery.Herein,we presented a facile method to introduce abundant LiNO_(3)additive to carbonate electrolyte system by introducing LiNO_(3)-PAN es as the interlayer of the cell.LiNO_(3)-PAN es is in sufficient contact with the electrolyte so that it can continuously releases LiNO_(3)to assist the formation of Li_(2)N_(2)O_(2)-rich single nitrogenous component SEI layer on Li surface.With the help of LiNO_(3)-PAN es,Li metal anode shows excellent cycle stability even at a high current density of 4mA/cm^(2),so that the cycle performance of the full cells was significantly improved,whether in the anode-free Cu||LFP cell or the Li||NCM622 cell.
基金supported by the National Natural Science Foundation of China(52172201,51732005,51902118,and 52102249)the China Postdoctoral Science Foundation(2019M662609and 2020T130217)for financial support。
文摘Ethylene carbonate(EC)is widely used in lithium-ion batteries due to its optimal overall performance with satisfactory conductivity,relatively stable solid electrolyte interphase(SEI),and wide electrochemical window.EC is also the most widely used electrolyte solvent in sodium ion batteries.However,compared to lithium metal,sodium metal(Na)shows higher activity and reacts violently with EC-based electrolyte(NaPF_(6)as solute),which leads to the failure of sodium metal batteries(SMBs).Herein,we reveal the electrochemical instability mechanism of EC on sodium metal battery,and find that the com-bination of EC and NaPF_(6) is electrically reduced in sodium metal anode during charging,resulting in the reduction of the first coulombic efficiency,and the continuous consumption of electrolyte leads to the cell failure.To address the above issues,an additive modified linear carbonate-based electrolyte is provided as a substitute for EC based electrolytes.Specifically,ethyl methyl carbonate(EMC)and dimethyl carbon-ate(DMC)as solvents and fluoroethylene carbonate(FEC)as SEI-forming additive have been identified as the optimal solvent for NaFP_(6)based electrolyte and used in Na_(4)Fe_(3)(PO_(4))_(2)(P_(2)O_(7))/Na batteries.The batter-ies exhibit excellent capacity retention rate of about 80%over 1000 cycles at a cut-off voltage of 4.3 V.
基金supported by the National Natural Science Foundation of China(22179149,22075329,51573215,and 21978332)Guangzhou Municipal Science and Technology Program(2025B01J2007,2025A03J4025,2025A03J4026)Fundamental Research Fund of Henan Academy of Sciences(232018002)。
文摘The low lithium transference number of conventional dual-ion polymer electrolytes will lead to concentration polarization and lithium dendrite growth,thereby affecting the safety and cycling performance of lithium batteries.Herein,we report a flame-retardant polycarbonate-based single-ion conducting polymer electrolyte(PAGEC-B/PFN).Due to the immobilization of anions within the polycarbonate crosslinking network,PAGEC-B/PFN exhibits a high lithium transference number(0.86),which is beneficial for alleviating concentration polarization and suppressing the growth of lithium dendrite.With the assistance of the TEP flame retardant and FEC,as well as LiNO_(3) additives,PAGEC-B/PFN exhibits excellent flame retardancy,high ionic conductivity,and outstanding interfacial compatibility with the lithium metal anode.As expected,PAGEC-B/PFN achieves a high critical current density of up to 2.0 mA cm^(-2)and stable cycling of Li‖Li cell for over 2200 h.Meanwhile,LFP‖PAGEC-B/PFN‖Li cell delivers a specific capacity of 147.8 mA h g^(-1)at 0.5 C and exhibits excellent cycling performance over 600 cycles.This work provides a strategy for designing solid-state lithium batteries with high safety and high performance.
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 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supported by the Higher Education and Science Committee of Armenia in the frames of the research projects 20TTSG-2F010,23AA-2F033 and ANSEF(EN-matsc-2660)grantConvex hull calculations were done on the Oracle HPC clouds provided by the Oracle for Research grant(16576595)The USPEX calculations were performed on the Armenian National Supercomputing Center(ANSCC).MLIP training and ionic conductivity calculations were performed with the support of the Russian Science。
文摘Halide solid-state electrolytes have gained significant attention in recent years due to their high ionic conductivity,making them promising candidates for future all-solid-state batteries.Recent studies have identified numerous crystal structures with the Li_(3)MX_(6)composition,although many remain unexplored across various chemical systems.In this research,we developed a comprehensive method to examine all conceivable space groups and structures within theLi-M-X system,where M includes In,Ga,and La,and X includes F,Cl,Br,and 1.Our findings revealed two metastable structures:Li_(3)InF_(6)with P3c1 symmetry and Li_(3)InI_(6)with C2/c symmetry,exhibiting ionic conductivities of 0.55 and 2.18mS/cm at 300K,respectively.Notably,the trigonal symmetry of Li3InF6 demonstrates that high ionic conductivities are not limited to monoclinic structures but can also be achieved with trigonal symmetries.The electrochemical stability windows,mechanical properties,and reaction energies of these materials with known cathodes suggest their potential for use in all-solid-state batteries.Additionally,we predicted the stability of novel materials,including Li_(5)InCl_(9),Li_(5)InBr_(9),Li_(5)InI_(8),LiIn_(2)Cl_(9),LiIn_(2)Br_(9),and LiIn_(2)Ig_(9).
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supported by the National Natural Science Foundation of China(Grant No.U21A20332).We also acknowledge support from the Collaborative Innovation Center of Suzhou Nano Science and Technology.
文摘Lithium-mediated nitrogen reduction reaction(LMNRR)is a promising route for sustainable ammonia synthesis,but the generation of excessive solid electrolyte interphase(SEI)severely limits its efficiency.Here,we tackle this challenge by introducing n-hexane as an electrolyte additive to weaken LiClO4 ionization,achieving minimized dissociation via squeezed solvation shells with compact ion pairs.Molecular dynamics simulations and experimental characterizations reveal that n-hexane enriches anion coordination around Li+,endowing the electrolyte with robust anti-reduction capability.This suppresses SEI overgrowth,reduces interfacial resistance,and accelerates N2 diffusion.Consequently,a thinner,inorganic-rich SEI is formed,enabling high nitrogen flux and rapid active Li3N generation kinetics.Consequently,the proof-of-concept system achieves unprecedentedly high Faradaic efficiency of 53.8%±8.2%at 10 mA cm^(−2)and NH3 yield rate of 88.57±9.5 nmol s^(−1)cm^(−2)under ambient conditions,making a giant step further toward industrializing the electrochemical ammonia production.
基金supported by the National Natural Science Foundation of China(52103299)。
文摘With the global push for energy conservation and the rapid development of low-power,flexible and wearable optical displays,the demand for electrochromic technology has surged.Gel polymer electrolytes(GPEs),a crucial component of electrochromic devices(ECDs),show great promise in applications.This is attributed to their efficient ion-transport capabilities,excellent mechanical properties and strong adhesion.All of these characteristics are conducive to enhancing the safety of the devices,streamlining the packaging process,significantly improving the electrochromic performance of ECDs and boosting their commercial application potential.This review provides a comprehensive overview of GPEs for ECDs,focusing on their basic designs,functional modifications and practical applications.Firstly,this review outlines the fundamental design of GPEs for ECDs,encompassing key performance index,classification,gelation mechanism and preparation methods.Building on this foundation,it provides an in-depth discussion of functionalized GPEs developed to enhance device performance or expand functionality,including electrochromic,temperature-responsive,photo-responsive and stretchable self-healing GPE.Furthermore,the integration of GPEs into various ECD applications,including smart windows,displays,energy storage devices and wearable electronic,are summarized to highlight the advantages that the design of GPEs brings to the practical application of ECDs.Finally,based on the summary of GPEs employed for ECDs,the challenges and development expectations in this direction were indicated.
基金financially supported by the Guangdong Major Project of Basic Research(No.2023B0303000002)Shenzhen Science and Technology Plan Project(No.SGDX20230116091644003)+3 种基金Shenzhen Key Laboratory of Advanced Energy Storage(No.ZDSYS20220401141000001)high-level special funds(No.G03034K001)the Guangxi Key Technologies R&D Program(AB23075171,AB25069180)National Natural Science Foundation of China(22265007,52263016)。
文摘With the escalating demand for safe,sustainable,and high-performance energy storage systems,hydrogel electrolytes have emerged as promising alternatives to conventional liquid electrolytes in zinc-ion batteries.By integrating the high ionic conductivity of liquid electrolytes with the mechanical robustness of solid frameworks,hydrogel electrolytes offer distinct advantages in suppressing zinc dendrite formation,enhancing interfacial stability,and enabling reliable operation under extreme environmental conditions.This review systematically summarizes the fundamental characteristics and design criteria of hydrogel electrolytes,including mechanical flexibility,ionic transport capabilities,and environmental adaptability.It further explores various compositional design strategies involving natural polymers,synthetic polymers,and composite systems,as well as the incorporation of electrolyte salts and functional additives.In addition,recent advances in functional optimization,such as anti-freezing properties,self-healing abilities,thermal responsiveness,and biocompatibility,are comprehensively discussed.Finally,the review outlines the current challenges and proposes potential directions for future research.
基金supported by the National Natural Science Foundation of China(22072048)the Guangdong Provincial Department of Science and Technology(2021A1515010128 and 2022A0505050013).
文摘Succinonitrile(SN)-based polymer plastic crystal electrolytes(PPCEs)are regarded as promising candidates for lithium metal batteries but suffer from serious side reactions with Li metal.Herein,we propose a multi-dimensional optimization strategy to alleviate the side reactions between SN and Li metal,and develop a highly stable poly-vinylethylene carbonate-based PPCE(PPCE-VEC).Moreover,we identify the intrinsic factors of multi-dimensional polymer structures on the electrolyte stability by three typical classes of polyesters.The PPCE-VEC constructed by in situ polymerization exhibits much better stability than poly-vinylene carbonate-based PPCE(PPCE-VCA)and poly-trifluoroethyl acrylate-based PPCE(PPCE-TFA),which is verified by its fewer SN-decomposition species in X-ray photoelectron spectroscopy(XPS)and outstanding full cell performance.The PPCE-VEC-enabled LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)full cell achieve 73.7%capacity retention after 1400 cycles,which outperforms PPCE-VCA-and PPCE-TFA-enabled full cells(61.9%and 46.9%).Spectral analysis and theoretical calculation reveal that the high solvation ability of the carbonyl site,flexible polymer chain,and homogeneous electrolyte phase of PPCE-VEC are favorable to maximizing competition coordination with Li^(+)to weaken the Li^(+)–SN binding and shape an anion-rich solvation structure.This optimized polymer-involved Li^(+)solvation enhances SN stability and facilitates the formation of B/F enriched solid-electrolyte interphase(SEI),thus significantly improving PPCE stability.
基金financially supported by Guangdong Major Project of Basic Research(No.2023B0303000002)Shenzhen Fundamental Research Programs(No.JCYJ20241202125404007)+1 种基金Shenzhen Key Laboratory of Advanced Energy Storage(No.ZDSYS20220401141000001)National Natural Science Foundation of China(No.52263016,22265007)。
文摘Aqueous zinc-ion batteries(AZIBs)hold great promise for next-generation energy storage but face challenges such as Zn dendrite growth,side reactions,and limited performance at low temperatures.Here,we propose an electrolyte design strategy that reconstructs the hydrogenbond network through the synergistic effect of glycerol(GL)and methylsulfonamide(MSA),enabling the formation of a(100)-oriented Zn anode.This design significantly broadens the operating current and temperature windows of AZIBs.As a result,Zn||Zn symmetric cells exhibit remarkable cycling stability,achieving 4,000 h at 1 mA cm^(-2)and 600 h at 40 mA cm^(-2)(both at 1 mAh cm^(-2)capacity);even at-20℃,Zn||Zn symmetric cells deliver ultra-stable cycling for over 5,400 h.Furthermore,Zn||VO_(2)full cells retain 77.3%of their capacity after 2,000 cycles at 30°C with a current density of 0.5 A g^(-1)and 85.4%capacity retention after 2,000 cycles at-20°C and 0.25 A g^(-1).These results demonstrate a robust pathway for enhancing the practicality and low-temperature adaptability of AZIBs.
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financial support for this research,from the National Natural Science Foundation of China(52076076,52006065)Fundamental Research Funds for Central Universities(2025JC003)Beijing Municipal Natural Science Foundation(3242022)is gratefully acknowledged.
文摘In the realm of large-scale power system energy storage,sodium-based batteries represent a cost-effective post-lithium energy storage technology,making inorganic solid-state sodium batteries(ISSSB)a critical branch of this development.Inorganic solid-state electrolytes(ISSEs)are the core components of sodium batteries;however,they face significant challenges such as insufficient ionic conductivity,interfacial instability,and dendrite growth,all of which severely hinder practical application.This review critically assesses experimental protocols and theoretical frameworks related to mainstream ISSEs and systematizes optimization strategies aimed at overcoming these challenges.Leveraging integrated insights from both experimental and computational studies,the review first categorizes and summarizes the primary types of ISSEs,namely oxide-,sulfide-,and halide-based electrolytes.It then details interfacial optimization strategies focused on addressing three core interfacial issues:ion transport barriers resulting from mechanical incompatibility,side reactions stemming from electrochemical mismatch,and dendrite formation.Finally,the review advocates prioritizing in-depth research that integrates experimental and theoretical approaches to establish a closed-loop methodology encompassing predictive design,multiscale investigation,mechanistic exploration,and high-throughput automated experimentation,with feedback-driven refinement.This work serves as a comprehensive reference and systematic roadmap for future research on solid-state electrolytes(SSEs).
基金supported by the National Natural Science Foundation of China(52273059,52203066,52403046 and 52473219)the Science and Technology Plans of Tianjin(22JCYBJC01030)+3 种基金the Tianjin Natural Science Foundation(23JCYBJC00660)the Tianjin Enterprise Science and Technology Commissioner Project(23YDTPJC00490)the China Postdoctoral Science Foundation Grant(2023M742135,2024T170525)the State Key Laboratory of Membrane and Membrane Separation,Tiangong University.
文摘The low ionic conductivity and poor mechanical strength of polyethylene oxide(PEO)-based electrolytes severely restrict their practical application.To address this problem,this work designs a scalable,high-strength(24.3 MPa)bicontinuous porous poly(m-phthaloyl-m-phenylenediamine)(PMIA)membrane integrated into PEO/LiTFSI(PL),thus forming a PMIA/PEO/LiTFSI(PPL)composite electrolyte.Compared to the PL electrolyte,the PPL electrolyte reinforced by a bicontinuous porous PMIA membrane exhibits significantly enhanced mechanical strength,reaching 13.4 MPa.In addition,the amide groups on PMIA strongly coordinate with LiTFSI and form hydrogen bonds with PEO,promoting Li salt dissociation and reducing the Li^(+)migration barrier.This creates efficient,fast Li^(+)transport channels at the PMIA/PL interfaces,effectively promoting the uniform Li^(+)deposition and minimizing lithium dendrite formation.The PPL electrolyte achieves high ionic conductivity(1×10^(−4)S cm^(−1)at 30°C)and Li^(+)transference number(tLi^(+)=0.43).The assembled LiFePO_(4)/Li battery demonstrates excellent cycling stability,retaining 80%capacity after 2000 cycles at 2 C,while the Li/Li symmetric cell operates stably for over 900 h at 0.3 mA cm^(−2).Therefore,the scalable porous PMIA membrane effectively enhances both the mechanical strength and Li^(+)transport in PEO-based electrolytes,offering a viable strategy for their commercial-scale implementation.
