Solid Polymer Electrolyte Research Articles

3D Printing of solvent-free PEO-Polyolefin solid polymer electrolyte by Fused Filament Fabrication

ABSTRACT 3D printing of energy storage systems is at the heart of In-Space Manufacturing strategy. Within this context, Li-ion polymer batteries printing through Fused Filament Fabrication (FFF) is envisaged. This study is devoted to optimising the extruded solid polymer electrolyte filament properties. As the poly(ethylene oxide) (PEO) – lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) electrolyte offers the best Li+ conductivities but suffers from poor mechanical behaviour, poly(propylene) (PP) is added to ensure filament printability. An exhaustive investigation highlights the impact of the PEO molar weight and the LiTFSI and PP proportions. Fine-tuning these parameters alters molten phase viscosity, which affects the electrolyte morphology and ionic conductivity. Best formulations feature a co-continuous structure that provides effective mechanical reinforcement and exhibits the best ionic conductivity reported so far for an FFF-printed solvent-free polymer electrolyte of 1.2 × 10−4 S.cm−1 at 70°C. Therefore, it opens the way towards polymer battery printing, on the Earth and in microgravity conditions.

Advanced High-Voltage Electrolyte Design Using Poly(ethylene Oxide) and High-Concentration Ionic Liquids for All-Solid-State Lithium-Metal Batteries.

Poly(ethylene oxide) (PEO)-based solid polymer electrolytes (SPEs) are among the most promising materials for solid-state lithium metal batteries (LMBs) due to their inherent safety advantages; however, they suffer from insufficient room-temperature ionic conductivity (up to 10-6 S cm-1) and limited oxidation stability (<4 V). In this study, a novel "polymer-in-high-concentrated ionic liquid (IL)" (PiHCIL) electrolyte composed of PEO, N-propyl-N-methylpyrrolidinium bis(fluorosulfonyl) imide (C3mpyrFSI) IL, and LiFSI is designed. The EO/[Li/IL] ratio has been widely varied, and physical and electrochemical properties have been explored. The Li-coordination and solvation structure has been explored through Fourier-transform infrared spectroscopy and solid-state magic-angle spinning nuclear magnetic resonance. The newly designed electrolyte provides a promisingly high oxidative stability of 5.1 V and offers high ambient temperature ionic conductivity of 5.6 × 10-4 S cm-1 at 30 °C. Li|Li symmetric cell cycling shows very stable and reversible cycling of Li metal over 100 cycles and a smooth dendrite-free deposition morphology. All-solid-state cells using a composite lithium iron phosphate cathode exhibit promising cycling with 99.2% capacity retention at a C/5 rate over 100 cycles. Therefore, the novel approach of PiHCIL enables a new pathway to design high-performing SPEs for high-energy-density all-solid-state LMBs.

Improving supercapacitor performance with novel potato starch-PVA solid polymer electrolyte blend modified by sodium perchlorate-glycerol additives

The synthesis and analysis of Solid Polymer Electrolytes (SPEs) derived from a blend of Potato Starch and Poly Vinyl Alcohol (PS-PVA), enhanced with Sodium perchlorate salt (NaClO4) and Glycerol (GCL) are explored in this work. Our focus is on their suitability for Electrical Double-Layer Capacitor (EDLC) devices. GCL, a non-toxic substance, served as the plasticizer, and sodium perchlorate was incorporated to enhance the ionic conductivity of the SPE film. The conductivity at room temperature for pure PS-PVA blend, in the absence of salt and GCL, was found to be 4.16 × 10−8 S cm−1. Upon adding an optimized quantity of NaClO4 salt, the conductivity increased to 1.02 × 10−5 S cm−1. Subsequent plasticization of the salt-polymer blend with GCL induced NaClO4 dissociation, further augmenting the conductivity by one order of magnitude. A conductivity value of 10.35 × 10−5 S cm−1 was achieved for the film with 30 wt% GCL. Morphological, electrical, and structural analyses revealed that synthesized polymer films exhibited favorable characteristics. The suitability of these electrolytes for Electric Double-Layer Capacitors (EDLC) was studied using electrochemical characterizations and cycling tests for 2000 cycles. The findings demonstrate their potential for use in energy storage devices, showcasing excellent performance in specific capacitance, energy, and power densities.

Fireproof Solid Polymer Electrolyte with Chemically Bonded Phosphorus Toward Stable and Safe Lithium‐Metal Battery

Fireproof Solid Polymer Electrolyte with Chemically Bonded Phosphorus Toward Stable and Safe Lithium‐Metal Battery

Ion-migration-induced synaptic plasticity in high ion-storable fluorine graphdiyne for information processing

Neuromorphic devices encounter constraints associated with complementary metal–oxide–semiconductor technology, such as intricate electronics and high power consumption. Recently, solid polymer electrolytes (SPE) have gained attraction in electronic devices for constructing artificial synapses, primarily due to their low-voltage operation enabled by ion-assisted signal transmission. This study presents a two-terminal artificial synapse fabricated using fluorine graphdiyne (F-GDY) synthesized through chemical vapor deposition and ion-doped SPE. The device architecture consists of Au/SPE/F-GDY/Si, which operates by ion migration induced by external potential pulses. Electrical measurements are conducted to depict the synaptic plasticity of the devices. Among devices employing different ion-doped SPEs (Li-SPE, Na-SPE, K-SPE, and Ca-SPE), the one utilizing Li-SPE demonstrates the highest synaptic weight. This is attributed to the superior Li+ ion storage capacity of F-GDY; hence, Li-SPE/F-GDY was chosen for in-depth examinations of synaptic activity presenting long-term potentiation, short-term depression, and pair-pulse facilitation. The device has good durability and stability and can respond to low action potential with power consumption at the pJ level. Furthermore, Modified National Institute of Standards and Technology simulations reveal its learning and pattern recognition capability with 91.3 % accuracy after 10 training epochs. Finally, flexible substrate-based SPE/F-GDY devices integrated with gate electrodes were fabricated to record physiological signals, showing promise for in-sensing applications. This work shows the potential of F-GDY/Li-SPE devices for low-power neuromorphic computing, though real-time parallel processing and multimodal integration (e.g., visual, auditory) remain unexplored. However, the biocompatibility and efficient ion-assisted transmission of F-GDY suggest promising future applications in these areas.

Lithium Plating Using a Thermoplastic Vulcanizate Electrolyte

Lithium metal anodes have generated significant interest due to their high theoretical capacity. However, issues such as dendrite growth or cell failure caused by lithium loss with either liquid electrolytes or solid polymer electrolytes (SPEs) have hindered its widespread commercialization. In this work, we report on the electrochemical characterization of symmetric Li-SPE-Li cells made with a thermoplastic vulcanizate electrolyte, PCl:HNBR LiTFSI. Full plating of the lithium metal (LiM) electrode was achieved at 100 μA.cm−2 in pressurized pouch cells. This was confirmed ex situ using scanning electron microscopy which showed the absence of dendrites. The Sand equation was employed at higher current densities to determine that the lithium diffusion coefficient at 60 °C is 1.7 × 10−8 cm2.s−1. The calculated threshold current density j* was approximately 200 μA.cm−2. The determination of the theoretical current density limit may provide critical information for the understanding of the behavior of cathode materials during cycling with lithium metal. Cell failure at high polarization or from short circuiting was experimentally confirmed in symmetric Li-Li cells where 100 cycles were performed at a current density below j* with 0.1 mAh.cm−2 of charge per cycle, while 0.5 mAh.cm−2 of charge rapidly induced cell failure.

Tuning Electrochemical Performance of Polymer Electrolyte Films through Metal Oxide Incorporation

AbstractWith the escalating global energy demand, the exploration of alternative, easily accessible, and cost‐effective energy sources has become imperative. The diminishing reserves of conventional energy resources underscore the urgency to transition towards renewable energy. Solid polymer electrolytes (SPEs) have gained prominence for energy storage electrochemical devices due to their high flexibility and favorable electrode–electrolyte interactions. This study focuses on synthesizing nano cuprous oxide (CuO) semiconductors via the precipitation method. The prepared CuO nanofiller is homogeneously dispersed into a polymer electrolyte solution. Utilizing the solution cast method, free‐standing polymer electrolyte films are fabricated, exhibiting commendable mechanical stability. Polyvinyl alcohol (PVA) serves as the host material, with potassium iodide (KI) salt, forming the basis for the polymer electrolyte. The resultant electrolyte films underwent comprehensive characterization for their electrical and optical properties. The investigation aims to identify the optimal composition of the electrolyte film with superior conductivity. The selected composition will be employed in the fabrication of various electrochemical devices, demonstrating the potential for enhanced energy storage applications. This work not only contributes to the synthesis of advanced solid polymer electrolyte films but also paves the way for the development of efficient and sustainable energy storage solutions in the realm of renewable energy technologies.

Diethylenetriaminepentaacetic Acid-based Conducting Solid Polymer Electrolytes Impede Lithium Dendrites and Impart Antioxidant Capacity in Lithium-Ion Batteries.

In the development of lithium-ion batteries (LIBs), cheaper and safer solid polymer electrolytes are expected to replace combustible organic liquid electrolytes to meet the larger market demand. However, low ionic conductivity and inadequate cycling stability impede their commercial viability. Herein, a novel flexible conducting solid polymer electrolytes (CSPEs) based on polyvinyl alcohol (PVA) and ion-polarized diethylenetriaminepentaacetic acid (P-DETP) is developed for the first time and applied in LIBs. PVA and P-DETP form a compact polymer network through hydrogen bonding, enhancing the thermomechanical stability of CSPE while restricting the migration of larger anions. Furthermore, density functional theory calculations confirm that P-DETP can facilitate the dissociation of Li+-TFSI- via electrostatic attraction, resulting in increased mobility of lithium ions. Additionally, P-DETP contributes to the formation of a stable electrode-electrolyte interface layer, effectively suppressing the growth of lithium dendrites and improving antioxidant capacity. These synergistic effects enable CSPE to exhibit remarkable properties including high ionic conductivity (2.8 × 10-4 S cm-1), elevated electrochemical potential (5.1V), and excellent lithium transference number (0.869). Notably, the P-DETP/LiTFSI CSPE demonstrates stable performance not only in LiFePO4 batteries but also adapts to high-nickel ternary LiNi0.88Co0.06Mn0.06O2 cathode, highlighting its immense potential for application in high energy density LIBs.

Improving thermal stability and electrochemical performance of polymer solid electrolyte membranes with a novel TiO2@PA-APP composite additive

Polymer solid electrolytes (PSEs) are still under the safety risk because of flammability and low mechanical strength. Here a TiO2 coated piperazine-modified ammonium polyphosphate (TiO2@PA-APP) is synthesized and incorporated into poly (ethylene oxide) (PEO)-based PSE membranes to meet the above challenges. The thermal stability and ionic conductivity of PSE membrane incorporated with TiO2@PA-APP have been improved. Micro-scale combustion calorimetry experiments indicate a dramatic 70 % decrease in heat release rate, from 919 W g−1 to 267 W g−1. The lithium symmetric cell demonstrates remarkable durability, operating normally for 500 h with minimal polarization potential across various current densities at 60 °C. The all solid-state LiFePO4//Li battery using the cathode-supported TiO2@PA-APP/PEO-PSE membrane can reach a high discharge specific capacity of 153 mAh g−1 at 0.1 C and demonstrates good cycle performance, achieving a capacity retention rate of 88 % after 200 cycles at 0.2 C, along with an average coulombic efficiency of 99.24 %. These findings underscore the effectiveness of the TiO2@PA-APP flame retardant in fabricating solid-state lithium-ion batteries that provide enhanced safety and exceptional electrochemical performance.

Ion Conduction Mechanism in Polymer Blend Electrolyte Films

AbstractThis paper presents the development of the blend polymer solid electrolyte films (BPSE) for potential applications in electrochemical devices. Two host polymers, polyvinyl alcohol (PVA) and polymethyl methacrylate (PMMA), along with the salt KI, are employed to create the solid polymer electrolytes (SPEs). The synthesis involves varying the weight percentage of salt within the SPEs to investigate its impact on the material properties. Conductivity measurements are conducted using AC impedance spectroscopy, unveiling the conductivity behavior of the BPSEs. Additionally, surface morphology is characterized using polarized optical microscopy (POM) at 10 pixel resolution, offering a detailed examination of the film's microstructure. This comprehensive study not only contributes to the understanding of the fundamental properties of BPSEs but also opens avenues for their utilization in various electrochemical applications.

Preparation of polyelectrolyte based on bottle brush Polyethylene glycol‐Poly(N‐isopropylacrylamide) copolymers

AbstractThe increased demand for high energy‐density batteries led to using lithium metal (Li) anode. However, safety issues associated with Li anode encouraged the researchers to use less reactive and safer electrolytes with higher electrochemical stability. High ionic conductivity (σ), wider electrochemical stability window, and higher mechanical strength alongside the ability to self‐heal possible structural damages were at the center of focus for developing efficient solid electrolytes. In this regard, we developed a group of solid polymer electrolytes (SPEs) with high σ and electrochemical stability. In this regard, bottle brush polyethylene glycol (bbPEG) was synthesized using a chain transfer reaction. Polynipaam (PNIPAAM) blocks were also incorporated into the structure to prepare a block copolymer based on PNIPAM‐bbPEG‐PNIMAM represented by the ABA structure. The block copolymer was then blended with polyvinylidene fluoride (PVDF) with the block copolymer to PVDF weight ratio of 7:2% and 25% bis(trifluoromethane) sulfonamide (TFSI) salt was added and the final mixture was UV‐cured. The results indicated that the final SPE possessed high ionic conductivity with a relatively high lithium‐ion transference number () of 0.416 and the σ of 1.265 × 10−5 S/cm at 25°C.

Lithiophilic Protective Dual Layer Enabling Stable Electrodeposition of Lithium at High Current Density

Lithium (Li) is an ideal anode material for rechargeable batteries and thus manufacturing Li metal is crucial for the practical development of Li metal batteries. Electrodeposition is an efficient technique for producing ultrathin and scalable Li metal electrodes. However, the dendritic growth and the side reactions of Li with electrolyte during the electrodeposition are the main obstacles to overcome. In this study, we designed a pre-coated protective dual layer (PDL) composed of a poly(ethylene oxide)-based solid polymer electrolyte (SPE) and a polydopamine-coated cellulose membrane (PD-CM). The adhesive and ion-conductive SPE layer suppressed the growth of Li dendrites and side reactions with liquid electrolyte. The PD-CM layer with high porosity and lithiophilicity promoted a facile and uniform Li-ion flux. By applying the pre-coated PDL, Li was uniformly electrodeposited on the Ag-coated Cu at a high current density of 6 mA cm−2. The Li/LiFePO4 cell composed of an electrodeposited Li anode with PDL and a LiFePO4 cathode was assembled without an additional separator, and its cycling performance was evaluated. The cell initially delivered a high discharge capacity of 154.8 mAh g−1 at 45 °C and exhibited excellent cycling stability with a capacity retention of 97.0% after 200 cycles.

Preparation and Conductivity Analysis of LLTO Nanofiber‐Incorporated PEO‐PVDF‐HFP‐LiClO4 Solid Polymer Electrolytes for High‐Voltage Lithium Metal Batteries

ABSTRACTThis work focuses on the development of a composite polymer electrolyte (CPE) for all‐solid‐state lithium metal batteries (ASSLMBs), integrating LLTO nanofibers into a PEO (polyethylene oxide)‐PVDF‐HFP (poly(vinylidene fluoride‐cohexafluoropropylene)) matrix with LiClO4 as the lithium salt. The PEO has high ionic conductivity and flexibility, and the PVDF‐HFP has high mechanical strength and electrochemical stability. Therefore, the resulting composite has improved electrochemical performance and mechanical properties. Incorporating LLTO nanofibers enhances ionic conductivity due to the one‐dimensional ion transport pathways provided by the nanofibers while maintaining mechanical integrity and air stability, overcoming the challenges associated with conventional fillers. The prepared CPE demonstrates exceptional electrochemical stability up to 5.1 V versus Li/Li+, making it suitable for high‐voltage applications over traditional polymer electrolytes. The optimized CPE with 15 wt% LLTO provides the ionic conductivity of 1.1 × 10−5 S cm−1 at room temperature and reaches 1.46 × 10−4 S cm−1 at 80°C. The assembled LiNi1/3Mn1/3Co1/3PO4||PEO‐PVDF‐HFP‐LiClO₄‐LLTO||Li based 2032 coin cell worked in between 3 and 4.8 V versus Li/Li+ potential window without any electrolyte decomposition from 0.5 to 5 mV/s scan rates. Similarly, the fabricated LiFePO₄||PEO‐PVDF‐HFP (1:2)‐LiClO4‐LLTO (15 wt%)||Li cell provides an initial capacity of 149 mAh g−1 at 0.1 C and 85 mAh g−1 at 0.5 C, exploring its potential for lithium metal batteries. Overall, this work offers a promising pathway for developing advanced solid polymer electrolytes for next‐generation lithium metal batteries, which combine high ionic conductivity, excellent electrochemical performances, and robust mechanical properties.

Curved surface coupled structural battery composites manufactured by resin transfer molding process: Microstructure and multifunctional performance

To bridge industrial production and lab-scale research, this work demonstrates a technology to manufacture curved surface structural battery composites (CSBCs) that can simultaneously achieve electrochemical energy storage and load-bearing. The curved-surface carbon fiber structural anode and cathode are fabricated by coating the active materials on carbon fiber fabric with a vacuum-bag-assisted technique. The resin transfer molding (RTM) process is conducted to manufacture the coupled CSBCs by infusing bi-continuous phase epoxy resin electrolyte and curing at high temperatures. The microstructure of structural electrodes and CSBCs is characterized by scanning electron microscopy (SEM). Due to good interfacial compatibility between high mechanical strength carbon fiber structural electrode and high ionic conductivity solid polymer electrolyte bulk for load support, the fabricated CSBCs demonstrate a high density of 294 mWh kg−1 based on the whole mass of devices, a tensile strength of 257.4 MPa with Young's modulus of 12.9 GPa and a flexural strength of 194.1 MPa with flexural modulus of 11.1 GPa. In situ electrochemical-mechanical tests further confirm the durability of CSBCs under mechanical loads with a multifunctional efficiency of 1.07, suggesting the effectiveness of the introduced manufacturing techniques for coupled structural battery composites.

Sintesis dan Karakterisasi Solid Polymer Electrolyte (SPE) Berbasis Nanofiber Selulosa untuk Menunjang Baterai Litium Berdensitas Tinggi dan Ramah Lingkungan

Lithium battery as one of the energy storage has two important elements, namely electrodes and electrolyte. Electrolyte is a part of the battery element that has undergone many developments. In this study, the manufacture of electrolytes in the form of Solid Polymer Electrolyte (SPE) was carried out by utilizing the abundant availability of nata de coco. The nanofibrous cellulose structure in Bacterial Cellulose (BC) nata de coco has the advantages of good porosity, flexibility in surface functionality, compact porous structure that provides abundant ion pathways and hetero atoms (oxygen atoms) with free electron pairs that facilitate ionic conduction. The SPE synthesis process was carried out by varying the soaking time of nata de coco in ethanol, namely 1, 2 and 3 days to determine the structure with optimal results. FTIR characterization results show the synthesis of cellulose nanofiber has the same groups as commercial cellulose groups in the form of O-H, C-H, C=O and C-O. CV characterization results show the SPE electrolyte has good redox properties, especially in the 2-day variation with the highest specific capacitance. The EIS test showed the lowest resistance in the 1-day variation sample with a conductivity of 0.017 ohm-1.

Porous Lithium‐Doped ZnO Nanosheets with Abundant Oxygen Vacancies for Accelerating Li+ Transport in Solid‐State Composite Electrolyte

The flexible Li‐ion conducting solid polymer electrolyte (SPE) endows a stable long‐term cycling to Li‐metal anode to significantly improve the energy density of solid‐state lithium batteries; however, the practical application of the SPE is limited by its low ionic conductivity and small critical current density for dendrite nucleation. Herein, Li+‐doped porous ZnO (LZO) nanosheets are introduced into the poly(ethylene oxide) (PEO)‐based SPE, releasing more mobile Li ions for faster Li‐ion transport due to the enhanced interaction between abundant oxygen vacancies and anions of Li‐salt. As a result, the optimized LZO/PEO composite polymer electrolyte exhibits a high Li‐ion conductivity of 3.3 × 10−4 S cm−1 at 50 °C, 4 times higher than the pure PEO electrolyte. The solid‐state LiFePO4/Li cell shows extraordinarily long‐term stable cycling, up to 1500 cycles with a high average Coulombic efficiency of 99.8%. In addition, the cycling stability of the high‐voltage LiNi0.8Mn0.1Co0.1O2 (NMC811)/Li cell was also obviously improved compared to the nondoped pure PEO electrolyte, indicating the positive contribution of the LZO on interfacial stability.

The Self‐Expanding Frame of Graphydiyne Induces Rapid Transport of Lithium Ions in All‐Solid‐State Lithium Metal Batteries

AbstractLow ionic conductivity hinders the practical application of solid polymer electrolytes. Here, an interface‐oscillating polymer electrolyte (IOPE) based on graphdiyne (GDY) is designed and prepared to enable high‐performance all‐solid‐state lithium (Li) metal batteries (ASSLMBs). The affinity of GDY to Li ions induces the competitive adsorption of Li ions, weakens the coordination ability of Li ions with electron‐rich oxygen (on ethylene oxide), and accelerates the Li‐ion migration kinetics. The weak coordination between Li+‐acetylene greatly promotes the rapid reversible transition of GDY itself, resulting in strong self‐expanding/shrinking of the GDY skeleton and the GDY/polymer interface oscillation, and the reduction of the Li‐ion diffusion energy barrier at the interfaces. Consequently, the as‐prepared IOPE shows significantly improved Li‐ion conductivity (1.5 × 10−4 S cm−1 at 35 °C) and transference number, as well as excellent stability toward Li metal anodes. The ASSLMBs assembled with LiFePO4 cathodes and IOPE exhibit excellent rate and cycling performance, capable of stable operation for more than 250 cycles with a high‐capacity retention of 98% at 0.1C (1C = 170 mA g−1). The high‐performance all‐solid‐state Li metal pouch cells are also demonstrated to show great potential for the practical application of IOPE.

Synergism of lithium acetate salt toward surface chemistry and physical properties of carboxymethyl chitosan‐based solid polymer electrolyte

Synergism of lithium acetate salt toward surface chemistry and physical properties of carboxymethyl chitosan‐based solid polymer electrolyte

Sulfur/reduced graphite oxide and dual-anion solid polymer‒electrolyte integrated structure for high-loading practical all-solid-state lithium–sulfur batteries

The demand for high-capacity batteries with long cycle life and safety has been increasing owing to the expanding mid-to-large battery market. Li–S batteries are suitable energy-storage devices because of their reversibility, high theoretical capacity, and inexpensive construction materials. However, their performance is limited by various factors, including the shuttle effect and dendrite growth at the anode. Here, an integrated electrode for use in all-solid-state (ASS) Li–S batteries was formed via hot pressing. In detail, S particles dispersed in a functionalized reduced graphite oxide (rGO) cathode with a binder-less polymer electrolyte (PE) and a dual-anion ionic liquid-containing cross-linked poly(ethylene oxide)–Li bis(fluoromethanesulfonyl)imide–N-butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl) imide-based solid polymer electrolyte (SPE, PEO–LiFSI0.1(Pyr14TFSI)0.4) were hot-pressed into an integrated electrode, which serves as both the cathode and electrolyte. The resulting S/rGO-based solid-state Li–S batteries exhibited more stable performance than Li–S batteries using liquid electrolytes did, indicating that the dual-anion SPE layer effectively suppressed dendritic Li formation and the shuttle effect with high ionic conductivity. At 0.1 C, the battery discharge capacities were 957 and 576 mAh g−1 in the first cycle and after 100 cycles, respectively. At 1 C, the reversible capacity was 590 and 417 mAh g−1 in the first cycle and after 100 cycles, respectively (capacity retention = 71%). Therefore, the proposed S/rGO/PE//LiFSI0.1(Pyr14TFSI)0.4-integrated electrodes are beneficial for ASS Li–S batteries.

Solid polymer electrolytes with dual salts enhance lithium-metal interfacial stability for long cycle performance of lithium batteries

Solid-state lithium metal batteries (LMBs) are considered to be the ideal energy storage system for achieving higher energy density and high safety. However, poor physical contact at the interface between the solid-state electrolyte and lithium metal, as well as the growth of dendrites make the cycling stability of LMBs challenging. Therefore, we developed a multifunctional ionic liquid-based polymer electrolyte including montmorillonite (MMT) and double salts (NaFSI and LiTFSI). The self-concentration effect of MMT lithium ions, combined with the electrostatic shielding effect of the double salts, resulted in homogeneous ion deposition, reducing dendritic lithium generation and improving lithium battery performance, with lithium batteries achieving a stable cycling rate of 1000 cycles at 1 C. Moreover, Due to the integrated assembly of the battery assembly process using light curing, the physical interface between the positive electrode-electrolyte-negative electrode achieves good contact and wettability. NaFSI achieves the enhancement of solid electrolyte interface (SEI) by introducing NaF/LiF to SEI of lithium metal, and the optimization of ion deposition pattern at the interface can be achieved by electrostatic shielding effect. Ultimately, stable ion transport at the solid-solid interface for lithium metal solid-state batteries can be realized. Notably, the ionic liquid-based polymer electrolyte with high ionic conductivity (1.2 × 10−3 S cm−1) and high oxidative stability (5.2 V vs. Li/Li+) at room temperature. In addition, the good flame retardant properties of the electrolytes indicate that dual-salt polymer electrolytes are an effective strategy for achieving high safety and long cycle stability of LMBs.