Dendrite-Free Li5.5PS4.5Cl1.5-Based All-Solid-State Lithium Battery Enabled by Grain Boundary Electronic Insulation Strategy through In Situ Polymer Encapsulation.

Sulfide-based all-solid-state lithium batteries (ASSLBs) have attracted unprecedented attention in the past decade due to their excellent safety performance and high energy storage density. However, the sulfide solid-state electrolytes (SSEs) as the core component of ASSLBs have a certain stiffness, which inevitably leads to the formation of pores and cracks during the production process. In addition, although sulfide SSEs have high ionic conductivity, the electrolytes are unstable to lithium metal and have non-negligible electronic conductivity, which severely limits their practical applications. Herein, a grain boundary electronic insulation strategy through in situ polymer encapsulation is proposed for this purpose. A polymer layer with insulating properties is applied to the surface of the Li5.5PS4.5Cl1.5 (LPSC) electrolyte particles by simple ball milling. In this way, we can not only achieve a dense electrolyte pellet but also improve the stability of the Li metal anode and reduce the electronic conductivity of LPSC. This strategy of electronic isolation of the grain boundaries enables stable deposition/stripping of the modified electrolyte for more than 2000 h at a current density of 0.5 mA cm-1 in a symmetrical Li/Li cell. With this strategy, a full cell with Li(Ni0.8Co0.1Mn0.1)O2 (NCM811) as the cathode shows high performance including high specific capacity, improved high-rate capability, and long-term stability. Therefore, this study presents a new strategy to achieve high-performance sulfide SSEs.

Li5.5PS4.5Cl1.5-Based All-Solid-State Battery with a Silver Nanoparticle-Modified Graphite Anode for Improved Resistance to Overcharging and Increased Energy Density.

All-solid-state lithium batteries (ASSLBs) are attracting tremendous attention due to their improved safety and higher energy density. However, the use of a metallic lithium anode poses a major challenge due to its low stability and processability. Instead, the graphite anode exhibits high reversibility for the insertion/deinsertion of lithium ions, giving ASSLBs excellent cyclic stability but a lower energy density. To increase the energy density of ASSLBs with the graphite anode, it is necessary to lower the negative/positive (N/P) capacity ratio and to increase the charging voltage. These strategies bring new challenges to lithium metal plating and dendrite growth. Here, a nano-Ag-modified graphite composite electrode (Ag@Gr) is developed to overcome these shortcomings for Li5.5PS4.5Cl1.5-based ASSLBs. The Ag@Gr composite exhibits a strong ability to inhibit lithium metal plating and fast lithium-ion transport kinetics. Ag nanoparticles can accommodate excess Li, and the as-obtained Li-Ag alloy enhances the kinetics of the composite electrode. The ASSLB with the Li(Ni0.8Co0.1Mn0.1)O2 cathode and Ag@Gr anode achieves an energy density of 349 W h kg-1. The full cell using Ag@Gr with an N/P ratio of 0.6 also highlights the rate performance. This work provides a simple and effective method to regulate the charge transport kinetics of graphite anodes and improve the cyclic performance and energy density of ASSLBs.

A Stable Lithium Metal Anode Enabled by the Site-Directed Lithium Deposition of ZnO-Nanosheet-Modified Carbon Cloth.

Uneven lithium (Li) metal deposition typically results in uncontrollable dendrite growth, which renders an unsatisfactory cycling stability and coulombic efficiency (CE) of Li metal batteries (LMBs), preventing their practical application. Herein, a novel carbon cloth with the modification of ZnO nanosheets (ZnO@CC) is fabricated for LMBs. The as-prepared ZnO@CC with a cross-linked network significantly reduces the local current density, and the design of ZnO nanosheets can promote the uniform deposition of Li metal as lithiophilic sites. As a result, the Li metal anodes (LMAs) based on ZnO@CC (ZnO@CC@Li) enables a long cycle life over 640 hours with a low overpotential of 65 mV at a current density of 4 mA cm-2 with a capacity of 1 mAh cm-2 in the symmetric cell. Moreover, when coupling the ZnO@CC@Li with a LiFePO4 cathode, the assembled full cell exhibits excellent long cycle and rate performance, highlighting its promising practical application prospect.

In Situ Construction of LiF-Li3N-Rich Interface Contributed to Fast Ion Diffusion in All-Solid-State Lithium-Sulfur Batteries.

All-solid-state lithium-sulfur batteries (ASSLSBs) have attracted wide attention due to their ultrahigh theoretical energy density and the ability of completely avoiding the shuttle effect. However, the further development of ASSLSBs is limited by the poor kinetic properties of the solid electrode interface. It remains a great challenge to achieve good kinetic properties, by common strategies to substitute sulfur-transition metal and organosulfur composites for sulfur without reducing the specific capacity of ASSLSBs. In this study, a sulfur-(Ketjen Black)-(bistrifluoromethanesulfonimide lithium salt) (S-KB-LiTFSI) composite is constructed by introducing LiTFSI into the S-KB composite. The initial discharge capacity reaches up to 1483 mA h g-1, benefited from the improved ionic conductivity and diffusion kinetics of the S-KB-LiTFSI composite, where numerous LiF interphases with a Li3N component are in situ formed during cycling. Combined with DFT calculations, it is found that the migration barriers of LiF and Li3N are much smaller than that of the Li6PS5Cl solid electrolyte. The fast ionic conductors of LiF and Li3N not only enhance the Li+ transfer efficiency but also improve the interfacial stability. Therefore, the assembled ASSLSBs operate stably for 600 cycles at 200 mA g-1, and this study provides an effective strategy for the further development of ASSLSBs.

Scalable and Versatile Metal Ion Solidificated Alginate Hydrogel for Skin Wound Infection Therapy.

Bacterial infections in wounds continue to be a major challenge in clinical settings worldwide and represent a significant threat to human health. This work proposes novel expandable and versatile methods for solidifying sodium alginate (SA) with metal ions (such as Fe3+ , Co2+ , Ni2+ , Cu2+ , and Zn2+ ) to create Metal-Alginate (M-Alg) hydrogel with adjustable morphology, composition, and microstructure. It conforms to the wound site, protects against second infection, reduces inflammation, and promotes the healing of infected wounds. Among these hydrogels, Cu-Alginate (Cu-Alg) shows excellent sterilization effect and good efficacy against both gram-positive and gram-negative bacteria, including multidrug-resistant (MDR) strains such as Methicillin-resistant Staphylococcus aureus (MRSA) and Carbapenem-resistant Klebsiella pneumoniae (CRKP) due to its dual antibacterial mechanisms: contact-killing and reactive oxygen species (ROS) burst. Importantly, it exhibits low cytotoxicity and biodegradability. This simple and cost-effective gel-based system has the potential to introduce an innovative approach to the management of wound infection and offers promising new perspectives for the advancement of wound care practice.

Juice Vesicles Bioreactors Technology for Constructing Advanced Carbon-Based Energy Storage.

The construction of high-quality carbon-based energy materials through biotechnology has always been an eager goal of the scientific community. Herein, juice vesicles bioreactors (JVBs) bio-technology based on hesperidium (e.g., pomelo, waxberry, oranges) is first reported for preparation of carbon-based composites with controllable components, adjustable morphologies, and sizes. JVBs serve as miniature reaction vessels that enable sophisticated confined chemical reactions to take place, ultimately resulting in the formations of complex carbon composites. The newly developed approach is highly versatile and can be compatible with a wide range of materials including metals, alloys, and metal compounds. The growth and self-assembly mechanisms of carbon composites via JVBs are explained. For illustration, NiCo alloy nanoparticles are successfully in situ implanted into pomelo vesicles crosslinked carbon (PCC) by JVBs, and their applications as sulfur/carbon cathodes for lithium-sulfur batteries are explored. The well-designed PCC/NiCo-S electrode exhibits superior high-rate properties and enhanced long-term stability. Synergistic reinforcement mechanisms on transportation of ions/electrons of interface reactions and catalytic conversion of lithium polysulfides arising from metal alloy and carbon architecture are proposed with the aid of DFT calculations. The research provides a novel biosynthetic route to rational design and fabrication of carbon composites for advanced energy storage.

Plasma Technology for Advanced Electrochemical Energy Storage.

"Carbon Peak and Carbon Neutrality" is an important strategic goal for the sustainable development of human society. Typically, a key means to achieve these goals is through electrochemical energy storage technologies and materials. In this context, the rational synthesis and modification of battery materials through new technologies play critical roles. Plasma technology, based on the principles of free radical chemistry, is considered a promising alternative for the construction of advanced battery materials due to its inherent advantages such as superior versatility, high reactivity, excellent conformal properties, low consumption and environmental friendliness. In this perspective paper, we discuss the working principle of plasma and its applied research on battery materials based on plasma conversion, deposition, etching, doping, etc. Furthermore, the new application directions of multiphase plasma associated with solid, liquid and gas sources are proposed and their application examples for batteries (e. g. lithium-ion batteries, lithium-sulfur batteries, zinc-air batteries) are given. Finally, the current challenges and future development trends of plasma technology are briefly summarized to provide guidance for the next generation of energy technologies.

Hyphae Carbon Coupled with Gel Composite Assembly for Construction of Advanced Carbon/Sulfur Cathodes for Lithium-Sulfur Batteries.

The design and fabrication of novel carbon hosts with high conductivity, accelerated electrochemical catalytic activities, and superior physical/chemical confinement on sulfur and its reaction intermediates polysulfides are essential for the construction of high-performance C/S cathodes for lithium-sulfur batteries (LSBs). In this work, a novel biofermentation coupled gel composite assembly technology is developed to prepare cross-linked carbon composite hosts consisting of conductive Rhizopus hyphae carbon fiber (RHCF) skeleton and lamellar sodium alginate carbon (SAC) uniformly implanted with polarized nanoparticles (V2O3, Ag, Co, etc.) with diameters of several nanometers. Impressively, the RHCF/SAC/V2O3 composites exhibit enhanced physical/chemical adsorption of polysulfides due to the synergistic effect between hierarchical pore structures, heteroatoms (N, P) doping, and polar V2O3 generation. Additionally, the catalytic conversion kinetics of cathodes are effectively improved by regulating the 3D carbon structure and optimizing the V2O3 catalyst. Consequently, the LSBs assembled with RHCF/SAC/V2O3-S cathode show exceptional cycle stability (capacity retention rate of 94.0% after 200 cycles at 0.1 C) and excellent rate performance (specific capacity of 578 mA h g-1 at 5 C). This work opens a new door for the fabrication of hyphae carbon composites via fermentation for electrochemical energy storage.

An Advanced Gel Polymer Electrolyte for Solid-State Lithium Metal Batteries.

All-solid-state lithium metal batteries (LMBs) are regarded as one of the most viable energy storage devices and their comprehensive properties are mainly controlled by solid electrolytes and interface compatibility. This work proposes an advanced poly(vinylidene fluoride-hexafluoropropylene) based gel polymer electrolyte (AP-GPEs) via functional superposition strategy, which involves incorporating butyl acrylate and polyethylene glycol diacrylate as elastic optimization framework, triethyl phosphate and fluoroethylene carbonate as flameproof liquid plasticizers, and Li7La3Zr2O12 nanowires (LLZO-w) as ion-conductive fillers, endowing the designed AP-GPEs/LLZO-w membrane with high mechanical strength, excellent flexibility, low flammability, low activation energy (0.137 eV), and improved ionic conductivity (0.42 × 10-3 S cm-1 at 20 °C) due to continuous ionic transport pathways. Additionally, the AP-GPEs/LLZO-w membrane shows good safety and chemical/electrochemical compatibility with the lithium anode, owing to the synergistic effect of LLZO-w filler, flexible frameworks, and flame retardants. Consequently, the LiFePO4/Li batteries assembled with AP-GPEs/LLZO-w electrolyte exhibit enhanced cycling performance (87.3% capacity retention after 600 cycles at 1 C) and notable high-rate capacity (93.3 mAh g-1 at 5 C). This work proposes a novel functional superposition strategy for the synthesis of high-performance comprehensive GPEs for LMBs.

Facile Synthesis of Pre-Lithiated LiTiO2 Nanoparticles for Quick Charge and Long Lifespan Anode in Lithium-Ion Batteries.

Titanium dioxide (TiO2) has been widely used as an alternative anodic material for lithium-ion batteries (LIBs) due to its ultrahigh capacity retention and long cycle lifespan. However, the restriction of lithium insertion, intrinsically poor electronic conductivity, and sluggish lithium ionic kinetics of bulk TiO2 hinder their specific capacity and rate performance. Herein, LiTiO2 nanoparticles (NPs) are synthesized via a facile ball milling method by the reaction of anatase TiO2 with LiH. The as-prepared LiTiO2 NPs have strong structural stability and a "zero strain" effect during the repeated intercalation/deintercalation, even at low potential. As anodic materials for LIBs, LiTiO2 NPs exhibit a superior rate performance of ∼100 mA h g-1 at 10C (3350 mA g-1) with a capacity retention of 100% after 1000 cycles, which is 5 times higher than that of the original commercial anatase TiO2 powder. The higher specific capacity of LiTiO2 NPs is attributed to the increased conversion of Ti3+ to Ti2+ on the porous surface of LiTiO2 NPs, which provides a more capacitive contribution. This study not only provides a new fabrication approach toward Ti-based anodes for ultrafast LIBs but also underscores the potential importance of embedding lithium into transition metal oxides as a strategy for boosting their electrochemical performance.

An approach to enhance carbon/polymer interface compatibility for lithium-ion supercapacitors.

Developing high-efficiency and easy machining components, as well as high-performance energy storage components, is a pressing issue on the road to economic and social progress. Optimizing the interface compatibility between composites and promoting the efficient utilization of the electrochemical active sites are crucial factors in improving the electrochemical performance of composite electrode materials. To address this challenge, a carbon-based flexible lithium-ion supercapacitor positive material (Polyaniline @ Carbon Foam-Supercritical carbon dioxide (P@C-SC)) is synthesized using commercial melamine foam and aniline monomer. The synthesis process utilizes supercritical fluid technology, effectively solving the interface compatibility problem between the composite materials. Consequently, the electrochemical performance of the composite electrode materials is significantly improved. The supercapacitive properties of this material are investigated in 1 mol/L sulfuric acid (H2SO4) and lithium sulfate (Li2SO4) electrolytes using a three-electrode system. In H2SO4 electrolyte, the material exhibits a working voltage of up to 2.2 V and a specific capacitance of 898F/g (at 1 A/g), resulting in a maximum energy density of 50.8 Wh kg-1. Furthermore, this electrode demonstrates superior lithium storage performance, with a specific capacity of approximately 900 mAh/g (at 1 A/g) and a retention of about 400 mAh/g after 200 cycles, along with a coulomb efficiency of 100%. This work offers insights into the integrated design of composite materials with improved electrochemical properties and interface compatibility, thus providing potential applicability of supercritical fluids in the field of lithium-ion supercapacitors.

High-Performance Solid Lithium Metal Batteries Enabled by LiF/LiCl/LiIn Hybrid SEI via InCl3 -Driven In Situ Polymerization of 1,3-Dioxolane.

The use of poly(1,3-dioxolane) (PDOL) electrolyte for lithium batteries has gained attention due to its high ionic conductivity, low cost, and potential for large-scale applications. However, its compatibility with Li metal needs improvement to build a stable solid electrolyte interface (SEI) toward metallic Li anode for practical lithium batteries. To address this concern, this study utilized a simple InCl3 -driven strategy for polymerizing DOL and building a stable LiF/LiCl/LiIn hybrid SEI, confirmed through X-ray photoelectron spectroscopy (XPS) and cryogenic-transmission electron microscopy (Cryo-TEM). Furthermore, density functional theory (DFT) calculations and finite element simulation (FES) verify that the hybrid SEI exhibits not only excellent electron insulating properties but also fast transport properties of Li+ . Moreover, the interfacial electric field shows an even potential distribution and larger Li+ flux, resulting in uniform dendrite-free Li deposition. The use of the LiF/LiCl/LiIn hybrid SEI in Li/Li symmetric batteries shows steady cycling for 2000 h, without experiencing a short circuit. The hybrid SEI also provided excellent rate performance and outstanding cycling stability in LiFePO4 /Li batteries, with a high specific capacity of 123.5 mAh g-1 at 10 C rate. This study contributes to the design of high-performance solid lithium metal batteries utilizing PDOL electrolytes.

LiF-Rich Interfacial Protective Layer Enables Air-Stable Lithium Metal Anodes for Dendrite-Free Lithium Metal Batteries.

Lithium (Li) metal is considered as a promising anode candidate for high-energy-density batteries. However, the high reactivity of Li metal leads to poor air stability, limiting its practical application. Additionally, the interfacial instability, such as dendrite growth and an unstable solid electrolyte interphase layer, further complicates its utilization. Herein, a dense lithium fluoride (LiF)-rich interfacial protective layer is constructed on the Li surface through a simple reaction between Li and fluoroethylene carbonate (denoted as LiF@Li). The LiF-rich interfacial protective layer consists of both organic (ROCO2Li and C-F-containing species, which only exist on the outer layer) and inorganic (LiF and Li2CO3, distribute throughout the layer) components with a thickness of ∼120 nm. Specifically, chemically stable LiF and Li2CO3 play an important role in blocking air and hence improve the air durability of LiF@Li anodes. Notably, LiF with high Li+ diffusivity facilitates uniform Li+ deposition, while organic components with high flexibility relieve volume change upon cycling, thereby enhancing the dendrite inhibition capacity of LiF@Li. Consequently, LiF@Li exhibits remarkable stability and excellent electrochemical performance in both symmetric cells and LiFePO4 full cells. Moreover, LiF@Li maintains its initial color and morphology even after air exposure for 30 min, and the air-exposed LiF@Li anode still retains its superior electrochemical performance, further establishing its outstanding air-defendable capability. This work proposes a facile approach in constructing air-stable and dendrite-free Li metal anodes toward reliable Li metal batteries.

Slurry-Coated LiNi0.8Co0.1Mn0.1O2-Li3InCl6 Composite Cathode with Enhanced Interfacial Stability for Sulfide-Based All-Solid-State Batteries.

The implementation of all-solid-state lithium batteries (ASSLBs) is regarded as an important step toward the next-generation energy storage systems. The sulfide solid-state electrolyte (SSE) is a promising candidate for ASSLBs due to its high ionic conductivity and easy processability. However, the interface stability of sulfide SSEs toward high-capacity cathodes like nickel-rich layered cathodes is limited by the interfacial side reaction and narrow electrochemical window of the electrolyte. Herein, we propose introducing the halide SSE Li3InCl6 (LIC) with high (electro)chemical stability and superior Li+ conductivity to act as an ionic conductive additive in the Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM) cathode mixture through a slurry coating, aiming to build a stable cathode-electrolyte interface. This work demonstrates that the sulfide SSE Li5.5PS4.5Cl1.5 (LPSCl) is chemically incompatible with the NCM cathode, and the indispensable role of the substitution of LPSCl with LIC in enhancing the interfacial compatibility and oxidation stability of the electrolyte is highlighted. Accordingly, this new configuration shows superior electrochemical performance at room temperature. It shows a high initial discharge capacity (136.3 mA h g-1 at 0.1C), cycling performance (77.4% capacity retention at the 100th cycle), and rate capability (79.3 mA h g-1 at 0.5C). This work paves the way for investigating interfacial challenges regarding high-voltage cathodes and provides new insights into possible interface engineering strategies.

Fabrication and Characterization of Carbon Nanotube Filled PDMS Hybrid Membranes for Enhanced Ethanol Recovery.

Ethanol separation via the pervaporation process has shown growing application potential in solvent recovery and the bioethanol industry. In the continuous pervaporation process, polymeric membranes such as hydrophobic polydimethylsiloxane (PDMS) have been developed to enrich/separate ethanol from dilute aqueous solutions. However, its practical application remains largely limited due to the relatively low separation efficiency, especially in selectivity. In view of this, hydrophobic carbon nanotube (CNT) filled PDMS mixed matrix membranes (MMMs) aimed at high-efficiency ethanol recovery were fabricated in this work. The filler K-MWCNTs was prepared by functionalizing MWCNT-NH2 with epoxy-containing silane coupling agent (KH560) to improve the affinity between fillers and PDMS matrix. With K-MWCNT loading increased from 1 wt % to 10 wt %, membranes showed higher surface roughness and water contact angle was improved from 115° to 130°. The swelling degree of K-MWCNT/PDMS MMMs (2 wt %) in water were also reduced from 10 wt % to 2.5 wt %. Pervaporation performance for K-MWCNT/PDMS MMMs under varied feed concentrations and temperatures were evaluated. The results supported that the K-MWCNT/PDMS MMMs at 2 wt % K-MWCNT loading showed the optimum separation performance (compared with pure PDMS membranes), with the separation factor improved from 9.1 to 10.4, and the permeate flux increased by 50% (40-60 °C, at 6 wt % feed ethanol concentration). This work provides a promising method for preparing a PDMS composite with both high permeate flux and selectivity, which showed great potential for bioethanol production and alcohol separation in industry.

New Chemical Synthesis Strategy To Construct a Silicon/Carbon Nanotubes/Carbon-Integrated Composite with Outstanding Lithium Storage Capability.

The Si/C anode is one of the most promising candidate materials for the next-generation lithium-ion batteries (LIBs). Herein, a silicon/carbon nanotubes/carbon (Si/CNTs/C) composite is in situ synthesized by a one-step reaction of magnesium silicide, calcium carbonate, and ferrocene. Transmission electron microscopy reveals that the growth of CNTs is attributed to the catalysis of iron atoms derived from the decomposition of ferrocene. In comparison to a Si/C composite, the cycle stability of the Si/CNTs/C composite can obviously be improved as an anode for LIBs. The enhanced performance is mainly attributed to the following factors: (i) the perfect combination of Si nanoparticles and in situ grown CNTs achieves high mechanical integrity and good electrical contact; (ii) Si nanoparticles are entangled in the CNT cage, effectively reducing the volume expansion upon cycling; and (iii) in situ grown CNTs can improve the conductivity of composites and provide lithium ion transport channels. Moreover, the full cell constructed by a LiFePO4 cathode and Si/CNTs/C anode exhibits excellent cycling stability (137 mAh g-1 after 300 cycles at 0.5 C with a capacity retention rate of 91.2%). This work provides a new way for the synthesis of a Si/C anode for high-performance LIBs.

Solid-State Electrolytes in Lithium-Sulfur Batteries: Latest Progresses and Prospects.

Solid-state lithium-sulfur batteries (SSLSBs) have attracted tremendous research interest due to their large theoretical energy density and high safety, which are highly important indicators for the development of next-generation energy storage devices. Particularly, safety and "shuttle effect" issues originating from volatile and flammable liquid organic electrolytes can be fully mitigated by switching to a solid-state configuration. However, their road to thecommercial application is still plagued with numerous challenges, most notably the intrinsic electrochemical instability of solid-state electrolytes (SSEs) materials and their interfacial compatibility with electrodes and electrolytes. In this review, a critical discussion on the key issues and problems of different types of SSEs as well as the corresponding optimization strategies are first highlighted. Then, the state-of-the-art preparation methods and properties of different kinds of SSE materials, and their manufacture, characterization and performance in SSLSBs are summarized in detail. Finally, a scientific outlook for the future development of SSEs and the avenue to commercial application of SSLSBs is also proposed.

Stable LiF-Rich Electrode-Electrolyte Interface toward High-Voltage and High-Energy-Density Lithium Metal Solid Batteries.

Lithium-rich layered oxide (LRLO) materials have attracted significant attention due to their high specific capacity, low cost, and environmental friendliness. However, owing to its unique capacity activation mechanism, the release of lattice oxygen during the first charge process leads to a series of problems, such as severe voltage decay, poor cycle stability, and poor rate performance. Herein, a fluorinated quasi-solid-state electrolyte (QSSE) via a simple thermal polymerization method toward lithium metal batteries with LRLO materials is reported. The well-designed QSSE exhibits an ionic conductivity of 6.4 × 10-4 S cm-1 at 30 °C and a wide electrochemical stable window up to 5.6 V. Most importantly, XPS spectra demonstrate the generation of a LiF-rich electrode-electrolyte interface (EEI), where the in situ generated LiF provides strong protection against the structural degradation of LRLO materials and directs the uniform plating/stripping behaviors of lithium-ions to inhibit the formation of lithium dendrites. As a result, LRLO/QSSE/Li batteries exhibit excellent rate performance and demonstrate a large initial capacity for 209.7 mA h g-1 with a capacity retention of 80.8% after 200 cycles at 0.5C. This work provides a new insight for the LiF-rich EEI design of safe, high-performance quasi-solid-state lithium metal batteries.

Three-dimensional polyimide nanofiber framework reinforced polymer electrolyte for all-solid-state lithium metal battery.

The replacement of traditional liquid electrolytes with polyethylene oxide (PEO) based composite polymer electrolytes (CPEs) is an important strategy to address the current flammability and explosiveness of lithium batteries since PEO CPEs have high flexibility, excellent processability and moderate cost. However, the insufficient ionic conductivity and inferior mechanical strength of PEO CPEs do not suit the operating requirements of all-solid-state lithium metal batteries at room temperature. Herein, three-dimensional (3D) framework composed of interweaved high-modulus polyimide (PI) nanofibers along with functional succinonitrile (SN) plasticizers are employed to synergistically reinforce the ionic conductivity and mechanical strength of PEO CPEs. Impressively, benefitting from the synergistic effects of 3D PI framework and SN plasticizer, PI-PEO-SN CPEs exhibits high ionic conductivity of 1.03 × 10-4 S cm-1 at 30 °C, remarkable tensile strength of 4.52 MPa, and superior Li dendrites blocking ability (>400 h at 0.1 mA cm-2). Such favorable features of PI-PEO-SN CPEs endow LiFePO4/PI-PEO-SN/Li solid-state prototype cells with high specific capacity (151.2 mA h g-1 at 0.2 C), long cycling lifespan (>150 cycles with 91.7 % capacity retention), and superior operating safety even under bending, folding and cutting harsh conditions. This work will pave the avenues to design and fabricate new high-performance PEO CPEs for the high energy density and safety all-solid-state batteries.