Slurry Casted Ultrathin Li3Zr2Si2PO12 Electrolyte Film for Solid-State Lithium Metal Batteries.

Thin and flexible solid-state electrolyte (SSE) films with high ionic conductivity and low interfacial resistance are urgently required for lithium metal batteries (LMBs). However, it's still challenging to reduce the film thickness to <20 µm, especially for those with high ceramic contents. Herein, a facile slurry casting method is developed to prepare the ultra-thin (14 µm) Li3Zr2Si2PO12 (LZSP) films with ceramic content up to 91% using a composite polymer binder, polyvinylidene fluoride (PVDF), and polyethylene oxide (PEO). It shows that PEO not only enhanced the film flexibility but also makes it be easily peeled off to form a freestanding membrane, PLN. To promote the interfacial ion transport, PEO/lithium bis(trifluoromethylsulfonyl)imide (LiTFSI) is introduced to the film surface, and the resultant tri-layer film, PPLN, shows a satisfying room temperature ionic conductivity of 0.116 mS cm-1, high Li+ transference number of 0.79, and good compatibility with metal lithium. As a result, LMBs using LiFePO4 cathode and PPLN electrolyte exhibit excellent safety as well as electrochemical performances in the wide temperature range between room temperature (RT) and 100 °C.

Surface Coordination of Garnet Fillers Improves the Organic-Inorganic Interfacial Compatibility of Composite Solid Electrolyte.

Composite solid electrolytes (CSEs) have become one of the most promising solid-state electrolytes due to their favorable safety and flexibility. However, the weak interaction between inorganic fillers and polymer matrix leads to poor organic-inorganic interfacial compatibility, which degrades the electrochemical performance of CSEs. Herein, it is demonstrated that Li6.4La3Zr1.4Ta0.6O12 (LLZTO) can be chemically bonded to the polymer matrix by surface coordination of the 1,2-dithiolane group of lipoic acid (LA) with metal atoms on the surface of LLZTO through a combination of experimental investigations and theoretical calculations. The surface coordination not only enhances the interfacial compatibility between LLZTO and the polymer matrix, but also facilitates rapid Li+ transport, which leads to the ionic conductivity of the prepared CSE (P-V-M@LLZTO) as high as 6.1 × 10-4 S cm-1 at 30 °C. The excellent interface compatibility ensures a stable cycle of Li/P-V-M@LLZTO/Li symmetrical cell for more than 3500 h. As a result, LiFePO4/P-V-M@LLZTO/Li cell delivers the discharge capacity of 161 mAh g-1 after 5 cycles with a capacity retention of 81% after 500 cycles at 0.5C under 30 °C. This work demonstrates that surface coordination is an effective strategy to solve the inherent interfacial incompatibility problem in CSEs.

Toward Ultrastable Metal Anode/Li6PS5Cl Interface via an Interlayer as Li Reservoir.

All-solid-state sulfide-based Li metal batteries are promising candidates for energy storage systems. However, thorny issues associated with undesired reactions and contact failure at the anode interface hinder their commercialization. Herein, an indium foil was endowed with a formed interlayer whose surface film is enriched with LiF and LiIn phases via a feasible prelithiation route. The lithiated alloy of the interlayer can regulate Li+ flux and charge distribution as a Li reservoir, benefiting uniform Li deposition. Meanwhile, it can suppress the reductive decomposition of the Li6PS5Cl electrolyte and maintain sufficient solid-solid contact. In situ impedance spectra reveal that constant interface impedance and fast charge transfer are realized by the interlayer. Further, long-term Li stripping/plating over 2000 h at 2.55 mA cm-2 is demonstrated by this anode. All-solid-state cells employing a LiCoO2 cathode and the Pre In anode can work for over 700 cycles with a capacity retention of 96.15% at 0.5 C.

Uniformly Distributed Mixed Matrix Membranes via a Solution Processable Strategy for Propylene/Propane Separation.

Aggregation of filler particles during the formation of mixed matrix membranes is difficult to avoid when filler loadings exceed a 10-15 wt %. Such agglomeration usually leads to poor membrane performance. In this work, using a ZIF-67 metal-organic framework (MOF) as filler along with surface modification of Ag4 tz4 to improve processability and selective olefin adsorption, we demonstrate that highly loaded with a very low agglomeration degree membranes can be synthesized displaying unmatched separation selectivity (39) for C3 H6 /C3 H8 mixtures and high permeability rates (99 Barrer), far surpassing previous reports in the literature. Through molecular dynamics simulation, the enhanced compatibility between ZIF-67 and polymer matrix with adding Ag4 tz4 was proven and the tendency in gas permeability and C3 H6 selectivity in the mixed matrix membranes (MMMs) were well explained. More importantly, the membrane showed a wide range of pressure and temperature resistance, together with remarkable long-term stability (>900 h). The modification method might help solve interface issues in MMMs and can be extended to the fabrication of other fillers to achieve high performance MMMs for gas separation.

A Highly Stable and Non-Flammable Deep Eutectic Electrolyte for High-Performance Lithium Metal Batteries.

Deep eutectic electrolytes (DEEs) are regarded as one of the next-generation electrolytes to promote the development of lithium metal batteries (LMBs) due to their unparalleled advantages compared to both liquid electrolytes and solid electrolytes. However, its application in LMBs is limited by electrode interface compatibility. Here, we introduce a novel solid dimethylmalononitrile (DMMN)-based DEE induced by N coordination to dissociate LiTFSI. We confirmed that the DMMN molecule can promote the dissociation of LiTFSI by the interaction between the N atom and Li+, and form the hydrogen bond with TFSI- anion, which can promote the dissociation of LiTFSI to form DEE. More importantly, due to the absence of active α-hydrogen, DMMN exhibits greatly enhanced reduction stability with Li metal, resulting in favorable electrode/electrolyte interface compatibility. Polymer electrolytes based on this DEE exhibit high ionic conductivity (0.67 mS cm-1 at 25 °C), high oxidation voltage (5.0 V vs. Li+/Li), favorable interfacial stability, and nonflammability. Li‖LFP and Li‖NCM811 full batteries utilizing this DEE polymer electrolyte exhibit excellent long-term cycling stability and excellent rate performance at high rates. Therefore, the new DMMN-based DEE overcomes the limitations of traditional electrolytes in electrode interface compatibility and opens new possibilities for improving the performance of LMBs.

Self-Sorting of Interfacial Compatibility in MOF-Based Mixed Matrix Membranes.

Metal-organic framework (MOF)-based mixed matrix membranes (MMMs) have shown great promises to overcome the performance upper limit of polymeric membranes for various gas separation processes. However, the gas separation properties of the MMMs largely depend on the MOF-polymer interfacial compatibility which is a metric difficult to quantify. In most cases, whether a MOF filler and a polymer matrix make a good pair is not revealed until the gas transport experiments are performed. This is because there is a lack of characterization techniques to directly probe the MOF-polymer interfacial compatibility. In this work, we demonstrate a self-sorting method to rank the interface compatibility among several MOF-polymer pairs. By mixing one MOF with two polymers in an MMM, the demixing of two polymers will form two polymer domains. The MOF particles will preferably partition into the "preferred" polymer domain due to their higher interfacial affinity. By scanning different polymer pairs, a rank of MOF-polymer interfacial compatibility from high to low can be obtained. Moreover, based on this ranking, it was also found that a highly compatible MOF-polymer pair suggested by this method also corresponds to a more predictable MMM gas separation performance.

Design of Solid Polycationic Electrolyte to Enable Durable Chloride-Ion Batteries.

The high energy density and cost-effectiveness of chloride-ion batteries (CIBs) make them promising alternatives to lithium-ion batteries. However, the development of CIBs is greatly restricted by the lack of compatible electrolytes to support cost-effective anodes. Herein, we present a rationally designed solid polycationic electrolyte (SPE) to enable room-temperature chloride-ion batteries utilizing aluminum (Al) metal as an anode. This SPE endows the CIB configuration with improved air stability and safety (i.e. free of flammability and liquid leakage). A high ionic conductivity (1.3×10-2 S cm-1 at 25 °C) has been achieved by the well-tailored coordination structure of the SPE. Meanwhile, the solid polycationic electrolyte ensures stable electrodes|electrolyte interfaces, which effectively inhibit the growth of dendrites on the Al anodes and degradation of the FeOCl cathodes. The Al|SPE|FeOCl chloride-ion batteries showcased a high discharge capacity around 250 mAh g-1 (based on the cathodes) and extended lifespan. Our electrolyte design opens a new avenue for developing low-cost chloride-ion batteries.

Electrospun Sandwich-like Structure of PVDF-HFP/Cellulose/PVDF-HFP Membrane for Lithium-Ion Batteries.

Cellulose membranes have eco-friendly, renewable, and cost-effective features, but they lack satisfactory cycle stability as a sustainable separator for batteries. In this study, a two-step method was employed to prepare a sandwich-like composite membrane of poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)/cellulose/ PVDF-HFP (PCP). The method involved first dissolving and regenerating a cellulose membrane and then electrospinning PVDF-HFP on its surface. The resulting PCP composite membrane exhibits excellent properties such as high porosity (60.71%), good tensile strength (4.8 MPa), and thermal stability up to 160 °C. It also has exceptional electrolyte uptake properties (710.81 wt.%), low interfacial resistance (241.39 Ω), and high ionic conductivity (0.73 mS/cm) compared to commercial polypropylene (PP) separators (1121.4 Ω and 0.26 mS/cm). Additionally, the rate capability (163.2 mAh/g) and cycling performance (98.11% after 100 cycles at 0.5 C) of the PCP composite membrane are superior to those of PP separators. These results demonstrate that the PCP composite membrane has potential as a promising separator for high-powered, secure lithium-ion batteries.

Polyvinyl alcohol and aminated cellulose nanocrystal membranes with improved interfacial compatibility for environmental applications.

Biogas up-gradation is a useful method to control CO2 emission and enhance the green process. The demand for renewable sources is increasing due to the depletion of fossil fuels. Thin-film nanocomposites functionalized with tunable molecular-sieving nanomaterials have been employed to tailor membranes with enhanced permeability and selectivity. In this work, the cellulose nanocrystals as a filler in the polyvinyl alcohol matrix are prepared to achieve high-performance facilitated transport membranes for CO2 capture. Considering the mechanical stability, interfacial compatibility and high moisture uptake of the filler, the main objective of this work was to develop a novel aminated CNC (Am-CNC)/polyvinyl alcohol nanocomposite membrane for biogas upgrading. The hydroxyl groups (O-H) on the reducing end of the cellulose nanocrystals were replaced by amino groups (N-H2). It was discovered through Scanning electron microscopy (SEM), X-ray diffraction (XRD) and Fourier Transform Infrared Spectroscopy (FTIR) that adding Am-CNCs in PVA membranes shows an increment in the CO2 removal and effectively upgrades the biogas. The effect of change in concentration of Am-CNC and feed pressure was investigated. The results showed that with increasing Am-CNC concentration up to 1.5 wt%, the thickness of the selective membrane layer increased from 0.95 to 1.9 µm with a decrease in the moisture uptake from 85.04 to 58.84%. However, the best CO2 permeance and selectivity were achieved at 0.306 m3/m2.bar.h (STP) and 33.55, respectively. Furthermore, there was a more than two-fold decrease in CO2 permeance and a 27% decrease in the CO2/CH4 selectivity when the feed pressure increased from 5 to 15 bar. It was revealed that PVA/Am-CNC membrane is high performing for the biogas upgradation.

Graphitic Carbon Nitride (g-C3 N4 ): An Interface Enabler for Solid-State Lithium Metal Batteries.

Solid-state Li metal batteries (SSLMBs) have attracted considerable interests due to their promising energy density as well as high safety. However, the realization of a well-matched Li metal/solid-state electrolyte (SSE) interface remains challenging. Herein, we report g-C3 N4 as a new interface enabler. We discover that introducing g-C3 N4 into Li metal can not only convert the Li metal/garnet-type SSE interface from point contact to intimate contact but also greatly enhance the capability to suppress the dendritic Li formation because of the greatly enhanced viscosity, decreased surface tension of molten Li, and the in situ formation of Li3 N at the interface. Thus, the resulting Li-C3 N4 |SSE|Li-C3 N4 symmetric cell gives a significantly low interfacial resistance of 11â€…Ω cm2 and a high critical current density (CCD) of 1500 µA cm-2 . In contrast, the same symmetric cell configuration with pristine Li metal electrodes has a much larger interfacial resistance (428â€…Ω cm2 ) and a much lower CCD (50 µA cm-2 ).

Crustacean-inspired chitin-based flexible buffer layer with a helical cross-linked network for bamboo fiber/poly(3-hydroxybutyrate) biocomposites.

Marine biological resources, serving as a renewable and sustainable reservoir, holds significant import for the utilization of composite material. Hence, we produced bamboo fiber/poly(3-hydroxybutyrate) (BF/PHB) biocomposites with exceptional performance and economic viability, drawing inspiration from the resilience of crustacean shells. Polyaminoethyl modified chitin (PAECT) was synthesized using the alkali freeze-thaw method and introduced into the interface between BF and PHB to improve interfacial adhesion. The resulting chitin fibers, characterized by their intertwined helical chains, constructed a flexible mesh structure on the BF surface through an electrostatic self-assembly approach. The interwoven PAECT filaments infiltrated the dual-phase structure, acting as a promoter of interfacial compatibility, while the flexible chitin network provided a greater capacity for deformation accommodation. Consequently, both impact and tensile strength of the BF/PHB composites were notably enhanced. Additionally, this flexible layer ameliorated the thermal stability and crystalline properties of the composites. This investigation aimed to leverage the distinctive helical configuration of chitin to facilitate the advancement of bio-reinforced composites.

Facet Engineering Boosts Interfacial Compatibility of Inorganic-Polymer Composites.

The interfacial compatibility between inorganic particles and polymer is crucial for ensuring high performance of composites. Current efforts to improve interfacial compatibility preferentially rely on organic modification of inorganic particles, leading to their complex process, high costs, and short lifespans due to aging and decomposition of organic modifiers. However, the fabrication of inorganic particles free from organic modification that is highly compatible in polymer still remains a great challenge. Herein, a novel facet-engineered inorganic particle that exhibit high compatibility with widely used polymer interface without organic modification is reported. Theoretical calculations and experimental results show that (020) and (102) facets of inorganic particles modulate local coordination environment of Ca atoms, which in turn regulate d-orbital electron density of Ca atoms and electron transfer paths at interfaces between polymer and inorganic particles. This difference alters the molecular diffusion, orientation of molecular chains on surface of inorganic particles, further modulating interfacial compatibility of composites. Surprisingly, the facet-engineered inorganic particles show exceptional mechanical properties, especially for tensile strain at break, which increases by 395%, far superior to state-of-the-art composites counterparts. Thus, the method can offer a more benign approach to the general production of high-performance and low-cost polymer-inorganic composites for diverse potential applications.

Dual cross-linked network of the active starch film by incorporating palmitic acid and geraniol: A comprehensive evaluation of the hydrophobic mechanism and antimicrobial activity.

In this study, (3-Aminopropyl) triethoxysilane (APTES) was employed as a bridging agent to enhance the compatibility between the hydrophilic starch/pectin film and the hydrophobic palmitic acid (PA) coating through hydrogen bonding and chemical reactions. To address the insufficient antibacterial activity of starch films, geraniol was also incorporated. The intermolecular interactions among APTES, PA, and starch were confirmed using x-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), and hydrogen nuclear magnetic resonance spectroscopy (1H NMR). Notably, the inclusion of APTES and PA significantly increased the film's hydrophobicity, resulting in a water contact angle (WCA) of 95.12°, a water vapor permeability (WVP) of 2.08 × 10-10 g/(mm·s·Pa), and an oxygen permeability (OP) of 2.61 × 10-9 g·mm·mm-2·s-1. Molecular dynamics (MD) simulations revealed strong non-covalent interactions and exceptional compatibility between starch and PA. Furthermore, the integration of pectin and geraniol improved the mechanical strength and antimicrobial properties of the modified films compared to unmodified starch films. These environmentally friendly and biodegradable starch-based films present a promising option for sustainable packaging materials in food preservation.

Influence of bio-coupling agent on interfacial interlocking compatibility and toughness of ultrafine bamboo charcoal/polylactic acid composite film.

Applications for polylactic acid (PLA) are significantly impacted by its poor mechanical properties and lack of thermal stability. The goal of this work is to bridge the gap of poor compatibility among the components and enhance their interface interlocking capability to improve the toughness and thermal stability. Ultrafine bamboo charcoal (UFBC) was treated through deep eutectic solvent (DES) method to deposit sodium lignosulfonate (LS) on its surface. LS was used with PLA as a bio-coupling agent to create an eco-friendly PLA composite film with a wide range of characteristics. Benefiting from the penetration of PLA to the internal pores in UFBC, the resultant L-UFBC/PLA film has a good mechanical interlocking structure. Ls can increase the compatibility and strengthen the interface interlocking capability through DES method, which greatly improves the mechanical properties of the system. In comparison to pure PLA one, the elongation at break was 136.24 % greater, and the crystallinity (Xc) increased from 1.09 % to 3.33 %. Furthermore, the thermal stability of the system was also improved, and the residual at 600 °C rose by 4.83 %. These characteristics offer the prepared L-UFBC/PLA film a wide range of potential applications in the packaging, medical, agricultural, and other sectors.

Ferroelectric BaTiO3 Regulating the Local Electric Field for Interfacial Stability in Solid-State Lithium Metal Batteries.

Solid-state Li metal batteries (SSLMBs) are widely investigated since they possess promising energy density and high safety. However, the poor interfacial compatibility between the electrolyte and electrodes limits their promising development. Herein, a robust composite electrolyte (poly(vinyl ethylene carbonate) electrolyte with 3 wt % of BaTiO3, PVEC-3BTO) with excellent interfacial performance is rationally designed by incorporating ferroelectric BaTiO3 (BTO) nanoparticles into the poly(vinyl ethylene carbonate) (PVEC) electrolyte matrix. Benefiting from the high dielectric constant and ferroelectric properties of BTO, the interfacial compatibility between electrolytes and electrodes was significantly improved. The enhanced Li+ transference number (0.64) of solid electrolyte and in situ generated BaF2 inorganic interphase contribute to the enhanced cycling stability of PVEC-3BTO based Li//Li symmetrical batteries. Furthermore, the antioxidation ability of PVEC-3BTO has also been enhanced by modulating the local electric field for good pairing with high-voltage LiCoO2 material. Therefore, in this work, the mechanism of BTO for improving interfacial compatibility is revealed, and also useful methods for addressing the interface issues of SSLMBs have been provided.

Particle-Solid Transition Architecture for Efficient Passive Building Cooling.

Electricity consumption for building cooling accounts for a significant portion of global energy usage and carbon emissions. To address this challenge, passive daytime radiative cooling (PDRC) has emerged as a promising technique for cooling buildings without electricity input. However, existing radiative coolers face material mismatch issues, particularly on cementitious composites like concrete, limiting their practical application. Here, we propose a cementitious radiative cooling armor based on a particle-solid transition architecture (PSTA) to overcome these challenges. The PSTA design features an asymmetric yet monolithic morphology and an all-inorganic nature, decoupling radiative cooling from building compatibility while ensuring UV resistance. In the PSTA design, nanoparticles on the surface serve as sunlight scatterers and thermal emitters, while those embedded within a cementitious substrate provide build compatibility and cohesiveness. This configuration results in enhanced interfacial bonding strength, high solar reflectance, and strong mid-infrared emittance. Specifically, the PSTA delivers an enhanced interfacial shear strength (0.93 MPa), several-fold higher than that in control groups (metal, glass, plastic) along with a cooling performance (a subambient temperature drop of ∼6.6 °C and a cooling power of ∼92.8 W under a direct solar irradiance of ∼680 W/m2) that rivals or outperforms previous reports. Importantly, the design concept of the PSTA is applicable to various particles and solids, facilitating the practical application of PDRC technology in building scenarios.

Chemically bonding inorganic fillers with polymer to achieve ultra-stable solid-state sodium batteries.

Inorganic/organic composite solid electrolytes (CSEs) have attracted ever-increasing attentions due to their outstanding mechanical stability and processibility. However, the inferior inorganic/organic interface compatibility limits their ionic conductivity and electrochemical stability, which hinders their application in solid-state batteries. Herein, we report a homogeneously distributed inorganic fillers in polymer by in-situ anchoring SiO2 particles in polyethylene oxide (PEO) matrix (I-PEO-SiO2). Compared with ex-situ CSEs (E-PEO-SiO2), SiO2 particles and PEO chains in I-PEO-SiO2 CSEs are closely welded by strong chemical bonds, thus addressing the issue of interfacial compatibility and realizing excellent dendrite-suppression ability. In addition, the Lewis acid-base interactions between SiO2 and salts facilitate the dissociation of sodium salts and increase the concentration of free Na+. Consequently, the I-PEO-SiO2 electrolyte demonstrates an improved Na+ conductivity (2.3 × 10-4 S cm-1 at 60 °C) and Na+ transference number (0.46). The as constructed Na3V2(PO4)3 ‖ I-PEO-SiO2 ‖ Na full-cell demonstrates a high specific capacity of 90.5 mAh g-1 at 3C and an ultra-long cycling stability (>4000 cycles at 1C), outperforming the state-of-the-art literatures. This work provides an effective way to solve the issue of interfacial compatibility, which can enlighten other CSEs to overcome their interior compatibility.

High strength, controlled release of curcumin-loaded ZIF-8/chitosan/zein film with excellence gas barrier and antibacterial activity for litchi preservation.

Polysaccharide films containing protein additives have good application prospects in agriculture and food field. However, interfacial incompatibility between hydrophobic proteins and hydrophilic polymers remains a major technical challenge. In this work, the interfacial compatibility between hydrophobic zein and hydrophilic chitosan (CS) is improved by the chemical crosslinking between zinc ions of curcumin-loaded zeolitic imidazolate framework-8 (Cur-ZIF-8) with CS and zein. With the improvement of interface compatibility, the results show that the elongation at break and O2 barrier property of synthesized Cur-ZIF-8/CS/Zein are 9.2 and 1.5 times higher than CS/Zein, respectively. And the Cur-ZIF-8/CS/Zein exhibits superior antibacterial and antioxidant properties as well. Importantly, Cur-ZIF-8/CS/Zein can also be used as an intelligent-responsive release platform for curcumin. As a result, Cur-ZIF-8/CS/Zein can keep the freshness and appearance of litchi at least 8 days longer than that of CS/Zein. Therefore, this study provides a novel method to improve the interfacial compatibility between hydrophobic proteins and hydrophilic polymers, and is expected to expand the application of protein/polymer composites in agriculture and food field.

Flexible and Mechanically Enhanced Polyurethane Composite for γ-ray Shielding and Thermal Regulation.

Microencapsulation of paraffin with lead tungstate shell (Pn@PWO) shows the drawbacks of low wettability and poor leakage-proof property and thermal reliability, restricting the application of phase change microcapsules. Herein, a novel paraffin@lead tungstate@silicon dioxide double-shelled microcapsule (Pn@PWO@SiO2) has been successfully constructed by the emulsion-templated interfacial polycondensation and applied in the waterborne polyurethane (WPU). The results indicated that a SiO2 layer with controlled thickness was formed on the PbWO4 shell. The Pn@PWO@SiO2 microcapsules have exhibited superior leakage-proof properties and thermal reliability through double-shelled protection, and the leakage rate decreased by at least 54.11% compared to that of Pn@PWO microcapsules. The SiO2 layer with abundant polar groups ameliorated the wettability of microcapsules and the interfacial compatibility between microcapsules and the WPU matrix. The tensile strength of WPU/Pn@PWO@SiO2-2 composites reached 10.98 MPa, which was over 7 times greater than that of WPU/Pn@PWO composites. In addition, WPU/Pn@PWO@SiO2-2 composites with a latent heat capacity of over 41 J/g exhibited efficient phase change stability and γ-ray shielding properties. Also, the mass attenuation coefficients reached 1.38 cm2/g at 105.3 keV and 1.12 cm2/g at 86.5 keV, respectively. These properties will greatly promote the application of WPU/Pn@PWO@SiO2 composites into γ-ray-shielding devices with thermal regulation.

Embedding of Laser Generated TiO2 in Poly(ethylene oxide) with Boosted Li+ Conduction for Solid-State Lithium Metal Batteries.

Poly(ethylene oxide) (PEO)-based solid polymer electrolytes are considered promising materials for realizing high-safety and high-energy-density lithium metal batteries. However, the high crystallinity of PEO at room temperature triggers low ionic conductivity and Li+ transference number, critically hindering practical applications in solid-state lithium metal batteries. Herein, we prepared nanosized TiO2 with enriched oxygen vacancies down to 13 nm as fillers by laser irradiation, which can be coated by in situ generated polyacetonitrile, ensuring good dispersibility in PEO. The electrolytes with nanosized TiO2 show a combination of high ionic conductivity, high Li+ transference number, superior electrochemical stability, and enhanced mechanical robustness. Accordingly, the lithium symmetric batteries with nanosized TiO2 composite solid electrolytes exhibit a stable cycling life up to 590 h at 0.25 mA cm-2. The full Li metal batteries paired with a LiFePO4 cathode deliver superior durability for 550 cycles. Moreover, the proof-of-concept pouch cells demonstrate excellent safety performance under various harsh conditions. This work provides a realistic guide in designing novel fillers to achieve stable operation of high-safety and energy-dense solid-state lithium metal batteries.