Search Results (51)

Solid-state electrolytes (SSEs) have emerged as a promising solution for next-generation lithium-ion batteries due to their excellent safety and high energy density. However, their practical application is still hindered by critical challenges such as their low ionic conductivity and high interfacial resistance at room temperature. The innovative application of 3D printing in the field of electrochemistry, particularly in solid-state electrolytes, endows energy storage devices with attractive characteristics. In this study, ceramic-in-gel polymer electrolytes (GPEs) based on PVDF-HFP/PAN@LLZTO were fabricated using a direct ink writing (DIW) 3D printing technique. Under the optimal printing conditions (printing speed of 40 mm/s and fill density of 70%), the printed electrolyte exhibited a uniform and dense sponge-like porous structure, achieving a high ionic conductivity of 5.77 × 10⁻⁴ S·cm⁻¹, which effectively facilitated lithium-ion transport. A structural analysis indicated that the LLZTO fillers were uniformly dispersed within the polymer matrix, significantly enhancing the electrochemical stability of the electrolyte. When applied in a LiFePO₄|GPEs|Li cell configuration, the electrolyte delivered excellent electrochemical performance, with high initial discharge capacities of 168 mAh·g⁻¹ at 0.1 C and 166 mAh·g⁻¹ at 0.2 C, and retained 92.8% of its capacity after 100 cycles at 0.2 C. This work demonstrates the great potential of 3D printing technology in fabricating high-performance GPEs. It provides a novel strategy for the structural design and industrial scalability of lithium-ion batteries. Full article

Ceramic-coated polyolefin separator technology is considered a simple and effective method for the improvement of lithium-ion battery (LIB) safety. However, the characteristics of ceramic powder can adversely affect the surface structure and ion conductivity of the separators. Therefore, it is crucial to develop a ceramic powder that not only improves the thermal stability of the separators but also enhances ion conductivity. Herein, network spherical α-Al₂O₃ (N-Al₂O₃) with a multi-dimensional network pore structure was constructed. Furthermore, N-Al₂O₃ was applied as a coating to one side of polyethylene (PE) separators, resulting in N-Al₂O₃-PE separators that exhibit superior thermal stability and enhanced wettability with liquid electrolytes. Notably, the N-Al₂O₃-PE separators demonstrated exceptional ionic conductivity (0.632 mS cm⁻¹), attributed to the internal multi-dimensional network pore structures of N-Al₂O₃, which facilitated an interconnected and efficient “highway” for the transport of Li⁺ ions. As a consequence, LiCoO₂/Li half batteries equipped with these N-Al₂O₃-PE separators showcased remarkable rate and cycling performance. Particularly at high current densities, their discharge capacity and capacity retention rate significantly outperformed those of conventional PE separators. Full article

Developing thin-film sheets made of oxide-based solid electrolytes is essential for fabricating surface-mounted ultracompact multilayer oxide solid-state batteries. To this end, solid-electrolyte slurry must be optimized for excellent dispersibility. Although oxide-based solid electrolytes for multilayer structures require sintering, high processing temperatures cause problems such as Li-ion volatilization and reactions with graphite anodes. Thus, low-temperature sinterable oxide-based solid-electrolyte materials should be devised. We successfully developed the conditions for producing thin films from 21 μm thick solid-electrolyte sheets of Li₂O-B₂O₃-Al₂O₃, one of the most promising candidates for multilayer solid-state batteries. A comprehensive analysis of the fabricated thin films included X-ray diffraction (XRD) to confirm their amorphous structure, scanning electron microscopy (SEM) for particle morphology, and contact angle measurements to verify surface hydrophilicity. Evaluation of a 32-layer bulk sample of solid-electrolyte sheets revealed an ionic conductivity of 2.33 × 10⁻⁷ S/cm and charge transfer resistance of 100.1 kΩ at a sintering temperature of 430 °C. Based on these results, cathode and anode active materials will be applied to develop high-energy-density multilayer ceramic batteries with hundreds of layers in future work. Full article

Solid-state electrolytes for lithium-ion batteries, which enable a significant increase in storage capacity, are at the forefront of alternative energy storage systems due to their attractive properties such as wide electrochemical stability window, relatively superior contact stability against Li metal, inherently dendrite inhibition, and a wide range of temperature functionality. NASICON-type solid electrolytes are an exciting candidate within ceramic electrolytes due to their high ionic conductivity and low moisture sensitivity, making them a prime candidate for pure oxidic and hybrid ceramic-in-polymer composite electrolytes. Here, we report on producing pure and Y-doped Lithium Aluminum Titanium Phosphate (LATP) nanoparticles by spray-flame synthesis. The as-synthesized samples consist of an amorphous component and anatase-TiO₂ crystalline particles. Brief annealing at 750–1000 °C for one hour was sufficient to achieve the desired phase while maintaining the material’s sub-micrometer scale. Rietveld analysis of X-Ray diffraction data demonstrated that the crystal volume increases with Y doping. At the same time, with high Y incorporation, a segregation of the YPO₄ phase was observed in addition to the desired LATP phase. Another impurity phase, LiTiOPO₄, was observed besides YPO₄ and, with higher calcination temperature (1000 °C), the phase fraction for both impurities also increased. The ionic conductivity increased with Y incorporation from 0.1 mS/cm at room temperature in the undoped sample to 0.84 mS/cm in the case of LAY0.1TP, which makes these materials—especially considering the comparatively low sintering temperature—highly interesting for applications in the field of solid-state batteries. Full article

Lithium-ion batteries have garnered significant attention owing to their exceptional energy density, extended lifespan, rapid charging capabilities, eco-friendly characteristics, and extensive application potential. These remarkable features establish them as a critical focus for advancing next-generation battery technologies. However, the commonly used organic liquid electrolytes in batteries are explosive, volatile, and possess specific toxic properties, resulting in persistent safety concerns that remain to be addressed. Composite polymer electrolytes (CPEs) exhibit enhanced safety and stable electrochemical performance, emerging as one of the most promising alternatives. However, single polymers often need to meet the multifaceted performance requirements of batteries. In this study, a composite polymer electrolyte was prepared using solution casting, consisting of a blend of polyurethane (TPU) and polyacrylonitrile (PAN), along with the ceramic filler Li_1.3Al_0.3Ti_1.7(PO₄)₃ (LATP) and lithium perchlorate (LiClO₄). The optimal formulation, which included 40 wt% TPU, 60 wt% PAN, and 10 wt% LATP, exhibited a commendable ionic conductivity of 2.1 × 10⁻⁴ S cm⁻¹, a lithium-ion transference number (t_Li⁺) of 0.60, and notable electrochemical stability at 30 °C. The LiFePO₄/Li battery assembled with this CPE demonstrated excellent cycling stability and rate capability at room temperature. It delivered a discharge specific capacity of 130 mAh g⁻¹ at 1C. Under a charge–discharge rate of 0.2C, the battery achieved a discharge specific capacity of 168 mAh g⁻¹, retaining 98% of its capacity after 100 cycles at 25 °C. Additionally, the CPE exhibited robust safety performance. Consequently, this composite polymer electrolyte holds significant promise for application in lithium-ion batteries. Full article

The novel crosslinked composite polymer electrolyte (CPE) was developed and investigated using polytetrahydrofuran (PTHF) and polyethyleneglycol diacrylate (PEGDA), incorporating lithium aluminum titanium phosphate (LATP) particles and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt. Composite polymer electrolytes (CPEs) for solid-state lithium-ion batteries (LIBs) were synthesized by harnessing the synergistic effects of PTHF crosslinking and the addition of LATP ceramics, while systematically varying the film composition and LATP content. CPEs containing 15 wt% LATP (PPL15) demonstrated improved mechanical strength and electrochemical stability, achieving a high conductivity of 1.16 × 10⁻⁵ S·cm⁻¹ at 80 °C, outperforming conventional PEO-based polymer electrolytes. The CPE system effectively addresses safety concerns and mitigates the rapid degradation typically associated with polyether electrolytes. The incorporation of PEGDA not only enhances mechanical stability but also facilitates lithium salt dissociation and ion transport, leading to a uniform microstructure free from agglomerated particles. The temperature-dependent ionic conductivity measurements indicated optimal performance at lower LATP concentrations, highlighting the impact of ceramic particle agglomeration onion transport pathways. These findings contribute to advancing solid-state battery systems toward practical application. Full article

Rechargeable batteries play a crucial role in the utilization of renewable energy sources. Energy storage systems (ESSs) are designed to store renewable energy efficiently for immediate use. The market for energy storage systems heavily relies on lithium-ion batteries due to their high energy density, capacity, and competitiveness. However, the increasing cost and limited availability of lithium make long-term use challenging. As an alternative to Li-ion batteries, rechargeable seawater batteries are gaining attention due to their abundant and complementary sodium ion active materials. This study focuses on the preparation and characterization of Na_3.0Zr₂Si₂PO₁₂- and Na_3.15Zr₂Si₂PO₁₂-type ceramic membranes and testing their stability in seawater batteries used as solid electrolyte. From the surface analysis, it was observed that the Na_3.15Zr₂Si₂PO₁₂ powder showed a specific surface area of 2.94 m²/g compared to 2.69 m²/g for the Na_3.0Zr₂Si₂PO₁₂ powder. The measured NASICON samples achieved ionic conductivities between 7.42 × 10⁻⁵ and 4.4 × 10⁻⁴ S/cm compared to the NASICON commercial membrane with an ionic conductivity of 3.9 × 10⁻⁴ S/cm. Battery testing involved charging/discharging at various constant current values (0.6–2.0 mA), using Pt/C as the catalyst and seawater as the catholyte. Full article

The key objective of this study is to determine the effect of interphase boundaries, the formation of which is caused by the variation of Li₂ZrO₃/MgLi₂ZrO₄ phases in lithium-containing ceramics based on lithium metazirconate, on the resistance to near-surface layer destruction processes associated with irradiation with He²⁺ ions. During the observation of the deformation effects that have an adverse impact on the volumetric swelling of the near-surface layers of ceramics, the thermal expansion factor caused by high-temperature irradiation was considered, simulating conditions as close as possible to the operating conditions of these materials as blankets for tritium propagation. During the studies conducted, it was established that an elevation in the contribution of MgLi₂ZrO₄ in the composition of ceramics leads to a rise in resistance to deformation swelling caused by structural distortions of the crystal lattice, due to a decrease in the effect of thermal expansion, alongside the presence of interphase boundaries. The established dependencies of the change in the hardness of the near-surface layer of the studied ceramics made it possible to establish the kinetics of softening caused by the deformation distortion of the crystalline structure, as well as to determine the relationship between volumetric swelling and softening (change in hardness) and a decrease in crack resistance (change in the value of resistance to single compression). Full article

Although in general ions are not able to migrate in the solid-state position due to rigid skeletal structure, in some solid electrolytes with a low energy barrier and high ionic conductivities, these ion transition can occur. In this work, we considered several solid electrolytes including lithium phosphorus oxy-nitride (LIPON), a lithium super-ionic conductor (SILICON), and thio-LISICON. For the fabrication and characterization of the solid electrolyte’s fabrication, we used a single-step ball milling (SSBM) procedure. Through this research on all-solid-state rechargeable lithium-ion batteries, our target is to discuss solving several problems in solid LIBs that have recently escalated due to raised concerns relating to safety hazards such as solvent leakage and the flammability of the liquid electrolytes used for commercial LIBs. Through this research, we tested the conductivity amounts of various substrates containing amorphous glass, SSBM, and glass-ceramic samples. Obviously, the SSBM glass-ceramics increased the conductivity, and we also found that the values for conductivity attained by SSBM were higher than those values for glass-ceramics. Using an SSBM technique, silicon nanoparticles were used as an anode material and it was found that the charge and discharge curves in the battery cell cycled between 0.009 and 1.45 V versus Li⁺/Li at a current density of 210 mA g⁻¹ at room temperature. Since high resistance causes degradation between the cathode material (LiCoO₂) and the solid electrolyte, we added GeS2 and SiS₂ to the Li₂S-P₂S₅ system to obtain higher conductivities and better stability of the electrode–electrolyte interface. Full article

Stabilized Li_6.25La₃Al_0.25 Zr₂O₁₂ (cubic LLZO or c-LLZO) is a Li⁺-conducting ceramic with ionic conductivities approaching 1 mS-cm. Processing c-LLZO so that it is suitable for use as a solid state electrolyte in all solid state batteries, however, is challenging due to the formation of secondary phases at elevated temperatures. The work described in this manuscript examines the formation of one such secondary phase La₂Zr₂O₇ (LZO) formed during sintering c-LLZO at 1000 °C. Specifically, spatially resolved Raman spectroscopy and X-ray Diffraction (XRD) measurements have identified gradients in Li distributions in the Li ion (Li⁺)-conducting ceramic Li_6.25La₃Al_0.25 Zr₂O₁₂ (cubic LLZO or c-LLZO) created by thermal processing. Sintering c-LLZO under conditions relevant to solid state Li⁺ electrolyte fabrication conditions lead to Li⁺ loss and the formation of new phases. Specifically, sintering for 1 h at 1000 °C leads to Li⁺ depletion and the formation of the pyrochlore lanthanum zirconate (La₂Zr₂O₇ or LZO), a material known to be both electronically and ionically insulating. Circular c-LLZO samples are covered on the top and bottom surfaces, exposing only the 1.6 mm-thick sample perimeter to the furnace’s ambient air. Sintered samples show a radially symmetric LZO gradient, with more LZO at the center of the pellet and considerably less LZO at the edges. This profile implies that Li⁺ diffusion through the material is faster than Li⁺ loss through volatilization, and that Li⁺ migration from the center of the sample to the edges is not completely reversible. These conditions lead to a net depletion of Li⁺ at the sample center. Findings presented in this work suggest new strategies for LLZO processing that will minimize Li⁺ loss during sintering, leading to a more homogeneous material with more reproducible electrochemical behavior. Full article

Lithium (Li) metal is one of the most promising anode materials for next-generation, high-energy, Li-based batteries due to its exceptionally high specific capacity and low reduction potential. Nonetheless, intrinsic challenges such as detrimental interfacial reactions, significant volume expansion, and dendritic growth present considerable obstacles to its practical application. This review comprehensively summarizes various recent strategies for the modification and protection of metallic lithium anodes, offering insight into the latest advancements in electrode enhancement, electrolyte innovation, and interfacial design, as well as theoretical simulations related to the above. One notable trend is the optimization of electrolytes to suppress dendrite formation and enhance the stability of the electrode–electrolyte interface. This has been achieved through the development of new electrolytes with higher ionic conductivity and better compatibility with Li metal. Furthermore, significant progress has been made in the design and synthesis of novel Li metal composite anodes. These composite anodes, incorporating various additives such as polymers, ceramic particles, and carbon nanotubes, exhibit improved cycling stability and safety compared to pure Li metal. Research has used simulation computing, machine learning, and other methods to achieve electrochemical mechanics modeling and multi-field simulation in order to analyze and predict non-uniform lithium deposition processes and control factors. In-depth investigations into the electrochemical reactions, interfacial chemistry, and physical properties of these electrodes have provided valuable insights into their design and optimization. It systematically encapsulates the state-of-the-art developments in anode protection and delineates prospective trajectories for the technology’s industrial evolution. This review aims to provide a detailed overview of the latest strategies for enhancing metallic lithium anodes in lithium-ion batteries, addressing the primary challenges and suggesting future directions for industrial advancement. Full article

Recent advances in all-solid-state battery (ASSB) research have significantly addressed key obstacles hindering their widespread adoption in electric vehicles (EVs). This review highlights major innovations, including ultrathin electrolyte membranes, nanomaterials for enhanced conductivity, and novel manufacturing techniques, all contributing to improved ASSB performance, safety, and scalability. These developments effectively tackle the limitations of traditional lithium-ion batteries, such as safety issues, limited energy density, and a reduced cycle life. Noteworthy achievements include freestanding ceramic electrolyte films like the 25 μm thick Li_0.34La_0.56TiO₃ film, which enhance energy density and power output, and solid polymer electrolytes like the polyvinyl nitrile boroxane electrolyte, which offer improved mechanical robustness and electrochemical performance. Hybrid solid electrolytes combine the best properties of inorganic and polymer materials, providing superior ionic conductivity and mechanical flexibility. The scalable production of ultrathin composite polymer electrolytes shows promise for high-performance, cost-effective ASSBs. However, challenges remain in optimizing manufacturing processes, enhancing electrode-electrolyte interfaces, exploring sustainable materials, and standardizing testing protocols. Continued collaboration among academia, industry, and government is essential for driving innovation, accelerating commercialization, and achieving a sustainable energy future, fully realizing the transformative potential of ASSB technology for EVs and beyond. Full article

The study investigates alterations in the mechanical and thermophysical properties of ceramics composed of xLi₂ZrO₃–(1−x)Li₄SiO₄ as radiation damage accumulates, mainly linked to helium agglomeration in the surface layer. This research is motivated by the potential to develop lithium-containing ceramics characterized by exceptional strength properties and a resistance to the accumulation of radiation damage and ensuing deformation distortions in the near-surface layer. The study of the radiation damage accumulation processes in the near-surface layer was conducted through intense irradiation of ceramics using He²⁺ ions at a temperature of 700 °C, simulating conditions closely resembling operation conditions. Following this, a correlation between the accumulation of structural modifications (value of atomic displacements) and variations in strength and thermophysical characteristics was established. During the research, it was observed that two-component ceramics exhibit significantly greater resistance to external influences and damage accumulation related to radiation exposure compared to their single-component counterparts. Furthermore, the composition that provides the highest resistance to softening in two-component ceramics is an equal ratio of the components of 0.5Li₂ZrO₃–0.5Li₄SiO₄ ceramics. Full article

High-entropy materials (HEMs) constitute a revolutionary class of materials that have garnered significant attention in the field of materials science, exhibiting extraordinary properties in the realm of energy storage. These equimolar multielemental compounds have demonstrated increased charge capacities, enhanced ionic conductivities, and a prolonged cycle life, attributed to their structural stability. In the anode, transitioning from the traditional graphite (372 mAh g⁻¹) to an HEM anode can increase capacity and enhance cycling stability. For cathodes, lithium iron phosphate (LFP) and nickel manganese cobalt (NMC) can be replaced with new cathodes made from HEMs, leading to greater energy storage. HEMs play a significant role in electrolytes, where they can be utilized as solid electrolytes, such as in ceramics and polymers, or as new high-entropy liquid electrolytes, resulting in longer cycling life, higher ionic conductivities, and stability over wide temperature ranges. The incorporation of HEMs in metal–air batteries offers methods to mitigate the formation of unwanted byproducts, such as Zn(OH)₄ and Li₂CO₃, when used with atmospheric air, resulting in improved cycling life and electrochemical stability. This review examines the basic characteristics of HEMs, with a focus on the various applications of HEMs for use as different components in lithium-ion batteries. The electrochemical performance of these materials is examined, highlighting improvements such as specific capacity, stability, and a longer cycle life. The utilization of HEMs in new anodes, cathodes, separators, and electrolytes offers a promising path towards future energy storage solutions with higher energy densities, improved safety, and a longer cycling life. Full article

The solid oxide electrolyte Li_1.5Al_0.5Ge_1.5(PO₄)₃ (LAGP) with a NASICON structure has a high bulk ionic conductivity of 10⁻⁴ S cm⁻¹ at room temperature and good stability in the air because of the strong P⁵⁺-O²⁻ covalence bonding. However, the Ge⁴⁺ ions in LAGP are quickly reduced to Ge³⁺ on contact with the metallic lithium anode, and the LAGP ceramic has insufficient physical contact with the electrodes in all-solid-state batteries, which limits the large-scale application of the LAGP electrolyte in all-solid-state Li-metal batteries. Here, we prepared flexible PEO/LiTFSI/LAGP composite electrolytes, and the introduction of LAGP as a ceramic filler in polymer electrolytes increases the total ionic conductivity and the electrochemical stability of the composite electrolyte. Moreover, the flexible polymer shows good contact with the electrodes, resulting in a small interfacial resistance and stable cycling of all-solid-state Li-metal batteries. The influence of the external pressure and temperature on Li⁺ transfer across the Li/electrolyte interface is also investigated. Full article