Chain Segments Research Articles

Efficient Alcoholysis of Poly(ethylene terephthalate) by Using Supercritical Carbon Dioxide as a Green Solvent.

In order to reduce the environmental impact of poly(ethylene terephthalate) (PET) plastic waste, supercritical fluids were used to facilitate effective recovery via improved solvent effects. This work focuses on the mechanisms of supercritical CO2 (ScCO2) during the alcoholysis processing of PET using systematic experiments and molecular dynamics (MD) simulations. The results of the alcoholysis experiment indicated that PET chips can be completely depolymerized within only an hour at 473 K assisted with ScCO2 at an optimal molar ratio of CO2/ethanol of 0.2. Random scission of PET dominates the early stage of the depolymerization reaction process, while specific scission dominates the following stage. Correspondingly, molecular dynamics (MD) simulations revealed that the solubilization and self-diffusion properties of ScCO2 facilitate the transportation of alcohol molecules into the bulk phase of PET, which leads to an accelerated diffusion of both oligomers and small molecules in the system. However, the presence of excessive CO2 has a negative impact on depolymerization by weakening the hydrogen bonding between polyester chain segments and ethanol, as well as decreasing the swelling degree of PET. These data provide a deep understanding of PET degradation by alcohols and the enhancement of ScCO2. It should be expected to achieve an efficient and high-yield depolymerization process of wasted polyesters assisted with ScCO2 at a relatively low temperature.

Controllable Synthesis of Titanium Silicon Molecular Zeolite Nanosheet with Short b-Axis Thickness and Application in Oxidative Desulfurization.

Titanium silicon molecular zeolite (TS-1) plays an important role in catalytic reactions due to its unique nanostructure. The straight channel on TS-1 was parallel to the orientation of the short b-axis and directly exposed to the aperture of the 10-member ring with a diameter of 0.54 nm × 0.56 nm. This structure could effectively reduce the diffuse restriction of bulk organic compounds during the oxidative desulfurization process. As a kind of cationic polymer electrolyte, polydimethyldiallyl ammonium chloride (PDDA) contains continuous [C8H16N+Cl-] chain segments, in which the Cl- could function as an effective structure-directing agent in the synthesis of nanomaterials. The chain of PDDA could adequately interact with the [0 1 0] plane in the preparation process of zeolite, and then the TS-1 nanosheet with short b-axis thickness (6 nm) could be obtained. The pore structure of the TS-1 nanosheet is controlled by regulating the content of PDDA. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), N2 physical adsorption analysis, infrared absorption spectrum and ultraviolet-visible spectrum were used to determine the TS-1. The thinner nanosheets exhibit excellent catalytic performance in oxidative desulfurization of dibenzothiophene (DBT), in which the removal rate could remain at 100% after three recycles. Here, the TS-1 nanosheet with short b-axis thickness has a promising future in catalytic reactions.

Sizing agent induces the oriented attachment of 2D nanosheets for preparing high-performance carbon fiber composites

Inducing highly oriented 2D nanosheets to create a mussel-inspired interface phase on the carbon fiber (CF) surface to enhance its composites’ strength and toughness has become a great challenge. In this study, a novel coating was synthesized to induce the graphene oxide (GO) oriented distributed on the CF surface while constructing a biomimetic "Brick-and-Mortar" structural interface phase, which simultaneously promoted the strength and toughness of CF composites. Acting as a sizing agent, di-pyrene terminated PEG (py-PEG-py) facilitates abundant π-π* stacking interactions, and enables flexible chain segment motion during interface fracture of composites, as well as effectively improving the toughness of composites. Eventually, the formation of a superior mechanism on the CF surface results in remarkable properties for composites, including an interfacial shear strength (IFSS) of 99.3 MPa, interlaminar shear strength of 93.2 MPa, and flexural strength of 1430 MPa. The tensile strength and toughness increased to 1777 MPa and 45.0 MJm−3, respectively. Simultaneously, the continuous thermal conduction pathway produced by the oriented attachment of GO on the CF surface increased in-plane thermal conductivity. The reinforcing mechanisms of the unique mussel-inspired coating were systematically investigated. This work opens up an effective and scalability avenue for obtaining high-performance CF composites.

Micropore engineering of polyamide loose nanofiltration membrane for efficient dye/salt separation

Loose nanofiltration membranes (LNF) with efficient sieving and excellent permeance are desirable for dye/salt separation, and engineering the micropore of the LNF membranes is a promising approach to maximize membrane performance. Herein, we present a highly permeable and sieving polyamide LNF membrane with high porosity and suitable pore size that is prepared by interfacial polymerization using twisted aqueous phase monomer and subsequent alkali-treatment. The large-size, rigid and twisted structure of the adamantane-1,3-diamine effectively inhibits the dense-packing of polymer chain segments, resulting in a polyamide membrane with enhanced porosity and enlarged pore size. The alkali treatment hydrolyzes the partial amide linkage to further enlarge the membrane pore size, increasing the flux while maintaining high dye rejection. The optimum membrane exhibits a high salt/dye selective factor of 735 for Na2SO4/Evans blue and an excellent water permeance of 87.72 L m−2 h−1 bar−1. This study is expected to provide a valuable guidance for the targeted design and fabrication of LNF membranes.

Suppression of Segmental Chain Dynamics on a Particle's Surface in Well-Dispersed Polymer Nanocomposites.

The Rouse dynamics of polymer chains in model nanocomposite polyethylene oxide/silica nanoparticles (NPs) was investigated using quasielastic neutron scattering. The apparent Rouse rate of the polymer chains decreases as the particle loading increases. However, there is no evidence of an immobile segment population on the probed time scale of tens of ps. The slowing down of the dynamics is interpreted in terms of modified Rouse models for the chains in the NP interphase region. Thus, two chain populations, one bulk-like and the other characterized by a suppression of Rouse modes, are identified. The spatial extent of the interphase region is estimated to be about twice the adsorbed layer thickness, or ≈2 nm. These findings provide a detailed description of the suppression of the chain dynamics on the surface of NPs. These results are relevant insights on surface effects and confinement and provide a foundation for the understanding of the rheological properties of polymer nanocomposites with well-dispersed NPs.

Separating Charge Centers of Chain Segments in Dielectric Elastomer through Steric Hindrance Engineering.

Theoretically, separating the positive and negative charge centers of the chain segments of dielectric elastomers (DEs) is a viable alternative to the conventional decoration of chain backbone with polar handles, since it can dramatically increase the dipole vector and hence the dielectric constant (ε') of the DEs while circumvent the undesired impact of the decorated polar handles on the dielectric loss (tan δ). Herein, a novel and universal method is demonstrated to achieve effective separation of the charge centers of chain segments in homogeneous DEs by steric hindrance engineering, i.e., by incorporating a series of different included angle-containing building blocks into the networks. Both experimental and simulation results have shown that the introduction of these building blocks can create a spatially fixed included angle between two adjacent chain segments, thus separating the charge center of the associated region. Accordingly, incorporating a minimal amount of these building blocks (≈5mol%) can lead to a considerably sharp increase (≈50%) in the ε' of the DEs while maintaining an extremely low tan δ (≈0.006@1kHz), indicating that this methodology can substantially optimize the dielectric performance of DEs based on a completely different mechanism from the established methods.

Stearate‐Modified Montmorillonite and Polylactic Acid Synergistically Enhanced the Microcellular of Thermoplastic Polyurethane Elastomer Foam and Improved Its Dimensional Stability

Thermoplastic polyurethane (TPU) elastomer is a commonly used material for foam preparation. However, its application is hindered by significant shrinkage behavior. To reduce the foam shrinkage, polylactic acid (PLA) and calcium stearate‐modified montmorillonite (MMT‐St) are incorporated into the polyurethane matrix. The TPU/PLA/MMT‐St composite foams are formed using an intermittent supercritical carbon‐dioxide‐foaming process. The addition of PLA inhibits the relaxation of TPU chain segments, while the introduction of calcium stearate (GaSt2) improves the dispersion of MMT within the matrix, increases the nucleation sites of cell growth, and improves cell structure. The cell diameter decreases from 10 to 4 μm, while the cell density increased from 4.1 × 1012 to 15.8 × 1012 cell cm−3. In addition, the cell distribution range narrows from 4–19 to 2–6 μm. Incorporating MMT‐St increases the crystallinity and thermal stability of TPU/PLA, mitigates chain relaxation at room temperature, and enhances foam dimensional stability. As a result, this leads to a decrease in shrinkage rate from 27.5% to 5%. As both matrices of the material are thermoplastic, this composite foam possesses recyclability with enhanced material utilization.

Mechanically robust poly(urethane-imide) aerogels with excellent thermal insulation and sound absorption by ambient drying

Polyimide (PI) aerogels are the great candidates for sound absorption, thermal insulation and mechanical cushioning materials due to their low density, excellent mechanical properties and good thermal stability. However, the high shrinkage and hydrophilicity of PI aerogels, as well as the time-consuming and complexity of the process directly limit their wide application in many fields. Herein, a facile one-step method for the synthesis of porous monolithic poly(urethane-imide) (PUI) aerogels was successfully developed. Hydrothermal synthesis and ambient drying methods were adopted in the construction of monolithic chemically cross-linked PUI aerogels, which avoids the complex imidization process. PUI aerogels were homogeneously produced by a chemical cross-linking copolymerization reaction between polyurethane (PU) oligomers, Benzene-1,2,4,5-tetracarboxylic dianhydride (PMDA) and 1, 3, 5-tris (6-isocyanatohexyl)-1, 3, 5-triazine-2, 4, 6(1H, 3H, 5H)-trione without any catalysts. Interestingly, the introduction of linear flexible PU oligomers chain segments effectively prevented the shrinkage of the network backbone and enhanced the hydrophobicity of PUI aerogels. The obtained PUI aerogels have low density (0.196 g/cm3), low shrinkage (9.30%), high porosity (79.54%) and hydrophobicity (water contact angle of 129.2°). Under high pressure, PUI aerogel was compressed but not break and the compression Young's modulus as high as 3.638 MPa. Moreover, the thermal conductivity of PUI aerogels was only 59.92 mW/m/K at 150 °C. When the back cavity depth was 5 mm, the highest sound absorption coefficient of PUI aerogel was up to 0.7219. This work provides a new method for the development of lightweight, high-mechanical-strength polymer aerogels, and the prepared aerogels have a potential application in the field of multifunctional integrated sound absorption materials.

Synthesis of star‐shaped epoxy resin with excellent mechanical properties using triazine as a skeleton

AbstractThe high‐performance development of advanced resin matrix composites has resulted in higher requirements for the mechanical strength and toughness of epoxy resin matrices. However, enhancing the toughness of the epoxy resin while maintaining its mechanical strength remains a considerable challenge. In this study, we utilized triazine rings as the skeleton, and introduced flexible chain segments and other forces into the polymer cross‐linked network to fabricate a star‐shaped epoxy resin (CNE) with exceptional mechanical properties. Benefiting from its meticulously designed rigid‐flexible integrated structure, after curing by 4,4′‐diaminodiphenylmethane (DDM), it demonstrated outstanding mechanical properties. The storage modulus of CNE/DDM was measured at up to 5.48 GPa; moreover, its tensile modulus and strength went as high as 5.04 GPa and 134.72 MPa respectively, and it also exhibited an elongation at break of up to 3.35%. The mechanical properties of CNE/DDM are far superior to those of AFG‐90 (N,N‐diglycidyl‐4‐glycidyloxyaniline)/DDM. Over all, the findings of this study thus provide an effective synthesis pathway toward achieving epoxy resins with high modulus, strength, and toughness.

Engineering Biodegradable Polyurethanes with Precisely Controlled Hierarchical Structures to Access Shape Memory Effect and Enhanced Bioactivities.

Biodegradable polymers with shape memory effects (SMEs) offer promising solutions for short-term medical interventions, facilitating minimally invasive procedures and subsequent degradation without requiring secondary surgeries. However, achieving a good balance among desirable SMEs, mechanical performance, degradation rate, and bioactivities remains a significant challenge. To address this issue, we established a strategy to develop a versatile biodegradable polyurethane (PPDO-PLC) with tunable hierarchical structures via precise chain segment control. Initial copolymerization of l-lactide and ε-caprolactone sets a tunable Tg close to body temperature, followed by block copolymerization with poly(p-dioxanone) to form a hard domain. This yields a uniform microphase-separation morphology, ensuring robust SME and facilitating the development of roughly porous surface structures in alkaline environments. Cell experiments indicate that these rough surfaces significantly enhance cellular activities, such as adhesion, proliferation, and osteogenic differentiation. Our approach provides a methodology for balancing biodegradability, SMEs, three-dimensional (3D) printability, and bioactivity in materials through hierarchical structure regulation.

Dynamic covalent polymer network enabled bio‐based vitrimers with excellent substrate bonding

AbstractIn this article, we report the synthesis of dynamic covalent polymer network (DCPN)‐enabled vitrimers derived from gum rosin—a pine tree extract. The concept of Diels Alder (DA) thermo‐reversibility has been used to introduce self‐healing/dynamic covalent ability into the polymer systems. For this purpose, the diene moieties were incorporated in the gum rosin‐based polymer network, and the bismaleimides served as the dienophiles. The thermo‐reversible crosslinks formed between the diene and dienophile moieties can enhance the service life of the materials by improving the durability, mechanical as well as chemical properties of the materials. Upon damage, the thermo‐reversible DA bonds de‐crosslink resulting in smaller chain segments, enabling the material to flow to the site of damage and seal the fractured edges. The formation of DA crosslinks has been confirmed by using Fourier transform‐infrared spectroscopic technique. Scanning electron microscopy analysis was used to verify the self‐healing ability of the resin matrix. The healing process was studied after manual scratches were made. The polymers' ability to heal multiple times is investigated using differential scanning calorimetry. The adhesion strength of the self‐healing material has been examined on variety of substrates such as glass, steel, and concrete. The materials exhibited superior adhesion strength on glass substrate.

(Thermo)mechanical and chemical characteristics of photochemically crosslinked acrylates from bio‐ and fossil‐based origin

AbstractThe acrylates with oligomers and monomers from (partially) bio‐based feedstock become available at (semi‐)industrial scale, which can be processed through photochemical crosslinking for applications in coatings, additive manufacturing, electronics, or inks. Although fossil‐ and bio‐based acrylates may have a similar chemical composition, it requires good understanding of processing and structure–property relationships as minor changes in microstructure may strongly alter the performance. A comparative study on mechanical properties and chemical structure of bio‐ and fossil‐based acrylates with different functionalities and backbone structures reveals higher ductility of bio‐based acrylates, in relation with a more complex organization of the intrinsic molecular structure. The latter is confirmed by mechanical testing and visco‐elastic characteristics (dynamic mechanical analysis) yielding lower stiffness and higher dampening of bio‐based acrylates, in parallel with a lower glass transition temperature (differential scanning calorimetry). The complex molecular arrangements include a nanoscale morphology with ordered structure (X‐ray diffraction), conformational changes (infrared spectroscopy), and a residual high‐molecular weight fraction (size exclusion chromatography). The visco‐elastic calculations indicate only 4% to 5% lower crosslinking density and around 10% higher mean molar mass of the polymer chains segments between chemical crosslinks and trapped chain entanglements, which explain the unique structure and performance of bio‐based acrylates.

Surface Topology of Redox- and Thermoresponsive Nanogel Droplets.

Hydrogels are usually depicted as a homogenous polymer block with a distinct surface. While defects in the polymer structure are looked into frequently, structural irregularities on the hydrogel surface are often neglected. In this work, thin hydrogel layers of ≈100nm thickness (nanogels) are synthesized and characterized for their structural irregularities, as they represent the surface of macrogels. The nanogels contain a main-chain responsiveness (thermo responsive) and a responsiveness in the cross-linking points (redox responsive). By combining data from ellipsometry using box-model and two-segment-model analysis, as well as atomic force microscopy, a more defined model of the nanogel surface can be developed. Starting with a more densely cross-linked network at the silica wafer surface, the density of cross-linking gradually decreases toward the hydrogel-solvent interface. Thermo-responsive behavior of the main chain affects the entire network equally as all chain segments change solubility. Cross-linker-based redox-responsiveness, on the other hand, is only governed by the inner, more cross-linked layers of the network. Such dual responsive nanogels hence allow for developing a more detailed model of a hydrogel surface from free radical polymerization. It provides a better understanding of structural defects in hydrogels and how they are affected by responsive functionalities.

High energy-dissipation PDMS polymer-fluid-gels over an ultra-wide temperature range

Viscoelastic polymers exhibit strong energy dissipation in the glass transition region due to the motion of chain segments. Yet, the damping temperature ranges are pretty narrow, and the damping effect is poor at low frequencies. Here, we report two PDMS polymer-fluid-gels prepared by traditional curing and solvothermal polymerization, both of which exhibit excellent energy-dissipation capacity with loss factor larger than 0.7 at 1 Hz both covering 255 K (−55 °C to 200 °C), and larger than 1.0 at 1 Hz covering 134.7 K and 146.7 K, respectively, exceeding all the literature reports. Furthermore, solvothermal polymerization realizes large cross-linking meshes in which polymer fluids can stretch with less restriction and have longer relaxation time, which is conducive to low-frequency damping. The lower the frequency, the more pronounced the relative increase in damping, with the ratio of the two being greater than 4 times in the measuring low-frequency range. Moreover, the gels can absorb impact in extreme environments and protect raw eggs from breaking at temperatures as low as −50 °C when dropped from a height of 2 m.

Migration of polydimethylsiloxane chain segments toward the surface of UV-cured waterborne poly(urethane-acrylate) films

Waterborne polyurethane (WPU) has poor water resistance and low surface hydrophobicity due to the incorporation of hydrophilic chain-extender. The water resistance and the surface hydrophobicity can be improved by incorporation of polydimethylsiloxane (PDMS), which is attributed to the migration of PDMS chain segments toward the surface of WPU film. However, whether the PDMS chain segments can migrate toward the surface of WPU film after UV-curing, resulting in higher hydrophobicity, needs further investigation? We prepared the different WPUA films by changing the molar ratio of aminopropyl-terminated polydimethylsiloxane (APT-PDMS) to hydroxyethyl acrylate (HEA), to deeply understand the migrating phenomenon of PDMS chain segments toward the surface of WPUA films. The migration cause of PDMS chain segments and the influence of chemical cross-linking on the migration were investigated by thermal annealing and solvent immersion of WPUA films. In addition, the migration activation energy and the relaxation time were studied by the migration rate of PDMS chain segments in the thermal annealing and the rheological behavior of WPUA film, aiming to elucidate the migration of PDMS chain segments depending on the chain motion and the fractional free volume. This investigation provides a simple and feasible strategy for improving the hydrophobicity of waterborne polyurethane.

Generic low-density corrections to the equation of state of chain molecules with repulsive intermolecular forces.

Molecular-based equations of state for describing the thermodynamics of chain molecules are often based on mean-field like arguments that reduce the problem of describing the interactions between chains to a simpler one involving only nonbonded monomers. While for dense liquids such arguments are known to work well, at low density they are typically less appropriate due to an incomplete description of the effect of chain connectivity on the local environment of the chains' monomer segments. To address this issue, we develop three semi-empirical approaches that significantly improve the thermodynamic description of chain molecules at low density. The approaches are developed for chain molecules with repulsive intermolecular forces; therefore, they could be used as reference models for developing equations of the state of real fluids based on perturbation theory. All three approaches are extensions of Wertheim's first-order thermodynamic perturbation theory (TPT1) for polymerization. The first model, referred to as TPT1-v, incorporates a second-virial correction that is scaled to zero at liquid-like densities. The second model, referred to as TPT1-y, introduces a Helmholtz-energy contribution to account for correlations between next-nearest-neighbor segments within chain molecules. The third approach, called TPT-E, directly modifies TPT1 without utilizing an additional Helmholtz energy contribution. By employing TPT1 at the core of these approaches, we ensure an accurate description of mixtures and enable a seamless extension from chains of tangentially bonded hard-sphere segments of equal size to hetero-segmented chains, fused chains, and chains of soft repulsive segments (which are influenced by temperature). The low-density corrections implemented in TPT1 are designed to preserve these good characteristics, as confirmed through comparisons with novel molecular simulation results for the pressure of various chain fluids. TPT1-v exhibits excellent transferability across different chain types, but it relies on knowing the second virial coefficient of the chain molecules, which is non-trivial to obtain and determined here using Monte Carlo simulation. The TPT1-y model, on the other hand, achieves comparable accuracy to TPT1-v while being fully predictive, requiring no input besides the geometry of the chain molecules.

A unified kinetic analysis for the hyperbranched polymerization with ABg type monomers

The unified analytical expressions of the size distribution function and the degree of branching for the hyperbranched polymerization with ABg type monomers are developed by kinetic theory of polymerization, based on the ABg + ABh + Bf model. The effect of the reactant parameters, the monomers branching degree g and h, the monomers feed ratio r, the functionality f and feed ratio α of the core molecule Bf, on the molecular parameters of the products formed was investigated. Compared with the general polycondensation of ABg monomer or copolycondensation of ABg and AB monomer without core molecule, the presence of multifunctional core molecules makes the polydispersity index of the products go down fast when the reaction approaches completion. At the end of the reaction, the polydispersity index increases with increasing g, and decreases with increasing α and f. For the ABg + AB + B3 polycondensation system, within the range of the feed ratio of ABg monomer less than 0.3, the average chain segment length significantly decreases with the increasing r, and then the change becomes moderate with its further increase. For g > 2, the average chain segment length shows a shallow minimum with increasing r. The degree of branching, fractions of terminal and branching units also show maximum value with the change of monomer feed ratio r. The information obtained in this work can help people understand the structure of ABg type hyperbranched polymers and carry out molecular design.

Potential of Establishing Industrial Hemp Value Chains in Northern Australia

Globally, industrial hemp offers consumers with over 25,000 value-added products that are valued at approximately US$4.2 billion of current market value and likely to surpass US$26.6 billion by 2025. In Northern Australia, the industrial hemp sector is at infancy stages of development. Given the suitability of certain Northern Australia’s geographical zones in terms of soil, water, and climate, a study was conducted to identify potential industrial hemp value chains. Probable value chains were developed by characterizing the production to market segments of the supply chains to determine the return on investment and analyzing the capacity of the stakeholders in terms of communication and relationships. Consequently, the strengths, weaknesses, opportunities and threats (SWOT) of the developed value chains were analyzed. This study collected data from three complementary sources that included review of the literature, results of variety trials evaluation conducted in Northern Australia, and survey of hemp industry stakeholders. Results suggested that Northern Australia offers conducive growing conditions for hemp that allows for the development of three value chains including seed, fiber and silage. The research recommended ongoing investment in the industry through engagement of public and private sector while focusing on further establishment of the industry.

Preparation and Performance Study of HTPB-g-(PNIPAM/PEG) Thermoresponsive Polymer Brush.

In recent years, a great deal of work has been devoted to the development of thermoresponsive polymers that can be made into new types of smart materials. In this paper, a branched polymer, HTPB-g-(PNIPAM/PEG), with polyolefin chain segments as the backbone and having polyethylene glycol (PEG) and poly(N-isopropylacrylamide) (PNIPAM) as side chains was synthesized by ATRP and click reactions using N3-HTPB-Br as the macroinitiator. This initiator was designed and synthesized using hydroxyl-terminated polybutadiene (HTPB) as the substrate. The temperature-responsive behavior of the branched polymer was investigated. The lower critical solution temperature (LCST) of the branched polymer was determined by ultraviolet and visible spectrophotometry (UV-vis) and was found to be 35.2 °C. The relationship between the diameter size of micelles and temperature was determined by dynamic light scattering (DLS). It was found that the diameter size changed at 36 °C, which was nearly consistent with the result obtained by UV-vis. The results of the study indicate that HTPB-g-(PNIPAM/PEG) is a temperature-responsive polymer. At room temperature, the polymer can self-assemble into composite micelles, with the main chain as the core and the branched chain as the shell. When the temperature was increased beyond LCST, the polyolefin main chain along with the PNIPAM branched chain assembled to form the nucleus, and the PEG branched chain constituted the shell.

Polyester-enhanced poly (cyclic carbonate-fluoride)-based polymer electrolyte for stable circulating solid lithium batteries

Polymer solid-state electrolytes have become one of the promising materials for constructing solid-state lithium batteries due to their excellent processability and good compatibility with electrode interfaces. However, their limited electrochemical performance and mechanical strength have hindered their widespread application. Through the adoption of an in-situ thermal curing method, we successfully prepared a poly(carbonate-fluoride) solid-state electrolyte, utilizing a polyester separator with abundant polar groups as a reinforcing framework. The introduction of ionic liquid into the solid polymer electrolyte not only enhances the mobility of polymer chain segments to improve ionic conductivity but also, in synergy with trifluoromethyl, promotes lithium salt dissociation while restricting the migration of lithium salt anions. Additionally, their reaction with the lithium metal anode generates the LiF-rich SEI, regulating the deposition of lithium dendrites. The resulting 31VPIF/OZ exhibited outstanding ionic conductivity (3.58 × 10−4 S cm−1 at 25 °C), Li-ion migration number (0.52), and electrochemical window (5.4 V). Li | 31VPIF/OZ | Li battery cycled for 1000 h at 0.1 mA cm−2 without short-circuiting. Importantly, Li | | LiFePO4 battery demonstrated a high capacity retention rate of 91.5 % after 600 cycles at 0.5C (25 °C). Thus, through the synergistic interplay of polymer structure design and fillers, we have successfully achieved stable cycling in solid-state lithium batteries, providing robust support for their application in rechargeable lithium battery technology.