Search Results (153)

All-solid-state lithium–sulfur batteries (ASSLSBs) couple the high theoretical energy density of sulfur (2600 Wh kg⁻¹) with the safety and polysulfide-shuttle suppression advantages of solid electrolytes (SEs). In practice, however, sluggish solid-state conversion kinetics, chemo-mechanical degradation in composite cathodes, and large solid–solid interfacial resistance remain the principal barriers to practical implementation. This review systematically examines recent progress across the three key components of ASSLSBs: cathodes, solid electrolytes, and interfaces. For cathodes, S/C composite design strategies and alternative active materials—including Li₂S, metal sulfides, and organosulfur compounds—are discussed. For solid electrolytes, inorganic (sulfide, oxide, halide, and hydride), polymer, and hybrid composite systems are compared. For interfaces, physical strategies (stack pressure, compliant interlayers, three-dimensional cathode architectures) and chemical strategies (cathode–SE and Li metal–SE interphase engineering, in situ stabilization) are evaluated. Outstanding challenges and design guidelines for next-generation ASSLSBs are discussed. Full article

Sodium-ion-based polymer electrolytes have emerged as an essential technology for the next generation of solid-state batteries, offering the possibility of greater safety and mechanical flexibility. This work aimed to prepare eco-friendly ormolytes based on a biohybrid host matrix, which were doped, for the first time, with a wide range of NaTFSI concentrations. The matrix consists of short poly(ε-caprolactone) segments covalently bonded to siliceous domains via urethane linkages. The samples obtained were thin and transparent films. They were characterized by means of thermogravimetric analysis (TGA) and X-ray diffraction (XRD), and the films exhibited an amorphous character over the entire composition range. Ionic conductivity measurements were performed, and at room temperature for n = 10, the ionic conductivity was 2.44 × 10⁻³ mS.cm⁻¹. The highest ionic conductivity value of 1.78 × 10⁻² mS.cm⁻¹ (n = 10) was obtained at 62.0 °C. To access the cation/urethane interactions, Fourier transform infrared (FT-IR) spectroscopy was employed, and it was noted that the global profile was slightly altered with the incorporation of salt, in which more interactions were observed for the more concentrated samples. Thus, the proposed material may be promising in the development of more sustainable and environmentally friendly electrochemical devices with Na ions. Full article

Limited ionic conductivity and unstable interfaces, primarily caused by poor solid–solid contact, pose significant challenges to the stable cycling of solid-state batteries. In this study, an interfacial in situ polymerization strategy is proposed to construct a poly(1,3-dioxolane) (PDOL) gel electrolyte layer between a poly(vinylidene fluoride) (PVDF)-based solid polymer electrolyte and the electrodes. This approach aims to address interfacial compatibility issues in solid-state lithium metal batteries. By precisely tuning the composition of the gel precursor and employing characterization techniques such as FTIR and NMR, the efficient ring-opening polymerization of 1,3-dioxolane (DOL) was confirmed, achieving a high conversion rate of 90%. The precursor was drop-cast onto the PVDF-based electrolyte/electrode interfaces before cell assembly. Electrochemical evaluations revealed that the in situ formed solidified interlayer significantly enhanced interfacial compatibility and ion transport, yielding a high Li⁺ transference number (0.341), an exceptional critical current density (1.4 mA cm⁻²), and remarkable cycling stability exceeding 1600 h in Li||Li symmetric cells. Furthermore, full cells incorporating LiFePO₄ cathodes demonstrated excellent rate capability and long-term cyclability, retaining 98.7% of their capacity after 1000 cycles. These results collectively underscore the effectiveness of this in situ solidification strategy in optimizing the interface structure and improving the overall performance of PVDF-based solid-state batteries. Full article

In this work, a composite solid polymer electrolyte was prepared for anodic bonding encapsulation. The effects of additives on the anodic bonding performance of the composites were investigated. Characterizations including AC impedance and X-ray diffraction show that CeO₂ and TiO₂ particles reduce the crystallinity of the (PEG)₁₂LiClO₄ matrix, thereby improving ionic conductivity and mechanical properties. The composite of (PEG)₁₂LiClO₄ with 5 wt.% CeO₂ and 5 wt.% TiO₂ achieves a room-temperature ionic conductivity of 1.01 × 10⁻⁵ S·cm⁻¹. Anodic bonding tests and interfacial characterization confirm its optimal bonding performance with aluminum. The interfacial tensile strength reaches 4.65 MPa at room temperature, and element migration is observed across the bonding interface. Full article

In this study, a polyethylene glycol (PEG)-based solid electrolyte composite (PEG)₁₀LiClO₄/NaAlOSiO suitable for anodic bonding packaging was successfully fabricated via a combined ball milling and hot pressing process. The micromorphology, ion transport characteristics, and mechanical packaging properties of the composite were systematically investigated using characterization techniques including electrochemical impedance spectroscopy, X-ray diffraction, scanning electron microscopy, and anodic bonding performance tests. The results demonstrate that doping with NaAlOSiO molecular sieve can effectively reduce the crystallinity of the polymer matrix, construct more efficient carrier transport pathways, and simultaneously enhance the ionic conductivity and mechanical properties of the material. When the mass fraction of NaAlOSiO doping is 8 wt.%, the composite exhibits a room temperature ionic conductivity of up to 1.31 × 10⁻⁵ S·cm⁻¹. Under room temperature and a bonding voltage of 800 V, the sample with this doping ratio achieves the optimal anodic bonding with metallic Al, and the tensile strength of the bonding interface reaches 5.93 MPa, showing excellent application prospects in micro–nano-packaging. Full article

Graphite remains the predominant negative electrode material in commercial lithium-ion batteries (LIBs); however, its practical performance is increasingly limited by interface-driven degradation rather than bulk intercalation. This review examines the interconnected electrochemical, mechanical, and safety challenges associated with uncoated and coated graphite, with particular focus on how solid electrolyte interphase (SEI) formation and evolution deplete cyclable lithium, increase interfacial resistance, and induce polarization that leads to lithium plating and dendritic growth during rapid charging and low-temperature operation. Electrolyte and solvation engineering are highlighted as coating-free strategies to mitigate these issues by reducing Li⁺ desolvation barriers and directing interphase chemistry toward thinner, more ion-conductive, fluorinated SEI films that inhibit plating while maintaining high-rate capability. Coated graphite approaches are compared, including carbon, inorganic, and polymer coatings that function as artificial SEI layers to minimize direct electrolyte contact, stabilize interphase composition, and enhance mechanical durability. Key trade-offs are discussed, including decreased first-cycle coulombic efficiency (FCCE) due to increased surface area, transport limitations arising from excessively thick coatings, nonuniform coverage leading to local current hotspots, and side reactions induced by the coatings. The discussion is further extended to sodium and potassium systems, explaining how larger ion sizes, unfavorable thermodynamics, and significant lattice expansion hinder their insertion into graphite, and summarizing strategies such as interlayer expansion and alternative carbon architectures that improve reversibility for larger ions. This review concludes that achieving durable, safe, and fast-charging graphite electrodes requires an integrated interfacial design that combines optimized graphite morphology, electrode architecture, and electrolyte chemistry. Full article

Solid polymer electrolytes (SPEs) hold great potential in high-safety energy storage but face two key bottlenecks: low room-temperature ionic conductivity and insufficient mechanical strength. This study proposes a synergistic optimization strategy of “long-carbon-chain regulation of polymer microstructure combined with porous polyimide (PI) support”. A linear random copolyester, poly(1,3-propylene-co-1,4-butylene succinate-co-sebacate) (PBPSS), was synthesized via melt polycondensation using 1,3-propanediol, 1,4-butanediol, succinic acid, and sebacic acid as monomers. Subsequently, the PBPSS-75 composite electrolyte was prepared with this copolyester as the matrix and porous PI as support. Results show that long-carbon-chain sebacic acid effectively regulates polymer segment flexibility and free volume, synergistically enhancing ionic conductivity and interfacial mechanical stability with lithium metal. Experimental data indicate that PBPSS-75 composite electrolyte exhibits an ionic conductivity of up to 4.25 × 10⁻⁵ S cm⁻¹ (30 °C), a lithium-ion transference number of 0.81, and an electrochemical stability window of 4.48 V (vs. Li/Li⁺). In LiFePO₄//Li batteries, it maintains nearly 100% capacity retention after 300 cycles at 0.5 C, and achieves stable cycling for over 800 h in lithium symmetric cells. This study confirms that the combined strategy effectively addresses the conductivity-mechanical property trade-off of SPEs, providing theoretical guidance and technical reference for high-performance solid-state battery material design. Full article

Due to its affordability, widespread availability, non-toxicity, biodegradability, and renewability, cellulose is considered a crucial material for addressing the depletion of petroleum resources. In this study, a rotaxane-based supramolecular polymer derived from thermoplastic polyurethane (TPU) was synthesized and combined with cellulose to create a TPU–cellulose composite (TPU-C). This composite was employed as a separator for acrylate-based quasi-solid polymer electrolytes (QPEs). The polymer electrolyte demonstrated a high ionic conductivity of 0.16 mS cm⁻¹ at room temperature, a lithium-ion transference number of 0.63, and an electrochemical stability window extending up to 4.7 V. When paired with a LiFePO₄ (LFP) cathode, the coin cell retained 88.8% of its capacity after 100 cycles at 1 C. A cell assembled with Li and a high-voltage NCM622 cathode maintained a capacity of 65.8% after 100 cycles at 0.3 C. Additionally, the excellent electrochemical performance was analyzed through density functional theory (DFT) calculations to identify the underlying reasons for its outstanding behavior. This study offers new insights into expanding the application potential of cellulose-based composite materials. Full article

A novel Lithium triflate-incorporated Solid Polymer Electrolyte (SPE) has been developed by using the optimized blend of Ghatti Gum (GG) and Xanthan Gum (XG) with a biodegradable synthetic polymer, Polyvinyl alcohol (PVA), ethylene glycol as a plasticizer, and formaldehyde as a cross-linker for energy storage applications. They are examined by X-ray diffraction, Fourier transform infrared spectroscopy, and electrochemical impedance analysis. The frequency-dependent conductivity adheres to Joshner’s universal power law, with the TF10 composition achieving the higher ionic conductivity of 2.73 × 10⁻⁵ S cm⁻¹. Temperature-dependent conductivity confirms Arrhenius-type behavior and shows a low activation energy of 0.15 eV that supports facile ion transport. The conduction process in TF10 follows the Correlated Barrier Hopping (CBH) model. Dielectric and modulus investigations indicate relaxation dynamics with the shorter relaxation time (6.45 × 10⁻⁶ s) from tangent loss spectra. From the SEM analysis, the uniform distribution and the porous nature of the electrode activated carbon are confirmed. A supercapacitor is assembled with TF10 displays electric double-layer capacitive features, delivering a specific capacitance of 7.1 Fg⁻¹ at 15 mVs⁻¹. Charge–discharge analysis reveals energy and power densities of 2.52 Wh kg⁻¹ and 2500 W kg⁻¹, respectively, for the supercapacitor. Full article

This article delineates the electrical characteristics and usefulness of a plasticized polymer electrolyte (PPE) manufactured from PVDF/PEO blends, using varying weight percentages of the plasticizer ethylene carbonate (EC) in conjunction with a liquid electrolyte. Micro-porous solid-state polymer electrolyte membranes were fabricated using the non-solvent-induced phase separation (NIPS) method. The polymer composite membranes modified by the incorporation of a plasticizer (40 weight percent of EC) exhibited enhanced porosity and absorbed a significant quantity of liquid electrolyte (313.3%). A N₂ adsorption isotherm study indicates an increase in pore volume and pore size resulting from the incorporation of EC in PPE. This resulted in a satisfactory level of ionic conductivity (2.08 mS/cm) at 25 °C, attributable to the inclusion of 40 wt.% EC-based PPE, which has a high dielectric constant and a rapid relaxation time. The AC/40 wt.% EC-based PPE/LTO hybrid supercapacitor exhibits a superior specific capacitance, reduced internal resistance, and enhanced retention values after 10,000 cycles in comparison to the AC/10 wt.% EC-based PPE/LTO hybrid supercapacitor. Full article

Gel polymer electrolytes (GPEs), which combine the safety of solid electrolytes with the high ionic conductivity of liquid electrolytes, have long been regarded as ideal electrolyte materials. This study proposes a polymer/ceramics composite gel electrolyte aimed at improving the performance of lithium-ion batteries. A nanofiber membrane was fabricated by electrospinning a mixture of polyacrylonitrile and lithium-salt-grafted helical mesoporous silica nanoparticles, followed by plasticizer absorption to obtain the composite gel electrolyte film (PAN/SiO₂-Li). Experimental results indicate that this gel electrolyte membrane possesses high thermal stability, a wide electrochemical window (>5.3 V vs. Li/Li⁺), high room-temperature ionic conductivity (~4.4 × 10⁻³ S cm⁻¹), and a good lithium-ion transference number (0.72). In symmetric Li||Li cells, this electrolyte suppresses lithium dendrite growth and maintains stable lithium deposition/stripping. This work presents a practical electrolyte design strategy for developing GPEs with enhanced safety and performance. Full article

Poly(ethylene oxide) (PEO)-based solid electrolytes are promising candidates for solid-state lithium metal batteries because of their flexibility and ease of processing. However, their practical application is limited by insufficient mechanical strength and poor interfacial stability. Conventional single-filler strategies typically improve either ionic conductivity or mechanical robustness, making it challenging to simultaneously optimize both properties. In this work, a dual-ceramic strategy is proposed that integrates inert and active ceramic fillers with complementary roles to construct a polymer electrolyte that is both mechanically robust and ionically conductive. The inert ceramic filler promotes lithium-salt dissociation and Li⁺ transport, whereas the active ceramic filler enhances structural integrity and suppresses lithium dendrite growth, enabling a synergistic balance between ionic transport and cycling stability. As a representative implementation, paraelectric SrTiO₃ and Li⁺-conducting Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO) are incorporated into the PEO/LiTFSI matrix to construct a composite solid electrolyte (PLLS). The optimized PLLS electrolyte, containing 8 wt% STO and 5 wt% LLZTO, exhibits a high ionic conductivity of $4.48\times {10}^{-4}\mathrm{S}{\mathrm{cm}}^{-1}$, an increased Li⁺ transference number of 0.20, and a wide electrochemical stability window of 5.165 V versus Li/Li⁺ at 60 °C. Li/Li symmetric cells demonstrate stable lithium plating/stripping for nearly 2000 h at a current density of$0.2\mathrm{mA}{\mathrm{cm}}^{-2}$. Furthermore, LiFePO₄/Li full cells retain 92.1% of their initial capacity after 500 cycles at 1 C, and stable cycling performance is also achieved with high-voltage LiCoO₂ cathodes. These results demonstrate that the proposed dual-ceramic synergistic strategy offers an effective and potentially generalizable approach to enhancing the durability of PEO-based solid electrolytes for long-life solid-state lithium metal batteries. Full article

Waterborne polyurethane (WPU) and waterborne poly(urethane-urea) (WPUU) dispersions allow safer and more sustainable manufacturing of rechargeable batteries via water-based processing, while offering tunable adhesion and segmented-domain mechanics. Beyond conventional roles as binders and coatings, WPU/WPUU chemistries also support separator/interlayer and polymer-electrolyte designs for lithium-ion and lithium metal systems, where interfacial integrity, stress accommodation, and ion transport must be balanced. Here, we review WPU/WPUU fundamentals (building blocks, dispersion stabilization, morphology, and film formation) and review prior studies through a battery-centric structure–processing–property lens. We point out key performance-limiting trade-offs—adhesion versus electrolyte uptake and ionic conductivity versus storage modulus—and relate them to practical formulation variables, including soft-/hard-segment selection, ionic center/counterion design, molecular weight/topology control, and crosslinking strategies. Applications are reviewed for (i) electrode binders (graphite/Si; cathodes such as LFP and NMC), (ii) separator coatings and functional interlayers, and (iii) gel/solid polymer electrolytes and hybrid composites, with a focus on practical design guidelines for navigating these trade-offs. Future advancements in WPU/WPUU chemistries will depend on developing stable, low-impedance interlayers, enhancing electrochemical behavior, and establishing application-specific design guidelines to optimize performance in lithium metal batteries (LMB). Full article

Poly(ethylene oxide) (PEO)-based solid polymer electrolytes typically suffer from limited ionic conductivity at near-room temperature and often require inorganic reinforcement. Halide solid-state electrolytes such as Li₃InCl₆ (LIC) offer fast Li⁺ transport but are moisture-sensitive and typically require pressure-assisted densification. Here, we fabricate a flexible LIC–PEO composite electrolyte via slurry casting in acetonitrile with a small amount of LiPF₆ additive. The free-standing membrane delivers an ionic conductivity of 1.19 mS cm⁻¹ at 35 °C and an electrochemical stability window up to 5.15 V. Compared with pristine LIC, the composite shows improved moisture tolerance, and its conductivity can be recovered by mild heating after exposure. The electrolyte enables stable Li|LIC–PEO|Li cycling for >620 h and supports Li|LIC–PEO|NCM111 cells with capacity retentions of 84.2% after 300 cycles at 0.2 C and 80.6% after 150 cycles at 1.2 C (35 °C). Structural and surface analyses (XRD, SEM/EDX, XPS) elucidate the composite microstructure and interfacial chemistry. Full article

Accurate potentiometric sensing critically depends on the stability and reproducibility of the reference electrode potential. Conventional liquid-filled Ag/AgCl or calomel electrodes, though well-established, are poorly compatible with miniaturized, portable, or long-term in situ sensing devices due to electrolyte leakage, junction potential instability, and maintenance requirements. Recent advances in solid-state and membrane-based reference electrodes offer a promising alternative by eliminating the liquid junction while maintaining stable and well-defined potential. This review summarizes the advancements in polymer-based and composite reference membranes, focusing on material strategies, stabilization mechanisms, and integration approaches. Emphasis is placed on ionic-liquid-doped membranes, conducting polymers, lipophilic salts, and carbon nanomaterials as functional components enhancing interfacial stability and charge transfer. The performances of various architectures, solid-contact, liquid-junction-free, and quasi-reference systems, are compared in terms of potential drift, matrix resistance, biocompatibility, and manufacturability. Furthermore, recent developments in printed, microfluidic, and wearable potentiometric platforms demonstrate how reference membrane innovations enable reliable operation in compact, low-cost, and flexible analytical systems. The review outlines current trends, challenges, and future directions toward universal, miniaturized, and leak-free reference electrodes suitable for innovative sensing technologies. Full article