RESUMEN

Solid polymer electrolytes (SPEs) are crucial in the development of lithium metal batteries. Recently, metal-organic frameworks (MOFs) with open metal sites (OMSs) have shown promise as solid fillers to improve the performance of SPEs. However, the number of OMS-containing MOFs is quite limited, comprising less than 5% of the total MOFs. When considering yield, cost, and processability, the commonly used OMS-containing MOFs are no more than 10 types, causing great limitations. Herein, we reported a simple and universal methodology that converted OMS-free MOFs to OMS-rich quasi-MOFs for developing high-performance SPEs, and explored the underlying mechanism. The "OMS-polymer" and "OMS-ion" interactions were investigated in detail to elucidate the role of quasi-MOFs on battery performance. It was found that quasi-MOFs, functioning as ion sieves, can effectively regulate ion migration, thus promoting uniform Li deposition and enabling an ultra-stable interface. As a result, the Li symmetric cell stably ran over 3000 h at 0.3 mA cm-2, while the full cell retained 85% of its initial capacity after 1500 cycles at 1.0 C. Finally, universal testing was performed using other MOFs, confirming the generalizability and effectiveness of our design concept.

RESUMEN

Multifunctional structural batteries promise advancements in structural energy storage technologies by seamlessly integrating load-bearing and energy-storage functions within a single material, reducing weight, and enhancing safety. Yet, commercialization faces challenges in materials processing, assembly, and design optimization. Here, we report a systematic approach to develop a carbon fiber (CF)-based structural battery impregnated with epoxy-based solid polymer electrolyte (SPE) via robust vacuum-assisted compression molding (VACM). Informed by cure kinetics, SPE processing enhances the multifunctional performance with no fillers or additives. The thin flexible CF-based laminae impregnated under high pressure achieved a substantial enhancement of ∼160% in the fiber volume fraction (FVF) as although thin and strip-shaped, the fibers were optimally packed with low void. A CF/SPE-based battery was fabricated, with a hybrid layered ionic liquid (IL)/ carbonate electrolyte (CE) showing enhanced safety and multifunctional performance. Enhanced by thin, uniform, and stiff CF-based composites, this study propels the development of advanced multifunctional structures, thereby expediting sustainable commercialization.

RESUMEN

Lithium-ion batteries (LIBs) have revolutionized the energy storage landscape and are the preferred power source for various applications, ranging from portable electronics to electric vehicles. The constant drive and growth in battery research and development aim to enhance their performance, energy density, and safety. Advanced lithium batteries (LIBs) are considered to be the most promising electrochemical storage devices, which can provide high specific energy, volumetric energy density, and power density. However, the trade-off between ionic conductivity and cycling stability is still a major contradiction for SPEs. In this work, a novel hydroxylated PAF-1 was designed and synthesized through post-modification, and the lithium-rich single-ion porous aromatic framework PAF-1-OLi was thereafter prepared by lithiation, achieved with a specific surface area to be 155 m2 g-1 and a lithium content of 2.01 mmol g-1. PAF-1-OLi, lithium bis(trifluoromethanesulfony)limine (LiTFSI), and poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP) were compounded to obtain PAF-1-OLi/PVDF by solution casting, which had good mechanical, thermodynamic, and electrochemical properties. The ion conductivity of PAF-1-OLi/PVDF infiltrated with plasticizer was 2.93 × 10-4 S cm-1 at 25 °C. The tLi+ was 0.77, which was much higher than that of the traditional dual-ion polymer electrolytes. The electrochemical window of PAF-1-OLi/PVDF can reach 4.9 V. The Li//PAF-1-OLi/PVDF//LiFePO4 battery initial discharge specific capacity was 147 mAh g-1 and reached 134.9 mAh g-1 after 600 cycles with a capacity retention rate of 91.2%, demonstrating its good cycling stability. The anionic part of lithium salt was fixed on the framework of PAF-1 to increase the Li+ transfer number of PAF-1-OLi/PVDF. The lithium-rich PAF-1-OLi and the LiTFSI provided abundant Li+ sources to transfer, while PAF-1-OLi helped to form a continuous Li+ transport channel, effectively promoting the migration of Li+ in the PAF-1-OLi/PVDF and effectively improving the Li+ conductivity. This study afforded a novel polymer electrolyte based on lithium-rich PAF-1-OLi, which has excellent electrochemical performance, providing a new choice for the polymer electrolyte of lithium batteries.

RESUMEN

Solid-state lithium-sulfur batteries (SSLSBs) have attracted a great deal of attention because of their high theoretical energy density and intrinsic safety. However, their practical applications are severely impeded by slow redox kinetics and poor cycling stability. Herein, we revealed the detrimental effect of aggregation of lithium polysulfides (LiPSs) on the redox kinetics and reversibility of SSLSBs. As a paradigm, we introduced a multifunctional hyperbranched ionic conducting (HIC) polymer serving as a solid polymer electrolyte (SPE) and cathode binder for constructing SSLSBs featuring high electrochemical activity and high cycling stability. It is demonstrated that the unique structure of the HIC polymer with numerous flexible ether oxygen dangling chains and fast segmental relaxation enables the dissociation of LiPS clusters, facilitates the conversion kinetics of LiPSs, and improves the battery's performance. A Li|HIC SPE|HIC-S battery, in which the HIC polymer acts as an SPE and cathode binder, exhibits an initial capacity of 910.1 mA h gS-1 at 0.1C and 40 °C, a capacity retention of 73.7% at the end of 200 cycles, and an average Coulombic efficiency of approximately 99.0%, demonstrating high potential for application in SSLSBs. This work provides insights into the electrochemistry performance of SSLSBs and provides a guideline for SPE design for SSLSBs with high specific energy and high safety.

RESUMEN

Two-dimensional materials (2D Ms) as fillers have been applied in polyethylene oxide (PEO)-based electrolyte to enhance the low ionic conductivity and poor interface compatibility. However, the randomly dispersed fillers in PEO matrix result in anisotropy of Li+ transportation and insufficent ionic conductivity. Herein, NiFe2O4 (NFO) nanosheets are firstly introduced in polymer matrix to form vertically aligned NFO-PEO (ANFO-PEO) composite solid-state electrolytes (CSEs) through magnetic field-assisted alignment strategy. The vertically aligned NFO/PEO interface in CSEs can construct oriented Li+ transport channels and maximize the utilization of high in-plane conductivity. Meanwhile, the NFO nanosheets with abundant oxygen vacancies could effectively anchor TFSI- to promote the dissociation of Li salts. Furthermore, the optimized Li+ transport flux in CSEs enables homogeneous Li deposition and effectively mitigates the growth of dendrites. Owing to the synergistic effects, the ANFO-PEO CSEs exhibit high ionic conductivity (9.16 × 10-4 S cm-1 at 60 °C) and stable potential window up to 5.0 V vs Li/Li+. Therefore, LiFePO4 in the full cell and pouch cell with ANFO-PEO CSEs could deliver excellent cycling performance (92.78 % capacity retention after 1000 cycles at 0.5C; 96.88 % capacity retention after 105 cycles at 0.1C).

RESUMEN

Solid polymer electrolytes (SPE) and composite polymer electrolytes (CPE) serve as crucial components in all-solid-state energy storage devices. Structural batteries and supercapacitors present a promising alternative for electric vehicles, integrating structural functionality with energy storage capability. However, despite their potential, these applications are hampered by various challenges, particularly in the realm of developing new solid polymer electrolytes that require more investigation. In this study, novel solid polymer electrolytes and composite polymer electrolytes were synthesized using epoxy resin blends, ionic liquid, lithium salt, and alumina nanoparticles and subsequently characterized. Among the formulations tested, the optimal system, designated as L70P30ILE40Li1MAl2 and containing 40 wt.% of ionic liquid and 5.7 wt.% of lithium salt, exhibited exceptional mechanical properties. It displayed a remarkable storage modulus of 1.2 GPa and reached ionic conductivities of 0.085 mS/cm at 60 °C. Furthermore, a proof-of-concept supercapacitor was fabricated, demonstrating the practical application of the developed electrolyte system.

RESUMEN

The practical application of solid polymer electrolyte is hindered by the small transference number of Li+, low ionic conductivity and poor interfacial stability, which are seriously determined by the microenvironment in polymer electrolyte. The introduction of functional fillers is an effective solution to these problems. In this work, based on density functional theory (DFT) calculations, it is demonstrated that the anion vacancy of filler can anchor anions of lithium salt, thereby significantly increasing the transference number of Li+ in the electrolyte. Therefore, flower-like SnS2-based filler with abundant sulfur vacancies is prepared under the regulation of functionalized carbon dots (CDs). It is worth mentioning that the CDs dotted on the surface of SnS2 have rich organic functional groups, which can serve as the bridging agent to enhance the compatibility of filler and polymer, leading to superior mechanical performance and fast ion transport pathway. Additionally, the in-situ formed Li2S/Li3N at the interface of Li metal and electrolyte facilitate the fast Li+ diffusion and uniform Li deposition, effectively mitigating the growth of lithium dendrites. As a result, the assembled lithium metal batteries exhibit excellent cycling stability, reflecting the superiority of the carbon dots derived vacancy-rich inorganic filler modification strategy.

RESUMEN

A critical challenge in solid polymer lithium batteries is developing a polymer matrix that can harmonize ionic transportation, electrochemical stability, and mechanical durability. We introduce a novel polymer matrix design by deciphering the structure-function relationships of polymer side chains. Leveraging the molecular orbital-polarity-spatial freedom design strategy, a high ion-conductive hyperelastic ternary copolymer electrolyte (CPE) is synthesized, incorporating three functionalized side chains of poly-2,2,2-Trifluoroethyl acrylate (PTFEA), poly(vinylene carbonate) (PVC), and polyethylene glycol monomethyl ether acrylate (PEGMEA). It is revealed that fluorine-rich side chain (PTFEA) contributes to improved stability and interfacial compatibility; the highly polar side chain (PVC) facilitates the efficient dissociation and migration of ions; the flexible side chain (PEGMEA) with high spatial freedom promotes segmental motion and interchain ion exchanges. The resulting CPE demonstrates an ionic conductivity of 2.19×10-3 S cm-1 (30 °C), oxidation resistance voltage of 4.97 V, excellent elasticity (2700 %), and non-flammability. The outer elastic CPE and the inner organic-inorganic hybrid SEI buffer intense volume fluctuation and enable uniform Li+ deposition. As a result, symmetric Li cells realize a high CCD of 2.55 mA cm-2 and the CPE-based Li||NCM811 full cell exhibits a high-capacity retention (~90 %, 0.5 C) after 200 cycles.

RESUMEN

Extensively-used rechargeable lithium-ion batteries (LIBs) face challenges in achieving high safety and long cycle life. To address such challenges, ultrathin solid polymer electrolyte (SPE) is fabricated with reduced phonon scattering by depositing the composites of ionic-liquid (1-ethyl-3-methylimidazolium dicyamide, EMIM:DCA), polyurethane (PU) and lithium salt on the polyethylene separator. The robust and flexible separator matrix not only reduces the electrolyte thickness and improves the mobility of Li+, but more importantly provides a relatively regular thermal diffusion channel for SPE and reduces the external phonon scattering. Moreover, the introduction of EMIM:DCA successfully breaks the random intermolecular attraction of the PU polymer chain and significantly decreases phonon scattering to enhance the internal thermal conductivity of the polymer. Thus, the thermal conductivity of the as-obtained SPE increases by approximately six times, and the thermal runaway (TR) of the battery is effectively inhibited. This work demonstrates that optimizing thermal safety of the battery by phonon engineering sheds a new light on the design principle for high-safety Li-ion batteries.

RESUMEN

Solid polymer electrolytes have been considered as promising candidates for solid-state batteries (SSBs), owing to their excellent interfacial compatibility and high mechanical toughness; however, they suffer from intrinsic low ionic conductivity (lower than 10-6 S/cm) and large thickness (usually surpassed over 100 µm or even 500 µm), which has a negative influence on the interface resistance and ionic migration. In this work, ceria quantum dot (CQD)-modified composite polymer electrolyte (CPE) membranes with a thickness of 20 µm were successfully manufactured via 3D printing technology. The CQD fillers can reduce the crystallinity of the polymer, and the oxygen vacancies on CQDs can facilitate the dissociation of ion pairs in the NaTFSI salt to release more free Na+, improving the ionic conductivity. Meanwhile, tailoring the thickness of the CPE-CQDs membrane via 3D printing can further promote the migration and transport of Na+. Furthermore, the printed NNM//CPE-CQDs//Na SSB exhibited outstanding rate capability and cycling stability. The combination of CQD modification and thickness tailoring through 3D printing paves a new avenue for achieving high performance solid electrolyte membranes for practical application in Na SSBs.

RESUMEN

Polyether-based polymer electrolytes are attractive but still challenging for high-energy-density solid-state lithium metal batteries due to their limited Li-ion conductivity at room temperature. Herein, an oligomeric polyethylene glycol methyl ether methacrylate (PEGMEM)-modified silica-coated polyimide fibrous scaffold (PINF@PEGMEM-SiO2) was introduced in polyethylene glycol dimethyl ether (PEGDME) to enhance the Li-ion transportation at room temperature. PINF@PEGMEM-SiO2 was developed to build a continuous and interconnected interface for continuous Li-ion transportation in bulk. The carbonyl groups (C═O) of PEGMEM on SiO2 can promote the dissociation of lithium salts and enhance the migration of free Li ions at the interface. The same -C-C-O- unit contained in both PEGMEM and PEGDME ensures the compatibility of PEGMEM at the interface and PEGDME in the bulk. The prepared PEGDME-based polymer electrolyte exhibits a high ionic conductivity of 1.14 × 10-4 S cm-1 at 25 °C and an improved Li-ion transference number of 0.41. Furthermore, LiFePO4/Li and LiNi0.8Co0.1Mn0.1O2/Li cells with excellent cyclability and rate capability at ambient temperature are obtained.

RESUMEN

Solid polymer electrolytes (SPEs) are the key components of lithium metal batteries to overcome the obstacle of insecurity in conventional liquid electrolytes; however, the trade-off between their ionic conductivity and mechanical properties remains a significant challenge. In this work, two-dimensional ZSM-5 nanosheets as fillers are incorporated into a poly(ethylene oxide) (PEO) matrix and lithium salts to obtain composite polymer electrolytes (CPEs). The improved physicochemical and electrochemical properties of the CPE membranes are characterized in full detail. Stripping/plating measurements in symmetric Li/Li cells and cyclic charge/discharge tests are performed to investigate the cyclability and stability of the CPEs. All-solid-state LiFePO4/Li batteries deliver excellent cycling performance with an initial discharge capacity of 152.3 mAh g-1 and 91.4% capacity retention after 200 cycles at 0.2 C, with a discharge specific capacity of 118.8 mAh g-1 remaining after 350 cycles at 0.5 C. Therefore, CPEs containing ZSM-5 nanosheets are a promising option for all-solid-state lithium-ion batteries.

RESUMEN

Elastomeric solid polymer electrolytes (SPEs) are highly promising to address the solid-solid-interface issues of solid-state lithium metal batteries (LMBs), but compromises have to be made to balance the intrinsic trade-offs among their conductive, resilient and recyclable properties. Here, we propose a dual-bond crosslinking strategy for SPEs to realize simultaneously high ionic conductivity, elastic resilience and recyclability. An elastomeric SPE is therefore designed with hemiaminal dynamic covalent networks and Li+-dissociation co-polymer chains, where the -C-N- bond maintains the load-bearing covalent network under stress but is chemically reversible through a non-spontaneous reaction, the weaker intramolecular hydrogen bond is mechanically reversible, and the soft chains endow the rapid ion conduction. With this delicate structure, the optimized SPE elastomer achieves high elastic resilience without loading-unloading hysteresis, outstanding ionic conductivity of 0.2 mS cm-1 (25 °C) and chemical recyclability. Then, exceptional room-temperature performances are obtained for repeated Li plating/stripping tests, and stable cycling of LMBs with either LiFePO4 or 4.3 V-class LiFe0.2Mn0.8PO4 cathode. Furthermore, the recycled and reprocessed SPEs can be circularly reused in LMBs without significant performance degradation. Our findings provide an inspiring design principle for SPEs to address the solid-solid-interface and sustainability challenges of solid-state LMBs.

RESUMEN

As miniaturization of semiconductor memory devices is reaching its physical and technological limits, there is a demand for memory technologies that operate on new principles. Atomic switches are nanoionic devices that show repeatable resistive switching between high-resistance and low-resistance states under bias voltage applications, based on the transport of metal ions and redox reactions in solids. Their essential structure consists of an ion conductor sandwiched between electrochemically active and inert electrodes. This review focuses on the resistive switching mechanism of atomic switches that utilize a solid polymer electrolyte (SPE) as the ion conductor. Owing to the superior properties of polymer materials such as mechanical flexibility, compatibility with various substrates, and low fabrication costs, SPE-based atomic switches are a promising candidate for the next-generation of volatile and nonvolatile memories. Herein, we describe their operating mechanisms and key factors for controlling the device performance with different polymer matrices. In particular, the effects of moisture absorption in the polymer matrix on the resistive switching behavior are addressed in detail. As potential applications, atomic switches with inkjet-printed SPE and quantum conductance behavior are described. SPE-based atomic switches also have great potential in use for neuromorphic devices. The development of these devices will be enhanced using nanoarchitectonics concepts, which integrate functional materials and devices.

This article reviews a series of works starting with the author's 2011 paper on solid polymer electrolyte-based atomic switches, and describes the current status and future prospects for this technology.

RESUMEN

Solid-state polymer-based electrolytes (SSPEs) exhibit great possibilities in realizing high-energy-density solid-state lithium metal batteries (SSLMBs). However, current SSPEs suffer from low ionic conductivity and unsatisfactory interfacial compatibility with metallic Li because of the high crystallinity of polymers and sluggish Li+ movement in SSPEs. Herein, differing from common strategies of copolymerization, a new strategy of constructing a high-entropy SSPE from multivariant polymeric ligands is proposed. As a protocol, poly(vinylidene fluoride-co-hexafluoropropylene) (PH) chains are grafted to the demoed polyethylene imine (PEI) with abundant -NH2 groups via a click-like reaction (HE-PEIgPHE). Compared to a PH-based SSPE, our HE-PEIgPHE shows a higher modulus (6.75 vs 5.18 MPa), a higher ionic conductivity (2.14 × 10-4 vs 1.03 × 10-4 S cm-1), and a higher Li+ transference number (0.55 vs 0.42). A Li|HE-PEIgPHE|Li cell exhibits a long lifetime (1500 h), and a Li|HE-PEIgPHE|LiFePO4 cell delivers an initial capacity of 160 mAh g-1 and a capacity retention of 98.7%, demonstrating the potential of our HE-PEIgPHE for the SSLMBs.

RESUMEN

Solid-state batteries based on lithium metal anodes, solid electrolytes, and composite cathodes constitute a promising battery concept for achieving high energy density. Charge carrier transport within the cells is governed by solid-solid contacts, emphasizing the importance of well-designed interfaces. A key parameter for enhancing the interfacial contacts among electrode active materials and electrolytes comprises externally applied pressure onto the cell stack, particularly in the case of ceramic electrolytes. Reports exploring the impact of external pressure on polymer-based cells are, however, scarce due to overall better wetting behavior. In this work, the consequences of externally applied pressure in view of key performance indicators, including cell longevity, rate capability, and limiting current density in single-layer pouch-type NMC622||Li cells, are evaluated employing cross-linked poly(ethylene oxide), xPEO, and cross-linked cyclodextrin grafted poly(caprolactone), xGCD-PCL. Notably, externally applied pressure substantially changes the cell's electrochemical cycling performance, strongly depending on the mechanical properties of the considered polymers. Higher external pressure potentially enhances electrode-electrolyte interfaces, thereby boosting the rate capability of pouch-type cells, despite the fact that the cell longevity may be reduced upon plastic deformation of the polymer electrolytes when passing beyond intrinsic thresholds of compressive stress. For the softer xGCD-PCL membrane, cycling of cells is only feasible in the absence of external pressure, whereas in the case of xPEO, a trade-off between enhanced rate capability and minimal membrane deformation is achieved at cell pressures of ≤0.43 MPa, which is considerably lower and more practical compared to cells employing ceramic electrolytes with ≥5 MPa external pressure.

RESUMEN

High ionic conductivity, outstanding mechanical stability, and a wide electrochemical window are the keys to the application of solid-state lithium metal batteries (LMBs). Due to their regular channels for ion transport and tailored functional groups, covalent organic frameworks (COFs) have been applied to solid electrolytes to improve their performance. Herein, we report a flexible polyethylene oxide-COF-LZU1 (abbreviated as PEO-COF) electrolyte membrane with a high lithium ion transference number and satisfactory mechanical strength, allowing for dendrite-free and long-time cycling for LMBs. Benefiting from the interaction between bis(triflfluoromethanesulonyl)imide anions (TFSI-) and aldehyde groups in COF-LZU1, the Li+ transference number of the PEO-5% COF-LZU1 electrolyte reached up to 0.43, much higher than that of neat PEO electrolyte (0.18). Orderly channels are conducive to the homogenous Li-+ deposition, thereby inhibiting the lithium dendrites. The assembled LiFePO4|PEO-5% COF-LZU1/Li cells delivered a discharge specific capacity of 146 mAh g-1 and displayed a capacity retention of 80% after 200 cycles at 0.1 C (60 °C). The Li/Li symmetrical cells of the PEO-5% COF-LZU1 electrolyte presented a longer working stability at different current densities compared to that of the PEO electrolyte. Therefore, the enhanced comprehensive performance of the solid electrolyte shows potential application prospects for use in LMBs.

RESUMEN

Quasi-solid polymer electrolyte (QPE) lithium (Li)-metal battery holds significant promise in the application of high-energy-density batteries, yet it suffers from low ionic conductivity and poor oxidation stability. Herein, a novel self-built electric field (SBEF) strategy is proposed to enhance Li+ transportation and accelerate the degradation dynamics of carbon-fluorine bond cleavage in LiTFSI by optimizing the termination of MXene. Among them, the SBEF induced by dielectric Nb4C3F2 MXene effectively constructs highly conductive LiF-enriched SEI and CEI stable interfaces, moreover, enhances the electrochemical performance of the QPE. The related Li-ion transfer mechanism and dual-reinforced stable interface are thoroughly investigated using ab initio molecular dynamics, COMSOL, XPS depth profiling, and ToF-SIMS. This comprehensive approach results in a high conductivity of 1.34 mS cm-1, leading to a small polarization of approximately 25 mV for Li//Li symmetric cell after 6000 h. Furthermore, it enables a prolonged cycle life at a high voltage of up to 4.6 V. Overall, this work not only broadens the application of MXene for QPE but also inspires the great potential of the self-built electric field in QPE-based high-voltage batteries.

RESUMEN

The potential applications of epoxy-based solid polymer electrolytes are continually expanding because of their versatile characteristics. These characteristics include mechanical rigidity, nonvolatility, nonflammability, and electrochemical stability. However, it is worth noting that pure epoxy-based solid polymer electrolytes inherently exhibit lower ion transport capabilities when compared to traditional liquid electrolytes. Striking a balance between high mechanical integrity and superior ionic conductivity at room temperature poses a significant challenge. In light of this challenge, this review is dedicated to elucidating the fundamental concepts of epoxy-based solid polymer electrolytes. It will explore various preparation techniques, the incorporation of different nanomaterials into epoxy-based solid polymer electrolytes, and an evaluation of their multifunctional properties. This comprehensive evaluation will cover both mechanical and electrical properties with a specific focus on their potential applications in batteries and structural supercapacitors.

RESUMEN

Solid-state lithium metal batteries (LMBs), constructed through the in situ fabrication of polymer electrolytes, are considered a critical strategy for the next-generation battery systems with high energy density and enhanced safety. However, the constrained oxidation stability of polymers, such as the extensively utilized polyethers, limits their applications in high-voltage batteries and further energy density improvements. Herein, an in situ fabricated fluorinated and crosslinked polyether-based gel polymer electrolyte, FGPE, is presented, exhibiting a high oxidation potential (5.1 V). The fluorinated polyether significantly improves compatibility with both lithium metal and high-voltage cathode, attributed to the electron-withdrawing -CF3 group and the generated LiF-rich electrolyte/electrode interphase. Consequently, the solid-state Li||LiNi0.6Co0.2Mn0.2O2 batteries employing FGPE demonstrate exceptional cycling performances of 1000 cycles with 78 % retention, representing one of the best results ever reported for polymer electrolytes. Moreover, FGPE enables batteries to operate at 4.7 V, realizing the highest operating voltage of polyether-based batteries to date. Notably, our designed in situ FGPE provides the solid-state batteries with exceptional cycling stability even at practical conditions, including high cathode loading (21 mg cm-2) and industry-level 18650-type cylindrical cells (1.3 Ah, 500 cycles). This work provides critical insights into the development of oxidation-stable polymer electrolytes and the advancement of practical high-voltage LMBs.