The deterioration of aqueous zinc-ion batteries(AZIBs)is confronted with challenges such as unregulated Zn^(2+)diffusion,dendrite growth and severe decay in battery performance under harsh environments.Here,a design c...The deterioration of aqueous zinc-ion batteries(AZIBs)is confronted with challenges such as unregulated Zn^(2+)diffusion,dendrite growth and severe decay in battery performance under harsh environments.Here,a design concept of eutectic electrolyte is presented by mixing long chain polymer molecules,polyethylene glycol dimethyl ether(PEGDME),with H_(2)O based on zinc trifluoromethyl sulfonate(Zn(OTf)2),to reconstruct the Zn^(2+)solvated structure and in situ modified the adsorption layer on Zn electrode surface.Molecular dynamics simulations(MD),density functional theory(DFT)calculations were combined with experiment to prove that the long-chain polymer-PEGDME could effectively reduce side reactions,change the solvation structure of the electrolyte and priority absorbed on Zn(002),achieving a stable dendrite-free Zn anode.Due to the comprehensive regulation of solvation structure and zinc deposition by PEGDME,it can stably cycle for over 3200 h at room temperature at 0.5 mA/cm^(2)and 0.5 mAh/cm^(2).Even at high-temperature environments of 60℃,it can steadily work for more than 800 cycles(1600 h).Improved cyclic stability and rate performance of aqueous Zn‖VO_(2)batteries in modified electrolyte were also achieved at both room and high temperatures.Beyond that,the demonstration of stable and high-capacity Zn‖VO_(2)pouch cells also implies its practical application.展开更多
The development of flexible supercapacitors(FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and elec...The development of flexible supercapacitors(FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and electrode materials stand as two key components that significantly impact the efficacy of hightemperature-tolerant FSCs(HT-FSCs). They should not only exhibit high electrochemical performance and excellent flexibility, but also withstand intense thermal stress. Considerable efforts have been devoted to enhancing their thermal stability while maintaining high electrochemical and mechanical performance. In this review, the fundamentals of HT-FSCs are outlined. A comprehensive overview of state-of-the-art progress and achievements in HT-FSCs, with a focus on thermally stable gel polymer electrolytes and electrode materials is provided. Finally, challenges and future perspectives regarding HT-FSCs are discussed, alongside strategies for elevating operational temperatures and performance.This review offers both theoretical foundations and practical guidelines for designing and manufacturing HT-FSCs, further promoting their widespread adoption across diverse fields.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
Silica nanosheets(SN)derived from natural vermiculite(Verm)were successfully incorporated into polyethersulfone-polyvinylpyrrolidone(PES-PVP)polymer to fabricate high-temperature proton exchange membranes(HT-PEMs).The...Silica nanosheets(SN)derived from natural vermiculite(Verm)were successfully incorporated into polyethersulfone-polyvinylpyrrolidone(PES-PVP)polymer to fabricate high-temperature proton exchange membranes(HT-PEMs).The content of SN filler was varied(0.1-0.75 wt%)to study its influence on proton conductivity,power density and durability.Benefiting from the hydroxyl groups of SN that enable the formation of additional proton-transferring pathways,the inorganic-organic membrane displayed enhanced proton conductivity of 48.2 mS/cm and power density of 495 mW/cm^(2) at 150℃ without humidification when the content of SN is 0.25 wt%.Furthermore,exfoliated SN(E-SN)and sulfonated SN(S-SN),which were fabricated by a liquid-phase exfoliation method and silane condensation,respectively,were embedded in PES-PVP polymer matrix by a simple blending method.Due to the significant contribution from sulfonic groups in S-SN,the membrane with 0.25 wt%S-SN reached the highest proton conductivity of51.5 mS/cm and peak power density of 546 mW/cm^(2) at150℃,48%higher than the pristine PES-PVP membranes.Compared to unaltered PES-PVP membrane,SN added hybrid composite membrane demonstrated excellent durability for the fuel cell at 150℃.Using a facile method to prepare 2D SN from natural clay minerals,the strategy of exfoliation and functionalization of SN can be potentially used in the production of HT-PEMs.展开更多
Acid loss and plasticization of phosphoric acid(PA)-doped high-temperature polymer electrolyte membranes(HT-PEMs)are critical limitations to their practical application in fuel cells.To overcome these barriers,poly(te...Acid loss and plasticization of phosphoric acid(PA)-doped high-temperature polymer electrolyte membranes(HT-PEMs)are critical limitations to their practical application in fuel cells.To overcome these barriers,poly(terphenyl piperidinium)s constructed from the m-and p-isomers of terphenyl were synthesized to regulate the microstructure of the membrane.Highly rigid p-terphenyl units prompt the formation of moderate PA aggregates,where the ion-pair interaction between piperidinium and biphosphate is reinforced,leading to a reduction in the plasticizing effect.As a result,there are trade-offs between the proton conductivity,mechanical strength,and PA retention of the membranes with varied m/p-isomer ratios.The designed PA-doped PTP-20m membrane exhibits superior ionic conductivity,good mechanical strength,and excellent PA retention over a wide range of temperature(80–160°C)as well as satisfactory resistance to harsh accelerated aging tests.As a result,the membrane presents a desirable combination of performance(1.462 W cm^(-2) under the H_(2)/O_(2)condition,which is 1.5 times higher than that of PBI-based membrane)and durability(300 h at 160°C and 0.2 A cm^(-2))in the fuel cell.The results of this study provide new insights that will guide molecular design from the perspective of microstructure to improve the performance and robustness of HT-PEMs.展开更多
Solid polymer electrolytes(SPEs)with high ionic conductivity are desirable for solid-state lithium metal batteries(SSLMBs)to achieve enhanced safety and energy density.Incorporating nanofillers into a polymeric matrix...Solid polymer electrolytes(SPEs)with high ionic conductivity are desirable for solid-state lithium metal batteries(SSLMBs)to achieve enhanced safety and energy density.Incorporating nanofillers into a polymeric matrix to develop nanocomposite solid electrolytes(NCSEs)has become a promising method for improving the ionic conductivity of the SPEs.Here,a novel ZIF-8-functionalized NCSE was prepared for high-temperature S SLMB s using an in situ radical polymerization method.It is found that the ZIF-8 nanoparticles could reduce the crystallinity of polymer segments and offer a Lewis acid surface that promotes the dissociation of lithium bis(trifluoromethanesulfonyl)imide(LiTFSI)and stabilizes the TFSI^(-) anion movement.Thus,the as-prepared NCSE exhibits an outstanding ionic conductivity of 1.63×10^(-3)S·cm^(-1),an electrochem ical stability window of 5.0 V at 80℃,and excellent interface compatibility with lithium metal anode with a stable polarization over 2000 h.Furthermore,the assembled SSLMBs with LiFePO_(4)cathode show dendrite-free Li-metal surface,good rate capability,and stable cycling stability with a capacity retention of 70%over 1000 cycles at a high temperature of 80℃.This work provides valuable insights into promoting the ionic conductivity of SPEs.展开更多
This study investigated the physicochemical properties,enzyme activities,volatile flavor components,microbial communities,and sensory evaluation of high-temperature Daqu(HTD)during the maturation process,and a standar...This study investigated the physicochemical properties,enzyme activities,volatile flavor components,microbial communities,and sensory evaluation of high-temperature Daqu(HTD)during the maturation process,and a standard system was established for comprehensive quality evaluation of HTD.There were obvious changes in the physicochemical properties,enzyme activities,and volatile flavor components at different storage periods,which affected the sensory evaluation of HTD to a certain extent.The results of high-throughput sequencing revealed significant microbial diversity,and showed that the bacterial community changed significantly more than did the fungal community.During the storage process,the dominant bacterial genera were Kroppenstedtia and Thermoascus.The correlation between dominant microorganisms and quality indicators highlighted their role in HTD quality.Lactococcus,Candida,Pichia,Paecilomyces,and protease activity played a crucial role in the formation of isovaleraldehyde.Acidic protease activity had the greatest impact on the microbial community.Moisture promoted isobutyric acid generation.Furthermore,the comprehensive quality evaluation standard system was established by the entropy weight method combined with multi-factor fuzzy mathematics.Consequently,this study provides innovative insights for comprehensive quality evaluation of HTD during storage and establishes a groundwork for scientific and rational storage of HTD and quality control of sauce-flavor Baijiu.展开更多
Fluoride-based electrolyte exhibits extraordinarily high oxidative stability in high-voltage lithium metal batteries(h-LMBs) due to the inherent low highest occupied molecular orbital(HOMO) of fiuorinated solvents. Ho...Fluoride-based electrolyte exhibits extraordinarily high oxidative stability in high-voltage lithium metal batteries(h-LMBs) due to the inherent low highest occupied molecular orbital(HOMO) of fiuorinated solvents. However, such fascinating properties do not bring long-term cyclability of h-LMBs. One of critical challenges is the interface instability in contacting with the Li metal anode, as fiuorinated solvents are highly susceptible to exceptionally reductive metallic Li attributed to its low lowest unoccupied molecular orbital(LUMO), which leads to significant consumption of the fiuorinated components upon cycling.Herein, attenuating reductive decomposition of fiuorinated electrolytes is proposed to circumvent rapid electrolyte consumption. Specifically, the vinylene carbonate(VC) is selected to tame the reduction decomposition by preferentially forming protective layer on the Li anode. This work, experimentally and computationally, demonstrates the importance of pre-passivation of Li metal anodes at high voltage to attenuate the decomposition of fiuoroethylene carbonate(FEC). It is expected to enrich the understanding of how VC attenuate the reactivity of FEC, thereby extending the cycle life of fiuorinated electrolytes in high-voltage Li-metal batteries.展开更多
This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature&l...This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature<300℃.Sulfur vapor is a highly flammable gas,which then auto-ignites to produce a flame.This behavior suggests that an O_(2)-S gas-gas reaction mechanism may contribute to all-solid-state battery thermal runaway.To improve all-solid-state battery safety,current work focuses on eliminating the O_(2)source by changing the cathode active material.The conclusion of this study suggests that all-solidstate battery safety can also be realized by the development of solid-state electrolytes with less susceptibility to sulfur volatilization.展开更多
High-temperature industries,as the primary consumers of energy,are greatly concerned with energy savings.Designing refractory linings with low thermal conductivity to reduce heat dissipation through high-temperature f...High-temperature industries,as the primary consumers of energy,are greatly concerned with energy savings.Designing refractory linings with low thermal conductivity to reduce heat dissipation through high-temperature furnace linings is a critical concern.In this study,a series of novel entropy-stabilized spinel materials are reported,and their potential applications in high-temperature industries are investigated.XRD and TEM results indicate that all materials possess a cubic spinel crystal structure with the■space group.Furthermore,these materials exhibit good phase stability at high temperatures.All entropy-stabilized spinel aggregates demonstrated high refractoriness(>1800℃)and a high load softening temperature(>1700℃).The impact of configurational entropy on the properties of entropy-stabilized spinel materials was also studied.As configurational entropy increased,the thermal conductivity of the entropy-stabilized spinel decreased,while slag corrosion resistance deteriorated.For the entropy-stabilized spinel with a configurational entropy value of 1.126R,it showed good high-temperature stability,reliable resistance to slag attack,and a low thermal conductivity of 2.776 W·m^(-1)·K^(-1)at 1000℃.展开更多
This study focuses on the impact of Gd^(3+),Sm^(3+),Er^(3+).Y^(3+),and Bi^(3+)multi-doping on the crystal structure,microscopic surface features,and ionic conductivity of cerium dioxide in the Ce_(1-x)(Gd_(1/5)Sm_(1/5...This study focuses on the impact of Gd^(3+),Sm^(3+),Er^(3+).Y^(3+),and Bi^(3+)multi-doping on the crystal structure,microscopic surface features,and ionic conductivity of cerium dioxide in the Ce_(1-x)(Gd_(1/5)Sm_(1/5)Er_(1/5)Y_(1/)_5Bi_(1/5))_(x)O_(2-δ)(GSEYB)system.This system holds promise as a solid electrolyte material for low and medium-temperature solid oxide fuel cells.The powders of Ce_(1-x)(Gd_(1/5)Sm_(1/5)Er_(1/5)Y_(1/5)Bi_(1/5))_(x)O_(2-δ)(x=0,0.10,0.15,0.20,0.25,0.30)were synthesized using the solid-phase reaction method.The GSEYB electrolytes were comprehensively investigated for their phase structure,microstructure,oxygen vacancy concentration,and ionic conductivity using X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive spectroscopy(EDS),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),and impedance spectroscopy.XRD diffraction patterns confirm a cubic fluorite-type structure with Fm3m space groups in all multi-doped systems.After sintering at 1400℃for 10 h,the relative density of doped samples exceeds 96%.In terms of electrical properties,the Ce_(0.75)Gd_(0.05)Sm_(0.05)Er_(0.05)Y_(0.05)Bi_(0.05)O_(2-δ)(x=0.25)electrolyte exhibits the highest ionic conductivity(σ_(t)=4.45×10^(-2)S/cm)and the lowest activation energy(E_(a)=0.79 eV)at 800℃.The coefficient of thermal expansion of the developed electrolyte aligns well with that of the commonly used electrode materials.This compatibility positions it as a highly promising candidate for utilization as an electrolyte material in solid oxide fuel cells(SOFCs).展开更多
Burial dissolution is a critical diagenetic process influencing ultra-deep carbonate reservoir development and preservation.Artificial carbonate samples with different internal structures were prepared,and high-temper...Burial dissolution is a critical diagenetic process influencing ultra-deep carbonate reservoir development and preservation.Artificial carbonate samples with different internal structures were prepared,and high-temperature and highpressure dissolution kinetic simulations were conducted.The results demonstrate that the intensity of burial dissolution is controlled by temperature and pressure,while tectonic-fluid activity influences the development pattern of burial dissolution,ultimately determining the direction of its differential modification.Extensive burial dissolution is likely to occur primarily at relatively shallow depths,significantly influencing reservoir formation,preservation,modification,and adjustment.The development of faults facilitates the maintenance of the intensity of burial dissolution.The maximum intensity of burial dissolution occurs at the tips and overlap zones of faults and intersections of multiple faults.The larger the scale of the faults,the more conducive it is to the development of burial dissolution.Burial dissolution fosters the formation of fault networks characterized by enhanced reservoir capacity and permeability.Burial dissolution controlled by episodic tectonic-fluid activity is a plausible explanation for forming the Tarim Basin's ultra-deep fault-controlled“stringbead-like”reservoirs.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 development of flexible zinc-ion batteries(ZIBs)faces a threeway trade-off among the ionic conductivity,Zn^(2+)mobility,and the electrochemical stability of hydrogel electrolytes.To address this challenge,we desig...The development of flexible zinc-ion batteries(ZIBs)faces a threeway trade-off among the ionic conductivity,Zn^(2+)mobility,and the electrochemical stability of hydrogel electrolytes.To address this challenge,we designed a cationic hydrogel named PAPTMA to holistically improve the reversibility of ZIBs.The long cationic branch chains in the polymeric matrix construct express pathways for rapid Zn^(2+)transport through an ionic repulsion mechanism,achieving simultaneously high Zn^(2+)transference number(0.79)and high ionic conductivity(28.7 mS cm−1).Additionally,the reactivity of water in the PAPTMA hydrogels is significantly inhibited,thus possessing a strong resistance to parasitic reactions.Mechanical characterization further reveals the superior tensile and adhesion strength of PAPTMA.Leveraging these properties,symmetric batteries employing PAPTMA hydrogel deliver exceeding 6000 h of reversible cycling at 1 mA cm^(−2) and maintain stable operation for 1000 h with a discharge of depth of 71%.When applied in 4×4 cm2 pouch cells with MnO_(2) as the cathode material,the device demonstrates remarkable operational stability and mechanical robustness through 150 cycles.This work presents an eclectic strategy for designing advanced hydrogels that combine high ionic conductivity,enhanced Zn^(2+)mobility,and strong resistance to parasitic reactions,paving the way for long-lasting flexible ZIBs.展开更多
High-nickel ternary cathodes hold a great application prospect in solid-state lithium metal batteries to achieve high-energy density,but they still suffer from structural instability and detrimental side reactions wit...High-nickel ternary cathodes hold a great application prospect in solid-state lithium metal batteries to achieve high-energy density,but they still suffer from structural instability and detrimental side reactions with the solid-state electrolytes.To circumvent these issues,a continuous uniform layer polyacrylonitrile(PAN)was introduced on the surface of LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) via in situ polymerization of acrylonitrile(AN).Furthermore,the partial-cyclized treatment of PAN(cPAN)coating layer presents high ionic and electron conductivity,which can accelerate interfacial Li+and electron diffusion simultaneously.And the thermodynamically stabilized cPAN coating layer cannot only effectively inhibit detrimental side reactions between cathode and solid-state electrolytes but also provide a homogeneous stress to simultaneously address the problems of bulk structural degradation,which contributes to the exceptional mechanical and electrochemical stabilities of the modified electrode.Besides,the coordination bond interaction between the cPAN and NCM811 can suppress the migration of Ni to elevate the stability of the crystal structure.Benefited from these,the In-cPAN-260@NCM811 shows excellent cycling performance with a retention of 86.8%after 300 cycles and superior rate capability.And endow the solid-state battery with thermal safety stability even at hightemperature extreme environment.This facile and scalable surface engineering represents significant progress in developing high-performance solid-state lithium metal batteries.展开更多
All-solid-state Li batteries(ASSLBs)using solid electrolytes(SEs)have gained significant attention in recent years considering the safety issue and their high energy density.Despite these advantages,the commercializat...All-solid-state Li batteries(ASSLBs)using solid electrolytes(SEs)have gained significant attention in recent years considering the safety issue and their high energy density.Despite these advantages,the commercialization of ASSLBs still faces challenges regarding the electrolyte/electrodes interfaces and growth of Li dendrites.Elemental doping is an effective and direct method to enhance the performance of SEs.Here,we report an Al-F co-doping strategy to improve the overall properties including ion conductivity,high voltage stability,and cathode and anode compatibility.Particularly,the Al-F co-doping enables the formation of a thin Li-Al alloy layer and fluoride interphases,thereby constructing a relatively stable interface and promoting uniform Li deposition.The similar merits of Al-F co-doping are also revealed in the Li-argyrodite series.ASSLBs assembled with these optimized electrolytes gain good electrochemical performance,demonstrating the universality of Al-F co-doping towards advanced SEs.展开更多
Solid-state electrolytes(SSEs),as the core component within the next generation of key energy storage technologies-solid-state lithium batteries(SSLBs)-are significantly leading the development of future energy storag...Solid-state electrolytes(SSEs),as the core component within the next generation of key energy storage technologies-solid-state lithium batteries(SSLBs)-are significantly leading the development of future energy storage systems.Among the numerous types of SSEs,inorganic oxide garnet-structured superionic conductors Li7La3Zr2O12(LLZO)crystallized with the cubic Iaˉ3d space group have received considerable attention owing to their highly advantageous intrinsic properties encompassing reasonable lithium-ion conductivity,wide electrochemical voltage window,high shear modulus,and excellent chemical stability with electrodes.However,no SSEs possess all the properties necessary for SSLBs,thus both the ionic conductivity at room temperature and stability in ambient air regarding cubic garnet-based electrolytes are still subject to further improvement.Hence,this review comprehensively covers the nine key structural factors affecting the ion conductivity of garnet-based electrolytes comprising Li concentration,Li vacancy concentration,Li carrier concentration and mobility,Li occupancy at available sites,lattice constant,triangle bottleneck size,oxygen vacancy defects,and Li-O bonding interactions.Furthermore,the general illustration of structures and fundamental features being crucial to chemical stability is examined,including Li concentration,Li-site occupation behavior,and Li-O bonding interactions.Insights into the composition-structure-property relations among cubic garnet-based oxide ionic conductors from the perspective of their crystal structures,revealing the potential compatibility conflicts between ionic transportation and chemical stability resulting from Li-O bonding interactions.We believe that this review will lay the foundation for future reasonable structural design of oxide-based or even other types of superionic conductors,thus assisting in promoting the rapid development of alternative green and sustainable technologies.展开更多
The research on high-performance electromagnetic wave absorption materials with high-temperature and oxidative stability in extreme environments is gaining popularity.Herein,the lightweight silicon carbide nanowires(S...The research on high-performance electromagnetic wave absorption materials with high-temperature and oxidative stability in extreme environments is gaining popularity.Herein,the lightweight silicon carbide nanowires(SiC_(nws))/SiC composites are fabricated with in-situ SiC interface on one-dimensional oriented SiC_(nws)skeleton,which collaborative configuration by 3D printing and freeze casting assembly.The con-structed porous structure optimizes the impedance matching degree and scattering intensity,the maximum effective absorption bandwidth(EAB_(max))of 5.9 GHz and the minimum reflection loss(RL_(min))of−41.4 dB can be realized.Considering the inherent oxidation resistance of SiC,the composites present well-maintained absorption performance at 600℃.Even at 1100℃,the EAB_(max)of 4.9 GHz and RLmin of−30.4 dB also demonstrate the high-temperature absorption stability of the composites,indicating exceptional wave absorption properties and thermal stability.The slight attenuation can be attributed to the decrease in impedance matching capability accompanying the elevated dielectric constant.This work clarifies the impact of structure and component synergy on wave absorption behavior,and offers a novel approach to producing high-performance and high-temperature resistance ceramic-based electromagnetic wave absorption materials suitable for extreme environments.展开更多
Rechargeable zinc(Zn)-ion batteries(RZIBs) with hydrogel electrolytes(HEs) have gained significant attention in the last decade owing to their high safety, low cost, sufficient material abundance, and superb environme...Rechargeable zinc(Zn)-ion batteries(RZIBs) with hydrogel electrolytes(HEs) have gained significant attention in the last decade owing to their high safety, low cost, sufficient material abundance, and superb environmental friendliness, which is extremely important for wearable energy storage applications. Given that HEs play a critical role in building flexible RZIBs, it is urgent to summarize the recent advances in this field and elucidate the design principles of HEs for practical applications. This review systematically presents the development history, recent advances in the material fundamentals, functional designs, challenges, and prospects of the HEs-based RZIBs. Firstly, the fundamentals, species, and flexible mechanisms of HEs are discussed, along with their compatibility with Zn anodes and various cathodes. Then, the functional designs of hydrogel electrolytes in harsh conditions are comprehensively discussed, including high/low/wide-temperature windows, mechanical deformations(e.g., bending, twisting, and straining), and damages(e.g., cutting, burning, and soaking). Finally, the remaining challenges and future perspectives for advancing HEs-based RZIBs are outlined.展开更多
Vanadium pentoxide(V_(2)O_(5))displays the characteristics of high theoretical specific capacity,high operating voltage,and adjustable layered structure,possessing the considerable potential as cathode in magnesium me...Vanadium pentoxide(V_(2)O_(5))displays the characteristics of high theoretical specific capacity,high operating voltage,and adjustable layered structure,possessing the considerable potential as cathode in magnesium metal batteries(MMBs).Nevertheless,the large charge-radius ratio of Mg^(2+)induces the strong interactions of Mg^(2+)with solvent molecules of electrolyte and anionic framework of cathode,resulting in a notable voltage polarization and structural deterioration during cycling process.Herein,an in-situ multi-scale structural engineering is proposed to activate the interlayer-expanded V_(2)O_(5)cathode(pillared by tetrabutylammonium cation)via adding hexadecyltrimethylammonium bromide(CTAB)additive into electrolyte.During cycling,the in-situ incorporation of CTA^(+)not only enhances the electrostatic shielding effect and Mg species migration,but also stabilizes the interlayer spacing.Besides,CTA^(+)is prone to be adsorbed on cathode surface and induces the loss-free pulverization and amorphization of electroactive grains,leading to the pronounced effect of intercalation pseudocapacitance.CTAB additive also enables to scissor the Mg^(2+)solvation sheath and tailor the insertion mode of Mg species,further endowing V_(2)O_(5)cathode with fast reaction kinetics.Based on these merits,the corresponding V2O5‖Mg full cells exhibit the remarkable rate performance with capacities as high as 317.6,274.4,201.1,and 132.7 mAh g^(-1)at the high current densities of 0.1,0.2,0.5,and 1 A g^(-1),respectively.Moreover,after 1000 cycles,the capacity is still preserved to be 90,4 mAh g^(-1)at 1 A g^(-1)with an average coulombic efficiency of~100%.Our strategy of synergetic modulations of cathode host and electrolyte solvation structures provides new guidance for the development of high-rate,large-capacity,and long-life MMBs.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22208221,22178221)the Natural Science Foundation of Guangdong Province(Nos.2024A1515011078,2024A1515011507)+1 种基金the Shenzhen Science and Technology Program(Nos.JCYJ20220818095805012,JCYJ20230808105109019)the Start-up Research Funding of Shenzhen University(No.868-000001032522).
文摘The deterioration of aqueous zinc-ion batteries(AZIBs)is confronted with challenges such as unregulated Zn^(2+)diffusion,dendrite growth and severe decay in battery performance under harsh environments.Here,a design concept of eutectic electrolyte is presented by mixing long chain polymer molecules,polyethylene glycol dimethyl ether(PEGDME),with H_(2)O based on zinc trifluoromethyl sulfonate(Zn(OTf)2),to reconstruct the Zn^(2+)solvated structure and in situ modified the adsorption layer on Zn electrode surface.Molecular dynamics simulations(MD),density functional theory(DFT)calculations were combined with experiment to prove that the long-chain polymer-PEGDME could effectively reduce side reactions,change the solvation structure of the electrolyte and priority absorbed on Zn(002),achieving a stable dendrite-free Zn anode.Due to the comprehensive regulation of solvation structure and zinc deposition by PEGDME,it can stably cycle for over 3200 h at room temperature at 0.5 mA/cm^(2)and 0.5 mAh/cm^(2).Even at high-temperature environments of 60℃,it can steadily work for more than 800 cycles(1600 h).Improved cyclic stability and rate performance of aqueous Zn‖VO_(2)batteries in modified electrolyte were also achieved at both room and high temperatures.Beyond that,the demonstration of stable and high-capacity Zn‖VO_(2)pouch cells also implies its practical application.
基金Fundamental Research Funds for the Central Universities of China(Grant No. SWU-KT22030)Scientific and Technological Research Program of Chongqing Municipal Education Commission of China (No.KJQN202300205)financial support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under the project of 457444676。
文摘The development of flexible supercapacitors(FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and electrode materials stand as two key components that significantly impact the efficacy of hightemperature-tolerant FSCs(HT-FSCs). They should not only exhibit high electrochemical performance and excellent flexibility, but also withstand intense thermal stress. Considerable efforts have been devoted to enhancing their thermal stability while maintaining high electrochemical and mechanical performance. In this review, the fundamentals of HT-FSCs are outlined. A comprehensive overview of state-of-the-art progress and achievements in HT-FSCs, with a focus on thermally stable gel polymer electrolytes and electrode materials is provided. Finally, challenges and future perspectives regarding HT-FSCs are discussed, alongside strategies for elevating operational temperatures and performance.This review offers both theoretical foundations and practical guidelines for designing and manufacturing HT-FSCs, further promoting their widespread adoption across diverse fields.
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 EPSRC grant EP/009050/1supported by the Henry Royce Institute for Advanced Materials which is funded by EPSRC grants EP/S019367/1,EP/P025021/1,EP/R00661X/1 and EP/P025498/1.
文摘Silica nanosheets(SN)derived from natural vermiculite(Verm)were successfully incorporated into polyethersulfone-polyvinylpyrrolidone(PES-PVP)polymer to fabricate high-temperature proton exchange membranes(HT-PEMs).The content of SN filler was varied(0.1-0.75 wt%)to study its influence on proton conductivity,power density and durability.Benefiting from the hydroxyl groups of SN that enable the formation of additional proton-transferring pathways,the inorganic-organic membrane displayed enhanced proton conductivity of 48.2 mS/cm and power density of 495 mW/cm^(2) at 150℃ without humidification when the content of SN is 0.25 wt%.Furthermore,exfoliated SN(E-SN)and sulfonated SN(S-SN),which were fabricated by a liquid-phase exfoliation method and silane condensation,respectively,were embedded in PES-PVP polymer matrix by a simple blending method.Due to the significant contribution from sulfonic groups in S-SN,the membrane with 0.25 wt%S-SN reached the highest proton conductivity of51.5 mS/cm and peak power density of 546 mW/cm^(2) at150℃,48%higher than the pristine PES-PVP membranes.Compared to unaltered PES-PVP membrane,SN added hybrid composite membrane demonstrated excellent durability for the fuel cell at 150℃.Using a facile method to prepare 2D SN from natural clay minerals,the strategy of exfoliation and functionalization of SN can be potentially used in the production of HT-PEMs.
基金supported by The National Key Research and Development Program of China(2021YFB4001204)National Natural Science Foundation of China(22379143)。
文摘Acid loss and plasticization of phosphoric acid(PA)-doped high-temperature polymer electrolyte membranes(HT-PEMs)are critical limitations to their practical application in fuel cells.To overcome these barriers,poly(terphenyl piperidinium)s constructed from the m-and p-isomers of terphenyl were synthesized to regulate the microstructure of the membrane.Highly rigid p-terphenyl units prompt the formation of moderate PA aggregates,where the ion-pair interaction between piperidinium and biphosphate is reinforced,leading to a reduction in the plasticizing effect.As a result,there are trade-offs between the proton conductivity,mechanical strength,and PA retention of the membranes with varied m/p-isomer ratios.The designed PA-doped PTP-20m membrane exhibits superior ionic conductivity,good mechanical strength,and excellent PA retention over a wide range of temperature(80–160°C)as well as satisfactory resistance to harsh accelerated aging tests.As a result,the membrane presents a desirable combination of performance(1.462 W cm^(-2) under the H_(2)/O_(2)condition,which is 1.5 times higher than that of PBI-based membrane)and durability(300 h at 160°C and 0.2 A cm^(-2))in the fuel cell.The results of this study provide new insights that will guide molecular design from the perspective of microstructure to improve the performance and robustness of HT-PEMs.
基金financially supported by the Fundamental Research Program of Shanxi Province(No.202103021224177)the Science and Technology Cooperation and Exchange Special Project of Shanxi Province(No.202204041101005)+1 种基金the Key Laboratory Research Foundation of North University of China and Shanxi Key Laboratory of Advanced Carbon Electrode Materials(No.202104010910019)the funding support from the Australian Research Council(No.DP200102573)。
文摘Solid polymer electrolytes(SPEs)with high ionic conductivity are desirable for solid-state lithium metal batteries(SSLMBs)to achieve enhanced safety and energy density.Incorporating nanofillers into a polymeric matrix to develop nanocomposite solid electrolytes(NCSEs)has become a promising method for improving the ionic conductivity of the SPEs.Here,a novel ZIF-8-functionalized NCSE was prepared for high-temperature S SLMB s using an in situ radical polymerization method.It is found that the ZIF-8 nanoparticles could reduce the crystallinity of polymer segments and offer a Lewis acid surface that promotes the dissociation of lithium bis(trifluoromethanesulfonyl)imide(LiTFSI)and stabilizes the TFSI^(-) anion movement.Thus,the as-prepared NCSE exhibits an outstanding ionic conductivity of 1.63×10^(-3)S·cm^(-1),an electrochem ical stability window of 5.0 V at 80℃,and excellent interface compatibility with lithium metal anode with a stable polarization over 2000 h.Furthermore,the assembled SSLMBs with LiFePO_(4)cathode show dendrite-free Li-metal surface,good rate capability,and stable cycling stability with a capacity retention of 70%over 1000 cycles at a high temperature of 80℃.This work provides valuable insights into promoting the ionic conductivity of SPEs.
文摘This study investigated the physicochemical properties,enzyme activities,volatile flavor components,microbial communities,and sensory evaluation of high-temperature Daqu(HTD)during the maturation process,and a standard system was established for comprehensive quality evaluation of HTD.There were obvious changes in the physicochemical properties,enzyme activities,and volatile flavor components at different storage periods,which affected the sensory evaluation of HTD to a certain extent.The results of high-throughput sequencing revealed significant microbial diversity,and showed that the bacterial community changed significantly more than did the fungal community.During the storage process,the dominant bacterial genera were Kroppenstedtia and Thermoascus.The correlation between dominant microorganisms and quality indicators highlighted their role in HTD quality.Lactococcus,Candida,Pichia,Paecilomyces,and protease activity played a crucial role in the formation of isovaleraldehyde.Acidic protease activity had the greatest impact on the microbial community.Moisture promoted isobutyric acid generation.Furthermore,the comprehensive quality evaluation standard system was established by the entropy weight method combined with multi-factor fuzzy mathematics.Consequently,this study provides innovative insights for comprehensive quality evaluation of HTD during storage and establishes a groundwork for scientific and rational storage of HTD and quality control of sauce-flavor Baijiu.
基金supported by the National Natural Science Foundation of China (Nos. 22379121, 62005216)Basic Public Welfare Research Program of Zhejiang (No. LQ22F050013)+1 种基金Zhejiang Province Key Laboratory of Flexible Electronics Open Fund (2023FE005)Shenzhen Foundation Research Program (No. JCYJ20220530112812028)。
文摘Fluoride-based electrolyte exhibits extraordinarily high oxidative stability in high-voltage lithium metal batteries(h-LMBs) due to the inherent low highest occupied molecular orbital(HOMO) of fiuorinated solvents. However, such fascinating properties do not bring long-term cyclability of h-LMBs. One of critical challenges is the interface instability in contacting with the Li metal anode, as fiuorinated solvents are highly susceptible to exceptionally reductive metallic Li attributed to its low lowest unoccupied molecular orbital(LUMO), which leads to significant consumption of the fiuorinated components upon cycling.Herein, attenuating reductive decomposition of fiuorinated electrolytes is proposed to circumvent rapid electrolyte consumption. Specifically, the vinylene carbonate(VC) is selected to tame the reduction decomposition by preferentially forming protective layer on the Li anode. This work, experimentally and computationally, demonstrates the importance of pre-passivation of Li metal anodes at high voltage to attenuate the decomposition of fiuoroethylene carbonate(FEC). It is expected to enrich the understanding of how VC attenuate the reactivity of FEC, thereby extending the cycle life of fiuorinated electrolytes in high-voltage Li-metal batteries.
文摘This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature<300℃.Sulfur vapor is a highly flammable gas,which then auto-ignites to produce a flame.This behavior suggests that an O_(2)-S gas-gas reaction mechanism may contribute to all-solid-state battery thermal runaway.To improve all-solid-state battery safety,current work focuses on eliminating the O_(2)source by changing the cathode active material.The conclusion of this study suggests that all-solidstate battery safety can also be realized by the development of solid-state electrolytes with less susceptibility to sulfur volatilization.
基金financially supported by the National Natural Science Foundation of China(Nos.52472032 and 52172023)the Key Program of Natural Science Foundation of Hubei Province(No.2024AFA083)
文摘High-temperature industries,as the primary consumers of energy,are greatly concerned with energy savings.Designing refractory linings with low thermal conductivity to reduce heat dissipation through high-temperature furnace linings is a critical concern.In this study,a series of novel entropy-stabilized spinel materials are reported,and their potential applications in high-temperature industries are investigated.XRD and TEM results indicate that all materials possess a cubic spinel crystal structure with the■space group.Furthermore,these materials exhibit good phase stability at high temperatures.All entropy-stabilized spinel aggregates demonstrated high refractoriness(>1800℃)and a high load softening temperature(>1700℃).The impact of configurational entropy on the properties of entropy-stabilized spinel materials was also studied.As configurational entropy increased,the thermal conductivity of the entropy-stabilized spinel decreased,while slag corrosion resistance deteriorated.For the entropy-stabilized spinel with a configurational entropy value of 1.126R,it showed good high-temperature stability,reliable resistance to slag attack,and a low thermal conductivity of 2.776 W·m^(-1)·K^(-1)at 1000℃.
基金supported by the Guangdong Provincial Basic and Applied Basic Research Foundation(2021A1515010671,2020A1515011221)the Guangdong Provincial Key Discipline Research Capacity Enhancement Project(2021ZDJS071)the Guangdong Provincial College Innovation Project(2021KTSCX122,2022KQNCX077)。
文摘This study focuses on the impact of Gd^(3+),Sm^(3+),Er^(3+).Y^(3+),and Bi^(3+)multi-doping on the crystal structure,microscopic surface features,and ionic conductivity of cerium dioxide in the Ce_(1-x)(Gd_(1/5)Sm_(1/5)Er_(1/5)Y_(1/)_5Bi_(1/5))_(x)O_(2-δ)(GSEYB)system.This system holds promise as a solid electrolyte material for low and medium-temperature solid oxide fuel cells.The powders of Ce_(1-x)(Gd_(1/5)Sm_(1/5)Er_(1/5)Y_(1/5)Bi_(1/5))_(x)O_(2-δ)(x=0,0.10,0.15,0.20,0.25,0.30)were synthesized using the solid-phase reaction method.The GSEYB electrolytes were comprehensively investigated for their phase structure,microstructure,oxygen vacancy concentration,and ionic conductivity using X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive spectroscopy(EDS),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),and impedance spectroscopy.XRD diffraction patterns confirm a cubic fluorite-type structure with Fm3m space groups in all multi-doped systems.After sintering at 1400℃for 10 h,the relative density of doped samples exceeds 96%.In terms of electrical properties,the Ce_(0.75)Gd_(0.05)Sm_(0.05)Er_(0.05)Y_(0.05)Bi_(0.05)O_(2-δ)(x=0.25)electrolyte exhibits the highest ionic conductivity(σ_(t)=4.45×10^(-2)S/cm)and the lowest activation energy(E_(a)=0.79 eV)at 800℃.The coefficient of thermal expansion of the developed electrolyte aligns well with that of the commonly used electrode materials.This compatibility positions it as a highly promising candidate for utilization as an electrolyte material in solid oxide fuel cells(SOFCs).
基金supported by the National Natural Science Foundation of China(Grant No.U21B2062)supported by the Key Laboratory for Carbonate Reservoirs of China National Petroleum Corporation。
文摘Burial dissolution is a critical diagenetic process influencing ultra-deep carbonate reservoir development and preservation.Artificial carbonate samples with different internal structures were prepared,and high-temperature and highpressure dissolution kinetic simulations were conducted.The results demonstrate that the intensity of burial dissolution is controlled by temperature and pressure,while tectonic-fluid activity influences the development pattern of burial dissolution,ultimately determining the direction of its differential modification.Extensive burial dissolution is likely to occur primarily at relatively shallow depths,significantly influencing reservoir formation,preservation,modification,and adjustment.The development of faults facilitates the maintenance of the intensity of burial dissolution.The maximum intensity of burial dissolution occurs at the tips and overlap zones of faults and intersections of multiple faults.The larger the scale of the faults,the more conducive it is to the development of burial dissolution.Burial dissolution fosters the formation of fault networks characterized by enhanced reservoir capacity and permeability.Burial dissolution controlled by episodic tectonic-fluid activity is a plausible explanation for forming the Tarim Basin's ultra-deep fault-controlled“stringbead-like”reservoirs.
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.
基金financially supported by the General Research Fund(CityU 11315622 and CityU 11310123)National Natural Science Foundation(NSFC 52372229 and NSFC 52172241)+3 种基金Green Tech Fund(GTF202220105)Guangdong Basic and Applied Basic Research Foundation(2024A1515011008)City University of Hong Kong(No.9020002)the Shenzhen Research Institute of City University of Hong Kong.
文摘The development of flexible zinc-ion batteries(ZIBs)faces a threeway trade-off among the ionic conductivity,Zn^(2+)mobility,and the electrochemical stability of hydrogel electrolytes.To address this challenge,we designed a cationic hydrogel named PAPTMA to holistically improve the reversibility of ZIBs.The long cationic branch chains in the polymeric matrix construct express pathways for rapid Zn^(2+)transport through an ionic repulsion mechanism,achieving simultaneously high Zn^(2+)transference number(0.79)and high ionic conductivity(28.7 mS cm−1).Additionally,the reactivity of water in the PAPTMA hydrogels is significantly inhibited,thus possessing a strong resistance to parasitic reactions.Mechanical characterization further reveals the superior tensile and adhesion strength of PAPTMA.Leveraging these properties,symmetric batteries employing PAPTMA hydrogel deliver exceeding 6000 h of reversible cycling at 1 mA cm^(−2) and maintain stable operation for 1000 h with a discharge of depth of 71%.When applied in 4×4 cm2 pouch cells with MnO_(2) as the cathode material,the device demonstrates remarkable operational stability and mechanical robustness through 150 cycles.This work presents an eclectic strategy for designing advanced hydrogels that combine high ionic conductivity,enhanced Zn^(2+)mobility,and strong resistance to parasitic reactions,paving the way for long-lasting flexible ZIBs.
基金financially supported by the National Natural Science Foundation of China(Nos.22102212 and 22479067).
文摘High-nickel ternary cathodes hold a great application prospect in solid-state lithium metal batteries to achieve high-energy density,but they still suffer from structural instability and detrimental side reactions with the solid-state electrolytes.To circumvent these issues,a continuous uniform layer polyacrylonitrile(PAN)was introduced on the surface of LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) via in situ polymerization of acrylonitrile(AN).Furthermore,the partial-cyclized treatment of PAN(cPAN)coating layer presents high ionic and electron conductivity,which can accelerate interfacial Li+and electron diffusion simultaneously.And the thermodynamically stabilized cPAN coating layer cannot only effectively inhibit detrimental side reactions between cathode and solid-state electrolytes but also provide a homogeneous stress to simultaneously address the problems of bulk structural degradation,which contributes to the exceptional mechanical and electrochemical stabilities of the modified electrode.Besides,the coordination bond interaction between the cPAN and NCM811 can suppress the migration of Ni to elevate the stability of the crystal structure.Benefited from these,the In-cPAN-260@NCM811 shows excellent cycling performance with a retention of 86.8%after 300 cycles and superior rate capability.And endow the solid-state battery with thermal safety stability even at hightemperature extreme environment.This facile and scalable surface engineering represents significant progress in developing high-performance solid-state lithium metal batteries.
基金supported by the National Natural Science Foundation of China(Nos.52172243,52371215)。
文摘All-solid-state Li batteries(ASSLBs)using solid electrolytes(SEs)have gained significant attention in recent years considering the safety issue and their high energy density.Despite these advantages,the commercialization of ASSLBs still faces challenges regarding the electrolyte/electrodes interfaces and growth of Li dendrites.Elemental doping is an effective and direct method to enhance the performance of SEs.Here,we report an Al-F co-doping strategy to improve the overall properties including ion conductivity,high voltage stability,and cathode and anode compatibility.Particularly,the Al-F co-doping enables the formation of a thin Li-Al alloy layer and fluoride interphases,thereby constructing a relatively stable interface and promoting uniform Li deposition.The similar merits of Al-F co-doping are also revealed in the Li-argyrodite series.ASSLBs assembled with these optimized electrolytes gain good electrochemical performance,demonstrating the universality of Al-F co-doping towards advanced SEs.
基金supported by the National Natural Science Foundation of China(Nos.22171102 and 22090044)the National Key R&D Program of China(Nos.2021YFF0500502 and 2023YFA1506304)+2 种基金the Jilin Province Science and Technology Development Plan(No.20230101024JC)the"Medicine+X"crossinnovation team of Bethune Medical Department of Jilin University"Leading the Charge with Open Competition"construction project(No.2022JBGS04)the Jilin University Graduate Training Office(Nos.2021JGZ08 and 2022YJSJIP20).
文摘Solid-state electrolytes(SSEs),as the core component within the next generation of key energy storage technologies-solid-state lithium batteries(SSLBs)-are significantly leading the development of future energy storage systems.Among the numerous types of SSEs,inorganic oxide garnet-structured superionic conductors Li7La3Zr2O12(LLZO)crystallized with the cubic Iaˉ3d space group have received considerable attention owing to their highly advantageous intrinsic properties encompassing reasonable lithium-ion conductivity,wide electrochemical voltage window,high shear modulus,and excellent chemical stability with electrodes.However,no SSEs possess all the properties necessary for SSLBs,thus both the ionic conductivity at room temperature and stability in ambient air regarding cubic garnet-based electrolytes are still subject to further improvement.Hence,this review comprehensively covers the nine key structural factors affecting the ion conductivity of garnet-based electrolytes comprising Li concentration,Li vacancy concentration,Li carrier concentration and mobility,Li occupancy at available sites,lattice constant,triangle bottleneck size,oxygen vacancy defects,and Li-O bonding interactions.Furthermore,the general illustration of structures and fundamental features being crucial to chemical stability is examined,including Li concentration,Li-site occupation behavior,and Li-O bonding interactions.Insights into the composition-structure-property relations among cubic garnet-based oxide ionic conductors from the perspective of their crystal structures,revealing the potential compatibility conflicts between ionic transportation and chemical stability resulting from Li-O bonding interactions.We believe that this review will lay the foundation for future reasonable structural design of oxide-based or even other types of superionic conductors,thus assisting in promoting the rapid development of alternative green and sustainable technologies.
基金supported by the National Key R&D Program of China(No.2022YFB3707700)National Natural Science Foundation of China(No.52302121)+3 种基金Shanghai Sailing Program(No.23YF1454700)Shanghai Natural Science Foundation(No.23ZR1472700)Shanghai Post-doctoral Excellent Program(No.2022664)Shanghai Science and Technology Innovation Action Plan(No.21511104800).
文摘The research on high-performance electromagnetic wave absorption materials with high-temperature and oxidative stability in extreme environments is gaining popularity.Herein,the lightweight silicon carbide nanowires(SiC_(nws))/SiC composites are fabricated with in-situ SiC interface on one-dimensional oriented SiC_(nws)skeleton,which collaborative configuration by 3D printing and freeze casting assembly.The con-structed porous structure optimizes the impedance matching degree and scattering intensity,the maximum effective absorption bandwidth(EAB_(max))of 5.9 GHz and the minimum reflection loss(RL_(min))of−41.4 dB can be realized.Considering the inherent oxidation resistance of SiC,the composites present well-maintained absorption performance at 600℃.Even at 1100℃,the EAB_(max)of 4.9 GHz and RLmin of−30.4 dB also demonstrate the high-temperature absorption stability of the composites,indicating exceptional wave absorption properties and thermal stability.The slight attenuation can be attributed to the decrease in impedance matching capability accompanying the elevated dielectric constant.This work clarifies the impact of structure and component synergy on wave absorption behavior,and offers a novel approach to producing high-performance and high-temperature resistance ceramic-based electromagnetic wave absorption materials suitable for extreme environments.
基金supported by the National Natural Science Foundation of China (22379038)Science Research Project of Hebei Education Department (JZX2024015)+4 种基金Shijiazhuang Science and Technology Plan Project (241791357A)Central Guidance for Local Science and Technology Development Funds Project (246Z4408G)Excellent Youth Research Innovation Team of Hebei University (QNTD202410)High-level Talents Research Start-Up Project of Hebei University (521100224223)Hebei Province Innovation Capability Enhancement Plan Project (22567620H)。
文摘Rechargeable zinc(Zn)-ion batteries(RZIBs) with hydrogel electrolytes(HEs) have gained significant attention in the last decade owing to their high safety, low cost, sufficient material abundance, and superb environmental friendliness, which is extremely important for wearable energy storage applications. Given that HEs play a critical role in building flexible RZIBs, it is urgent to summarize the recent advances in this field and elucidate the design principles of HEs for practical applications. This review systematically presents the development history, recent advances in the material fundamentals, functional designs, challenges, and prospects of the HEs-based RZIBs. Firstly, the fundamentals, species, and flexible mechanisms of HEs are discussed, along with their compatibility with Zn anodes and various cathodes. Then, the functional designs of hydrogel electrolytes in harsh conditions are comprehensively discussed, including high/low/wide-temperature windows, mechanical deformations(e.g., bending, twisting, and straining), and damages(e.g., cutting, burning, and soaking). Finally, the remaining challenges and future perspectives for advancing HEs-based RZIBs are outlined.
基金supported by the National Natural Science Foundation of China(52372249)support by the Program of Shanghai Academic Research Leader(21XD1424400)。
文摘Vanadium pentoxide(V_(2)O_(5))displays the characteristics of high theoretical specific capacity,high operating voltage,and adjustable layered structure,possessing the considerable potential as cathode in magnesium metal batteries(MMBs).Nevertheless,the large charge-radius ratio of Mg^(2+)induces the strong interactions of Mg^(2+)with solvent molecules of electrolyte and anionic framework of cathode,resulting in a notable voltage polarization and structural deterioration during cycling process.Herein,an in-situ multi-scale structural engineering is proposed to activate the interlayer-expanded V_(2)O_(5)cathode(pillared by tetrabutylammonium cation)via adding hexadecyltrimethylammonium bromide(CTAB)additive into electrolyte.During cycling,the in-situ incorporation of CTA^(+)not only enhances the electrostatic shielding effect and Mg species migration,but also stabilizes the interlayer spacing.Besides,CTA^(+)is prone to be adsorbed on cathode surface and induces the loss-free pulverization and amorphization of electroactive grains,leading to the pronounced effect of intercalation pseudocapacitance.CTAB additive also enables to scissor the Mg^(2+)solvation sheath and tailor the insertion mode of Mg species,further endowing V_(2)O_(5)cathode with fast reaction kinetics.Based on these merits,the corresponding V2O5‖Mg full cells exhibit the remarkable rate performance with capacities as high as 317.6,274.4,201.1,and 132.7 mAh g^(-1)at the high current densities of 0.1,0.2,0.5,and 1 A g^(-1),respectively.Moreover,after 1000 cycles,the capacity is still preserved to be 90,4 mAh g^(-1)at 1 A g^(-1)with an average coulombic efficiency of~100%.Our strategy of synergetic modulations of cathode host and electrolyte solvation structures provides new guidance for the development of high-rate,large-capacity,and long-life MMBs.
