Search Results (442)

Metal anodes promise improvements in energy density and cost; however, their performance is determined within the first several nanometers at the interface. This review reports on how polymer-based artificial solid electrolyte interphases (SEIs) are engineered to stabilize Li and aqueous-Zn anodes, and how these designs are now evaluated against operando readouts rather than post-mortem snapshots. We group the related molecular strategies into three classes: (i) side-chain/ionomer chemistry (salt-philic, fluorinated, zwitterionic) to increase cation selectivity and manage local solvation; (ii) dynamic or covalently cross-linked networks to absorb microcracks and maintain coverage during plating/stripping; and (iii) polymer–ceramic hybrids that balance modulus, wetting, and ionic transport characteristics. We then benchmark these choices against metal-specific constraints—high reductive potential and inactive Li accumulation for Li, and pH, water activity, corrosion, and hydrogen evolution reaction (HER) for Zn—showing why a universal preparation method is unlikely. A central element is a system of design parameters and operando metrics that links material parameters to readouts collected under bias, including the nucleation overpotential (η_nuc), interfacial impedance (charge transfer resistance (R_ct)/SEI resistance (R_SEI)), morphology/roughness statistics from liquid-cell or cryogenic electron microscopy (Cryo-EM), stack swelling, and (for Li) inactive-Li inventory. By contrast, planar plating/stripping and HER suppression are primary success metrics for Zn. Finally, we outline parameters affecting these systems, including the use of lean electrolytes, the N/P ratio, high areal capacity/current density, and pouch-cell pressure uniformity, and discuss closed-loop workflows that couple molecular design with multimodal operando diagnostics. In this view, polymer artificial SEIs evolve from curated “recipes” into predictive, transferable interfaces, paving a path from coin-cell to prototype-level Li- and Zn-metal batteries. Full article

Solid polymer and composite polymer electrolytes have been investigated as a replacement for liquid electrolytes in lithium batteries and have shown promising conductivities at room temperature. However, the literature reports often do not fully investigate the effects of residual solvent or testing apparatus conditions, leading to discrepancies in reported performance and possible conflation of conductivity values. Using combinations of poly (vinylidene fluoride-co-hexafluoropropylene), succinonitrile, and lithium lanthanum zirconium tantalum oxide, this work aims to develop an understanding of how polymer electrolyte composition, including solvent retention, affects conductivity. A custom-designed controllable pressure test fixture was utilized to determine ionic conductivity of the composite polymer electrolyte films at a wide range of pressures (1.5–18.7 psi) and temperatures 10–90 °C. Applied pressure during testing greatly influences apparent conductivities, with optimal composite film conductivity values ranging from 1.2 × 10⁻⁵ to 4.1 × 10⁻⁵ S cm⁻¹ at room temperature. At elevated temperatures, the composite films achieved greater than 1 mS cm⁻¹. The ideal pressure was found to be dependent on the polymer electrolyte additives. Symmetric cell testing showed over 99% Coulombic efficiency for over one hundred cycles at 0.1 mA cm⁻². The results of this work highlight the importance of careful characterization of electrolyte films and controlled test fixture pressure when developing polymer electrolytes. Full article

Lithium-ion batteries, widely used in phones and electric vehicles, pose safety concerns due to the flammability of conventional liquid electrolytes, which are prone to ignition under elevated temperatures and mechanical stress, increasing the risk of fire. Polymer electrolytes have been employed as a safer solution thanks to their superior thermal stability and mechanical strength. However, despite these advantages, many polymer matrices pose a fire hazard, limiting their potential. This review assesses recent advances in enhancing the flame retardancy of polymer electrolytes through a variety of strategies, namely the incorporation of flame-retardant additives, the addition of nanoscale fillers to improve thermal resistance, and the design of layered or hybrid polymer membrane structures that function as thermal barriers. This review evaluates the effectiveness of these methods, examining their flame-retardancy as well as their influences on ionic conductivity and overall battery performance. By highlighting recent progress and enduring safety challenges in solid-state batteries, it aims to offer insights for developing lithium batteries with enhanced safety and high performance. Full article

Polymer materials have become promising candidates for next-generation energy storage, with structural tunability, multifunctionality, and compatibility with a variety of device platforms. They have a molecular design capable of customizing ion and electron transport routes, integrating redox-active species, and enhancing interfacial stability, surpassing the drawbacks of traditional inorganic systems. New developments have been made in multifunctional polymers that have the ability to combine conductivity, mechanical properties, thermal stability, and self-healing into a single scaffold system, which is useful in battery, supercapacitor, and solid-state applications. By incorporating polymers with carbon nanostructures, ceramics, or two-dimensional materials, hybrid polymer nanocomposites improve electrochemical performance, durability, and mechanical compliance, and the solid polymer electrolytes, as well as artificial solid electrolyte interphases, resolve dendrite growth and safety issues. The multifunctionality also extends to flexibility, stretchability, and miniaturization, which implies that polymers are suitable for use in wearable devices and biomedical devices. At the same time, sustainable polymer innovation focuses on bio-based feedstocks, which can be recycled, and green synthesis pathways. Polymer discovery using artificial intelligence and machine learning is faster than standard methods, predicts structure–property–performance relationships, and can be rationally engineered. Although there are difficulties in stability during long periods, scalability, and trade-offs between indeedness and mechanical endurance, polymers are a promising avenue with regard to dependable, safe, and sustainable power storage. This review presents the molecular strategies, multifunctional uses, and prospects, where polymers are at the center of the next-generation energy technologies. Full article

Aqueous zinc-ion batteries (ZIBs) have attracted growing interest as promising candidates for large-scale and flexible energy storage due to their intrinsic safety, low cost, and environmental sustainability. However, several persistent issues—such as uncontrolled Zn dendrite growth, hydrogen evolution-induced anode corrosion, and cathode dissolution—continue to hinder their commercial deployment. To address these challenges, hydrogel polymer electrolytes (HPEs) have emerged as an effective strategy. Their unique three-dimensional polymer networks not only retain water and confine ion transport, but also provide a solid–liquid hybrid environment that enhances ionic conductivity and interfacial compatibility. These features enable HPEs to suppress side reactions and improve both electrochemical stability and mechanical adaptability, which are especially valuable for flexible ZIB devices. This review first summarizes fundamental energy storage mechanisms in aqueous ZIBs, including reversible Zn²⁺ insertion/extraction, proton co-insertion, and cathode phase evolution. It then highlights recent progress in HPE design, with emphasis on polyacrylamide (PAM), polyvinyl alcohol (PVA), and polyacrylic acid (PAA)-based systems, with strategies for dendrite suppression, interfacial regulation, and mechanical robustness. Finally, current challenges and future directions are discussed, with a forward-looking perspective on scalable fabrication methods, advanced electrolyte design, and deeper mechanistic understanding necessary to fully realize the potential of HPE-enabled aqueous ZIBs. Full article

Traditional liquid electrolyte batteries face safety concerns such as leakage and flammability, while further optimization has reached a bottleneck. Solid electrolytes are therefore considered a promising solution. Here, a PEO–LiTFSI–LATP (PELT) composite electrolyte was developed by incorporating nanosized Li_1.3Al_0.3Ti_1.7(PO₄)₃ fillers into a polyethylene oxide matrix, effectively reducing crystallinity, enhancing mechanical robustness, and providing additional Li⁺ transport channels. The PELT electrolyte exhibited an electrochemical stability window of 4.9 V, an ionic conductivity of 1.2 × 10⁻⁴ S·cm⁻¹ at 60 °C, and a Li⁺ transference number (tLi+) of 0.46, supporting stable Li plating/stripping for over 600 h in symmetric batteries. More importantly, to address poor electrode–electrolyte contact in conventional layered cells, we proposed an integrated electrode–electrolyte architecture by in situ coating the PELT precursor directly onto LiFePO₄ cathodes. This design minimized interfacial impedance, improved ion transport, and enhanced electrochemical stability. The integrated PELT/LFP battery retained 74% of its capacity after 200 cycles at 1 A·g⁻¹ and showed superior rate capability compared with sandwich-type batteries. These results highlight that coupling LATP-enhanced polymer electrolytes with an integrated architecture is a promising pathway toward high-safety, high-performance solid-state lithium-ion batteries. Full article

MXenes, a rapidly emerging family of two-dimensional transition metal carbides and nitrides, have attracted considerable attention in recent years for their potential in next-generation energy storage technologies. In solid-state batteries (SSBs), they combine metallic-level conductivity (>10³ S cm⁻¹), adjustable surface terminations, and mechanical resilience, which makes them suitable for diverse functions within the cell architecture. Current studies have shown that MXene-based anodes can deliver reversible lithium storage with Coulombic efficiencies approaching ~98% over 500 cycles, while their use as conductive additives in cathodes significantly improves electron transport and rate capability. As interfacial layers or structural scaffolds, MXenes effectively buffer volume fluctuations and suppress lithium dendrite growth, contributing to extended cycle life. In solid polymer and composite electrolytes, MXene fillers have been reported to increase Li⁺ conductivity to the 10⁻³–10⁻² S cm⁻¹ range and enhance Li⁺ transference numbers (up to ~0.76), thereby improving both ionic transport and mechanical stability. Beyond established Ti-based systems, double transition metal MXenes (e.g., Mo₂TiC₂, Mo₂Ti₂C₃) and hybrid heterostructures offer expanded opportunities for tailoring interfacial chemistry and optimizing energy density. Despite these advances, large-scale deployment remains constrained by high synthesis costs (often exceeding USD 200–400 kg⁻¹ for Ti₃C₂T_x at lab scale), restacking effects, and stability concerns, highlighting the need for greener etching processes, robust quality control, and integration with existing gigafactory production lines. Addressing these challenges will be crucial for enabling MXene-based SSBs to transition from laboratory prototypes to commercially viable, safe, and high-performance energy storage systems. Beyond summarizing performance, this review elucidates the mechanistic roles of MXenes in SSBs—linking lithiophilicity, field homogenization, and interphase formation to dendrite suppression at Li|SSE interfaces, and termination-assisted salt dissociation, segmental-motion facilitation, and MWS polarization to enhanced electrolyte conductivity—thereby providing a clear design rationale for practical implementation. Full article

In order to form a solid electrolyte interphase (SEI) layer using aqueous processes, a graphite anode called MG-AQP was designed by wrapping and crosslinking graphite particles with aqueous composites (AQCs), which contained zwitterionic polymer, zwitterion molecules, and lithium salts. First, MG-AQP was used to fabricate a full lithium-ion battery (LIB) cell with Li[Ni_0.8Mn_0.1Co_0.1]O₂ (NMC811) as the cathode, denoted as LIB-MG-AQP//NMC811, to demonstrate its performance via a 0.5 C-rate break-in and 1 C-rate cycling. Accordingly, this showed that LIB-MG-AQP exhibits outstanding cyclic stability. To evaluate its electrochemical performance, MG-AQP and lithium metal were used to fabricate a half cell named LIBs-MG-AQP. According to the initial cyclic voltammetry curve, almost no surface reaction for forming an SEI layer exists in LIBs-MG-AQP, illustrating its high initial coulombic efficiency of 92% at a 0.5 C-rate break-in. These outstanding results are due to the fact that the AQC has fewer cracks, thus blocking solvent molecules from passing from the electrolyte into the graphite anode. This study provides new insights to optimize graphite anodes via 0.5 C-rate break-in rather than conventional SEI formation to save time and energy. Full article

In this work, a novel solid polymer electrolyte with a disordered structure has been designed, combining polyethylene glycol (PEG) as the flexible segments and hexamethylene diisocyanate (HDI) as the rigid segments. The synthesis was realized by alternating flexible PEG with rigid HDI through a peptide bond (–CO–NH–), which disrupts the ordered structures of PEG, generating electron-deficient Lewis acid groups. The pathbreaking introduction of HDI blocks not only bridges links between the PEG molecules but also generates electron-deficient Lewis acid groups. Therefore, the original ordered structures of PEG are disrupted by both the alternating chains between PEG and HDI and the Lewis acid groups. As a result, the PEG_H/L4000 electrolytes (PEG molecular weight of 4000) exhibit a strong anion-capture ability that decreases the crystallinity of polymers, which further achieves a high ionic conductivity close to 10⁻³ S·cm⁻¹ with the lithium-ion transference numbers up to 0.88. The symmetric Li|PEG_H/L4000|Li cells maintain a low and stable voltage polarization for more than 800 h at 0.1 mA·cm⁻². Furthermore, the LiFePO₄|PEG_H/L4000|Li all-solid-state cells perform well both in cycling and rate performances. The design of polymer disordered structures for polymer electrolytes provides a new thought for manufacturing all-solid-state lithium-ion batteries with high safety as well as long life. Full article

The pursuit of sustainable and environmentally benign energy storage solutions has propelled significant interest in organic batteries, which utilize redox-active organic compounds as electrode materials. A pivotal component in determining their electrochemical performance, safety, and long-term stability is the electrolyte. Polymer-based electrolytes (PBEs) have emerged as promising candidates owing to their intrinsic advantages, such as enhanced thermal stability, mechanical integrity, and the mitigation of leakage and flammability risks associated with conventional liquid electrolytes. Unlike previous reviews that broadly cover solid electrolytes, this review specifically focuses on the unique developments of polymer-based electrolytes tailored for organic batteries over the past few years. This review presents a comprehensive overview of the recent progress in PBEs specifically designed for organic battery systems. It systematically examines various categories, including solid polymer electrolytes (SPEs), valued for their structural simplicity and stability; gel polymer electrolytes (GPEs), noted for their high ionic conductivity and processability; and polymer-inorganic composite electrolytes, which synergistically integrate the mechanical flexibility of polymers with the ionic conductivity of inorganic fillers. Additionally, the review delves into the latest advancements in ionogels and poly(ionic liquid) electrolytes, highlighting their potential to overcome existing limitations and enable next-generation battery performance. The article concludes with a critical discussion on prevailing challenges and prospective research directions, emphasizing the importance of advanced material design, interfacial engineering, and sustainable synthesis approaches to facilitate the practical realization of high-performance organic batteries. Full article

Electrolyte-gated transistors (EGTs) have emerged as a highly promising platform for neuromorphic computing and bioelectronics, offering potential solutions to overcome the limitations of the von Neumann architecture. This comprehensive review examines recent advancements in EGT technology, focusing on three critical dimensions: materials, device configurations, and external field regulation strategies. We systematically analyze the development and properties of diverse electrolyte materials, including liquid electrolyte, polymer-based electrolytes, and inorganic solid-state electrolytes, highlighting their influence on ionic conductivity, stability, specific capacitance, and operational characteristics. The fundamental operating mechanisms of EGTs and electric double layer transistors (EDLTs) based on electrostatic modulation and ECTs based on electrochemical doping are elucidated, along with prevalent device configurations. Furthermore, the review explores innovative strategies for regulating EGT performance through external stimuli, including electric fields, optical fields, and strain fields/piezopotentials. These multi-field regulation capabilities position EGTs as ideal candidates for building neuromorphic perception systems and energy-efficient intelligent hardware. Finally, we discuss the current challenges such as material stability, interfacial degradation, switching speed limitations, and integration density. Furthermore, we outline future research directions, emphasizing the need for novel hybrid electrolytes, advanced fabrication techniques, and holistic system-level integration to realize the full potential of EGTs in next-generation computing and bio-interfaced applications. Full article

All-solid-state lithium batteries (ASSLBs) employing Li-rich layered oxide (LLO) cathodes are regarded as promising next-generation energy storage systems owing to their outstanding energy density and intrinsic safety. Polymer-in-salt solid electrolytes (PISSEs) offer advantages such as high room-temperature ionic conductivity, enhanced Li anode interfacial compatibility, and low processing costs; however, their practical deployment is hindered by poor oxidative stability especially under high-voltage conditions. In this study, we report the rational design of a bilayer electrolyte architecture featuring an in situ solidified LiClO₄-doped succinonitrile (LiClO₄–SN) plastic–crystal interlayer between a Li_1.2Mn_0.6Ni_0.2O₂ (LMNO) cathode and a poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based PISSE. This PISSE/SN–LiClO₄ configuration exhibits a wide electrochemical stability window up to 4.7 V vs. Li⁺/Li and delivers a high ionic conductivity of 5.68 × 10⁻⁴ S cm⁻¹ at 25 °C. The solidified LiClO₄-SN layer serves as an effective physical barrier, shielding the PVDF-HFP matrix from direct interfacial contact with LMNO and thereby suppressing its oxidative decomposition at elevated potentials. As a result, the bilayer polymer-based cells with the LMNO cathode demonstrate an initial discharge capacity of ∼206 mAh g⁻¹ at 0.05 C and exhibit good cycling stability with 85.7% capacity retention after 100 cycles at 0.5 C under a high cut-off voltage of 4.6 V. This work not only provides a promising strategy to enhance the compatibility of PVDF-HFP-based electrolytes with high-voltage cathodes through the facile in situ solidification of plastic interlayers but also promotes the application of LMNO cathode material in high-energy ASSLBs. Full article

All-solid-state lithium batteries (ASSLBs) are emerging as a promising alternative to conventional lithium-ion batteries, offering solutions to challenges related to energy density and safety. Their core advancement relies on breakthroughs in solid-state electrolytes (SEs). SEs can be broadly grouped into two main types: inorganic solid electrolytes (ISEs) and organic solid electrolytes (OSEs). ISEs offer high ionic conductivity (0.1~1 mS cm⁻¹), a lithium-ion transference number close to 1, and excellent thermal stability, but their intrinsic brittleness leads to poor interfacial wettability and processing difficulties, limiting practical applications. In contrast, OSEs exhibit good flexibility and interfacial compatibility but suffer from poor ionic conductivity (10⁻⁴~10⁻² mS cm⁻¹) due to high crystallinity at room temperature, in addition to poor thermal stability and weak mechanical integrity, making it difficult to match high-voltage cathodes and suppress lithium dendrite growth. Against this backdrop, the stability of the organic–inorganic interface plays a crucial role. However, challenges such as low overall conductivity and unstable interfaces still limit their performance. This review provides a microscopic perspective on lithium-ion transport pathways across the polymer phase, the inorganic filler phase, and their interfacial regions. It categorizes inert fillers and active fillers, analyzing their structure–performance relationships and emphasizing the synergistic effects of filler dimensionality, surface chemistry, and interfacial interactions. In addition, cutting-edge analytical methods such as time-of-flight secondary ion mass spectrometry (TOF-SIMS) and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) have also been employed and are summarized into their roles for revealing the microstructures and dynamic interfacial behaviors of OICSEs. Finally, future directions are proposed, such as hierarchical pore structure design, surface functionalization, and simulation-guided optimization, aiming to provide theoretical insights and technological strategies for the development of high-performance composite electrolytes for ASSLBs. Full article

High-performance batteries for military and extreme environment applications require alternatives to conventional liquid lithium-ion batteries (LIBs), which suffer from poor low-temperature performance and safety risks. All-solid-state lithium batteries (ASSLBs) offer enhanced safety and superior low-temperature capability. In this work, we designed and fabricated composite solid-state electrolytes using polyvinylidene fluoride (PVDF) and polyacrylic acid (PAA) as polymer matrices, N,N-dimethylformamide (DMF) as the solvent, and lithium bis(trifluoromethane sulfonimide) (LiTFSI) as the lithium salt. Composite solutions with varying PAA mass ratios were prepared. Advanced three-dimensional (3D) printing technology enabled the rapid and precise fabrication of electrolyte membranes. An ionic conductivity of about 2.71 × 10⁻⁴ S cm⁻¹ at 25 °C, high mechanical strength, and good thermal properties can be achieved through component and 3D printing process optimization. Assembled LiCoO₂||PVDF@PAA||Li ASSLBs delivered an initial discharge capacity of 165.3 mAh/g at 0.1 mA cm⁻² (room temperature), maintaining 98% capacity retention after 300 cycles. At 0 °C, these cells provided 157.4 mAh/g initial capacity with 85% retention over 100 cycles at 0.1 mA cm⁻². This work identifies the optimal PAA ratio for enhanced electrochemical performance and demonstrates the viability of 3D printing for advanced ASSLB manufacturing. Full article

Poly(ionic liquids) (PILs) show great promise as a new class of solid electrolytes for energy applications, including high-temperature polymer electrolyte fuel cells, owing to their combination of the unique electrochemical properties of ionic liquids and macromolecular architecture. In this study, we prepared and characterized PIL-based composite polymer electrolyte membranes containing silica nanofibers (SiO₂NFs). The SiO₂NFs were prepared via electrospinning, followed by calcination, and were used as a thermally and mechanically stable, porous substrate. The crosslinked protic PIL was synthesized via in situ radical polymerization of imidazolium hydrogensulfate-based reagents (one monomer and one crosslinker). It was then used as the membrane matrix. The prepared freestanding PIL membranes remained thermally stable at temperatures of up to 180 °C. Furthermore, the PIL/SiO₂NF composite electrolyte membranes demonstrated improved mechanical properties due to reinforcement by the NF framework. These composite membranes also exhibited relatively high proton conductivity (approximately 0.1 to 1 mS/cm) in the 100–150 °C temperature range. Full article