Supramolecular materials that combine toughness, transparency, self-healing, and environmental stability are crucial for advanced applications, such as flexible electronics, wearable devices, and protective coatings. However, integrating these properties into a single system remains challenging because of the inherent trade-offs between the mechanical strength, elasticity, and structural reconfigurability. Herein, we report a supramolecular ionogel designed via a simple one-step polymerization strategy that combines hydrogen bonding and ion-dipole interactions in a physically crosslinked network. This dual-interaction architecture enables the ionogel to achieve high tensile strength (9 MPa), remarkable fracture toughness (23.6 MJ·m⁻³), and rapid self-healing under mild thermal stimulation. The material remains highly transparent and demonstrates excellent resistance to moisture, acid, and salt environments, with minimal swelling and performance degradation. Furthermore, it effectively dissipates over 80 MJ·m⁻³ of energy during high-speed impacts, providing reliable protection to fragile substrates. This study offers a broadly applicable molecular design framework for resilient and adaptive soft materials.

Exploration of new green polymerization strategies for the construction of conjugated polymers is important but challengeable. In this work, a multicomponent polymerization of acetylarenes, alkynones and ammonium acetate for in situ construction of conjugated poly(triarylpyridine)s was developed. The polymerization reactions of diacetylarenes, aromatic dialkynones and NH₄OAc were performed in dimethylsulfoxide (DMSO) under heating in the presence of potassium tert-butoxide (t-BuOK), affording four conjugated poly(2,4,6-triarylpyridine)s (PTAPs) in satisfactory yields. The resulting PTAPs have good solubility in common organic solvents and high thermal stability with 5% weight loss temperatures reaching up to 460 °C. They are also electrochemically active. The PTAPs incorporating tetraphenylethene units manifest aggregation-induced emission features. Moreover, through simply being doped into poly(vinyl alcohol) (PVA) matrix, the polymer and model compound containing triphenylamine moieties exhibit room-temperature phosphorescence properties with ultralong lifetimes up to 696.2 ms and high quantum yields up to 28.7%. This work not only provides a facile green synthetic route for conjugated polymers but also offers new insights into the design of advanced materials with unique photophysical properties.

It is important to understand the evolution of the matter on the polymer membrane surface. The in situ and real-time monitoring of the membrane surface will not only favor the investigation of selective layer formation but can also track the fouling process during operation. Herein, an aggregation-induced emission (AIE)-active polymer membrane was prepared by the interfacial polymerization of a cyclodextrin-based glycocluster (CD@Glucose) and a tetraphenylethylene derivative modified with boronic acid groups (TPEDB) on the surface of a polyacrylonitrile (PAN) ultrafiltration membrane. This interfacial polymerization method can be stacked layer-by-layer to regulate the hydrophilicity and pore structure of the membrane. With the increase in the number of polymer layers, the separation and antifouling properties of the membrane gradually improved. Owing to the AIE property of the crosslinking agent TPEDB, the occurrence of interfacial polymerization and the degree of fouling during membrane operation can be monitored by the fluorescence distribution and intensity. With the aggravation of membrane fouling, the fluorescence decreased gradually, but recovered after cleaning. Therefore, this AIE effect can be used for real-time monitoring of interfacial polymerization as well as membrane fouling.

Polymer acceptor configuration and aggregation behavior are critical in determining the photovoltaic performance of all-polymer solar cells (all-PSCs). Effectively manipulating polymer self-aggregation through structural design to optimize the blend morphology remains challenging. Herein, we present a simple yet effective design strategy to modulate the aggregation behavior of the Y-series-based polymer acceptor PY-V-γ by introducing a pendant-fluorinated Y-series acceptor (Y2F-ET) into the main-conjugated backbone. Two random copolymer acceptors (PY-EY-5 and PY-EY-20) were synthesized with varying molar fractions of Y2F-ET pendant monomers. Our findings revealed that both the solution-phase and solid-state aggregation behaviors were progressively suppressed as the Y2F-ET content increased. Compared to the highly self-aggregating PY-V-γ-based all-PSCs, the more amorphous PY-EY-5 enabled devices to achieve an increased device efficiency from 17.31% to 18.45%, which is attributed to the slightly smaller polymer phase-separation domain sizes and reduced molecular aggregation in the PM6:PY-EY-5 blend. Moreover, the finely tuned blend morphology exhibited superior thermal stability, underscoring the significant advantages of the Y-series pendant random copolymerization approach.

The design of low-cost and high-performance cyclic olefin copolymers remains challenging. Ethylene copolymers with dicyclopentadiene (DCPD) were prepared using Ph₂C(Cp)(Flu)ZrCl₂ (Cat. 1), rac-Et(Ind)₂ZrCl₂ (Cat. 2), Me₂C(Cp)(Flu)ZrCl₂ (Cat. 3) and Me₂Si(Ind)₂ZrCl₂ (Cat. 4) combined with [Ph₃C][B(C₆F₅)₄]/ⁱBu₃Al. Ni(acac)₂/ⁱBu₃Al was then used to catalyze the hydrogenation of the intracyclic double bonds of ethylene/DCPD copolymers. The results showed that compared to C₂ symmetric catalysts (Cat. 2 and Cat. 4), C_s symmetric catalysts (Cat. 1 and Cat. 3) facilitated the incorporation of copolymers with higher DCPD. ¹H- and ¹³C-NMR spectra indicated that ethylene/DCPD copolymerization occurred via enhancement of the norbornene ring. Additionally, measurement of the reactivity ratios provided further confirmation that the copolymers had random sequence distributions. All these samples demonstrated transmittance values above 90% in the visible wavelength range from 400 nm to 800 nm. By changing the fraction of monomers, the glass transition temperature, refractive index, Young's modulus, and tensile strength of the copolymer increased as the incorporation of DCPD increased, whereas the Abbe number and elongation at break decreased. Compared with ethylene/norbornene and ethylene/tetracyclicdodecene copolymers, ethylene/DCPD copolymers, with excellent optical and mechanical properties, are promising materials.

The sulfonated poly(α-methyl styrene-b-isobutylene-b-α-methyl styrene) copolymers (S-ASIBS) with the average molar percentage of sulfonic acid (－SO₃H) groups (SP) ranging from 3.6 mol% to 14.3 mol% could be synthesized by sulfonation of ASIBS with acetyl sulfate. The hydrophilic ionic channels were generated for proton exchange membranes (PEMs) by ion aggregation of －SO₃H groups and microphase separation between hydrophobic polyisobutylene and hydrophilic sulfonated poly(α-methyl styrene) segments in S-ASIBS. The proton transport ability was improved while oxidative stability was decreased by increasing SP in S-ASIBS. The appropriate SP of about 12.7 mol% in S-ASIBS provides the available PEMs with high proton transport ability, low methanol permeability and good oxidative stability. The absence of active tertiary hydrogen atoms along S-ASIBS copolymer chains avoids their attack by peroxy radicals. The residual rates of weight (RW) and proton conductivity (Rσ) of S-ASIBS-12.7 membrane after oxidation treatment for 916 h were 84.3% and 88.1% respectively, near to those of commercial Nafion 117 (RW = 87.9%, Rσ = 90.3%). The membrane electrode assembly (MEA) could be prepared by using various S-ASIBS as PEMs for direct methanol fuel cell. The single cell with S-ASIBS-12.7 MEA behaves high performance of open circuit voltage (OCV) of 548 mV and peak power density (P_max) of 36.1 mW·cm^–2, which is similar to those of Nafion 117 (OCV = 506 mV, P_max = 35.6 mW·cm^–2). To the best of our knowledge, this is the first example of advanced S-ASIBS membrane with high proton conductivity, excellent fuel barrier property and remarkable oxidative stability for promising PEMs.

Herein, the effect of in situ formation of the stereocomplex polylactide (sc-PLA) on the crystallization behaviors of poly(L-lactide)/poly(D-lactide) (PLLA/PDLA) blends was assessed. When the melt-blending temperature of the PLLA/PDLA blend approached the melting temperature of sc-PLA (approximately 220 °C), a higher relative content of sc-PLA was achieved. Additionally, the relative content of sc-PLA in the PLLA/PDLA blend increased progressively with the increase in PDLA content. Differential scanning calorimetry analysis revealed that the overall crystallization rate of the homocrystal polylactide were enhanced by the presence of sc-PLA. After crystallization at the same temperature (115 and 120 °C), the PLLA/PDLA blends exhibited a shorter half-crystallization time compared to PLLA alone. The size of the microcrystals of PLLA decreased as the sc-PLA content increased. Furthermore, the storage modulus and complex viscosity of the PLLA/PDLA blend increased with higher sc-PLA content. Dynamic mechanical analysis indicated that the glass transition temperature of PLLA in the PLLA/PDLA blends increased with increasing sc-PLA content. Additionally, the Vicat softening temperature increased from 67.8 °C for PLLA alone to 164.7 °C for the PLLA/25PDLA blend, enhancing the heat resistance of the PLLA/PDLA blends. Compared to PLLA alone, the hydrolytic resistance of the PLLA/PDLA blends showed marked improvement.

Integrated conductive elastomers with excellent mechanical performance, stable high conductivity, self-healing capabilities, and high transparency are critical for advancing wearable devices. Nevertheless, achieving an optimal balance among these properties remains a significant challenge. Herein, through in situ free-radical copolymerization of 2-[2-(2-methoxyethoxy)ethoxy]ethyl acrylate (TEEA) and vinylimidazole (VI) in the presence of polyethylene glycol (PEG; M_n=400), tough P(TEEA-co-VI)/PEG elastomers with multiple functionalities were prepared, in which P(TEEA-co-VI) was dynamically cross-linked by imidazole-Zn²⁺ metal coordination crosslinks, and physically blended with PEG as polymer electrolyte to form a homogeneous mixture. Notably, Zn²⁺ has a negligible impact on the polymerization process, allowing for the in situ formation of numerous imidazole-Zn²⁺ metal coordination crosslinks, which can effectively dissipate energy upon stretching to largely reinforce the elastomers. The obtained P(TEEA-co-VI)/PEG elastomers exhibited a high toughness of 10.0 MJ·m^–3 with a high tensile strength of 3.3 MPa and a large elongation at break of 645%, along with outstanding self-healing capabilities due to the dynamic coordination crosslinks. Moreover, because of the miscibility of PEG with PTEEA copolymer matrix, and Li⁺ can form weak coordination interactions with the ethoxy (EO) units in PEG and PTEEA, acting as a bridge to integrate PEG into the elastomer network. The resulted P(TEEA-co-VI)/PEG elastomers showed high transparency (92%) and stable high conductivity of 1.09×10^–4 S·cm^–1. In summary, the obtained elastomers exhibited a well-balanced combination of high toughness, high ionic conductivity, excellent self-healing capabilities, and high transparency, making them promising for applications in flexible strain sensors.

The stretching-induced phase transition of biodegradable poly(butylene succinate) (PBS) was explored using a combination of mechanical testing and in situ wide angle X-ray diffraction characterization. The phase transition from α phase to β phase can be effectively triggered by severe stretching, in which the threshold strain is dependent on the PBS crystallites. Interestingly, this α-β phase transition can be reversed immediately once mechanical stretching begins to be released. It should be pointed out that the finish of β-α phase transition reversed, corresponding to the disappearance of the generated β phase, does not necessarily need the external stretching to completely release. For the relaxation-reversed phase transition, the evolution of the normalized β-phase fraction exhibited a similar correlation with the stress released. It was indicated that the decay kinetics followed a stretching-dominant mechanism, and the amount of β phase generated just prior to relaxation had a negligible influence on the reversed phase transition.

This paper presents a polymer-brush-guided templating strategy for fabricating ordered gold plasmonic architectures. The synthesized nanostructures featuring densely packed Au nanoparticles (NPs) exhibited strong surface-enhanced Raman scattering (SERS) activity. Using a simple mechanical transfer technique, these assemblies were integrated into flexible polydimethylsiloxane (PDMS) films. Polymer encapsulation during synthesis ensures structural integrity during processing, resulting in a mechanically robust SERS substrate with exceptional analytical performance. This platform achieved 4-mercaptobenzoic acid (4-MBA) detection at 100 pmol/L (10⁻¹⁰ mol/L) with high reproducibility (RSD=6.8%). Environmental and mechanical stability tests demonstrated 95% signal retention over 30 days and sustained functionality after 100 bending/twisting cycles. Combined with a non-destructive adhesion-transfer protocol, the substrate enabled on-site thiram detection on apple surfaces (1 μmol/L limit). This study provides a scalable approach for developing flexible SERS devices for food safety monitoring and environmental analysis.

High-entropy polymer blends composed of polypropylene (PP), polystyrene (PS), polyamide 6 (PA6), poly(lactic acid) (PLA), and styrene-ethylene-butylene-styrene (SEBS) were successfully fabricated using maleic anhydride-grafted SEBS (SEBS-g-MAH) as a compatibilizer. Dynamic mechanical analysis (DMA), differential scanning calorimetry (DSC), scanning electron microscopy (SEM), and mechanical testing demonstrated that SEBS-g-MAH significantly enhanced the compatibility between the polar (PA6, PLA) and nonpolar (PP, PS, SEBS) components. The compatibilizer effectively refined the microstructure, substantially reduced the domain sizes, and blurred the phase boundaries, indicating enhanced interfacial interactions among all the components. The optimal compatibilizer content (15 wt%) notably increased tensile ductility (elongation at break from 5.0% to 23.7%) while maintaining balanced crystallization behavior, despite slightly decreasing modulus. This work not only demonstrates the broad applicability of high-entropy polymer blends as a sustainable strategy for converting complex, unsorted plastic waste into high-performance value-added materials that significantly contribute to plastic upcycling efforts, but also highlights intriguing physical phenomena emerging from such complex polymer systems.

To retain its inherent biodegradability, simultaneously improving the strength and toughness of poly(lactic acid) (PLA) is a significant challenge. In this study, we propose an innovative multiple dynamic pressure (MDP) process that can produce pure PLA with excellent mechanical properties. The MDP process generates a dynamic stretching effect by regulating the application and release of pressure, prompting disordered molecular chains to be arranged regularly along the direction of the dynamic force field. This promoted the formation of more ordered crystal forms (α-form) and strengthened the connection between the crystalline and amorphous regions. Results show that after MDP treatment, the tensile strength and strain at break of MDP-PLA are significantly improved, reaching 91.6 MPa and 80.1% respectively, which are 49.4% higher and 10 times higher than those of the samples before treatment. The mechanical properties of MDP-PLA can be regulated as needed by adjusting the cycle times and peak pressure. In addition, through a systematic study of the structural evolution of MDP-PLA, the performance regulation mechanism of the MDP process was thoroughly investigated, and the internal relationship among the process-structure-performance was clarified. This research not only opens a new technical path for the preparation of high-performance pure PLA but also provides important guidance for the high-performance modification of other semi-crystalline polymers, thus possessing significant scientific and engineering value.

In rotationally extruded fittings, high-density polyethylene (HDPE) pipes prepared using conventional processing methods often suffer from poor pressure resistance and low toughness. This study introduces an innovative rotary shear system (RSS) to address these deficiencies through controlled mandrel rotation and cooling rates. We successfully prepared self-reinforced HDPE pipes with a three-layer structure combining spherical and shish-kebab crystals. Rotational processing aligned the molecular chains in the ring direction and formed shish-kebab crystals. As a result, the annular tensile strength of the rotationally processed three-layer shish-kebab structure (TSK) pipe increased from 26.7 MPa to 76.3 MPa, an enhancement of 185.8%. Notably, while maintaining excellent tensile strength (73.4 MPa), the elongation at break of the spherulite shish-kebab spherulite (SKS) tubes was improved to 50.1%, as compared to 33.8% in the case of shish-kebab spherulite shish-kebab (KSK) tubes. This improvement can be attributed to the changes in the micro-morphology and polymer structure within the SKS tubes, specifically due to the formation of small-sized shish-kebab crystals and the low degrees of interlocking.In addition,2D-SAXS analysis revealed that KSK tubes have higher tensile strength due to smaller crystal sizes and larger shish dimensions, forming dense interlocking structures. In contrast, the SKS and TSK tubes had thicker amorphous regions and smaller shish sizes, resulting in reduced interlocking and mechanical performance.

Development of polymers with underwater self-healing and antifouling properties is crucial, particularly in harsh marine environments. In this study, polydimethylsiloxane (PDMS)-based antifouling polymers with tunable self-healing capabilities in aqueous conditions were fabricated by incorporating amphiphilic segments and Fe³⁺-catechol dynamic coordination crosslinking. The microphase formed within the PDMS matrix imparted static antifouling properties to the coatings. The mechanical properties of the damaged sample were restored at room temperature in an aqueous environment for 24 h, achieving a self-healing efficiency of almost 100%. The synthesized material exploited the dynamic coordination between Fe³⁺ and catechol to facilitate underwater self-healing. No bacterial adhesion was observed at the scratch site after the coating was repaired. This material enables the long-term antifouling and autonomous repair of marine vessels and sensors, thereby reducing maintenance costs.

The thioacetamide derivative (TD)-composite preservation system (TDCPS) exhibits superior preservation effects on natural rubber latex (NRL) and significantly enhances its vulcanization efficiency and mechanical properties. This study primarily investigated the principal chemical groups and mechanism of action of TDCPS in promoting NRL vulcanization through a comparative analysis. The results indicated that the key functional groups (thioamide and pyridine) in TDCPS synergistically accelerated crosslinking, reducing the vulcanization time by 41.18% compared to the high-ammonia (HA) preservation system. At an optimal TDCPS dosage of 5 mmol·L^–1, vulcanized films achieved a tensile strength of 34.18 MPa, with a sulfur content of 1.5 phr further improving the strength by 42.26%. TD outperformed the conventional accelerators 2-imidazolidinethione (ETU) and 3-hydroxypyridine (3-Hp) in promoting the crosslinking density and mechanical performance while eliminating ammonia-related environmental risks. This eco-friendly system demonstrates the industrial potential for sustainable rubber production.

The current work addresses the challenge of elucidating the performance of fluoroelastomers within the HMX (octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine) based polymer-bonded explosives (PBXs). To simulate the confined interface in PBXs, bilayer films of F2314/HMX and F2311/HMX were designed. Neutron reflectivity (NR), nanoindentation, and X-ray reflectivity (XRR) were employed to examine the layer thickness, interface characteristics, diffusion behavior, and surface morphology of the bilayers. NR measurements revealed interface thicknesses of 45 Å and 98 Å for F2314/HMX and F2311/HMX, respectively, indicating deeper penetration of F2311 into the HMX matrix. NR also suggested a denser polymer network with a higher scattering length density (SLD) near the HMX interface for both fluoroelastomers, while the bound layer of F2311 was notably thicker. Nanoindentation cross-checks and confirms the presence of a bound layer, highlighting the differences in stiffness and diffusion ability between the two polymers. The consistency between the NR and nanoindentation results suggests that F2311 demonstrates better flexibility and elasticity, whereas F2314 is stiffer and more plastic. Accordingly, the structures and performances of different fluoroelastomers at the HMX interface are discussed, which can provide valuable insights into the selection of binders for PBX formulations tailored to specific applications.

Machine learning (ML) has emerged as a powerful tool for predicting polymer properties, including glass transition temperature (T_g), which is a critical factor influencing polymer applications. In this study, a dataset of polymer structures and their T_g values were created and represented as adjacency matrices based on molecular graph theory. Four key structural descriptors, flexibility, side chain occupancy length, polarity, and hydrogen bonding capacity, were extracted and used as inputs for ML models: Extra Trees (ET), Random Forest (RF), Gaussian Process Regression (GPR), and Gradient Boosting (GB). Among these, ET and GPR achieved the highest predictive performance, with R² values of 0.97, and mean absolute errors (MAE) of approximately 7–7.5 K. The use of these extracted features significantly improved the prediction accuracy compared to previous studies. Feature importance analysis revealed that flexibility had the strongest influence on T_g, followed by side-chain occupancy length, hydrogen bonding, and polarity. This work demonstrates the potential of data-driven approaches in polymer science, providing a fast and reliable method for T_g prediction that does not require experimental inputs.

The deformation mechanism of glycerol plasticized poly(vinyl alcohol) (PVA) with different hydrolyses (88%, 92%, 98%) at elevated temperatures (60‒100 °C) was elucidated by in situ synchrotron radiation X-ray scattering. The vinyl acetate (VAc) in PVA acts as a non-crystalline chain defect, which significantly influences the plastic deformation and stretching-induced crystallization behavior of PVA. The key microstructural parameters of PVA during deformation, such as crystallinity (χ_c), lateral crystallite size (L), and long period (l), in combination with the stress-strain curves, were obtained. The experimental results show that the deformation process of the plasticized PVA film present a three-stage evolution: (i) a plastic deformation zone. The plastic deformation of the crystallite occurs as evidenced by the apparent decrease in crystallinity and lamellar reorientation induced by stretching; (ii) the stress softening zone. The decreasing trend of crystallinity becomes slow, and the long period becomes smaller, which indicates that PVA crystallization is induced by stretching; and (iii) the strain-hardening zone. There is a synergistic effect between the crystallite destruction and formation. Further research reveals that a high temperature and low degree of alcoholysis favor the stretching-induced crystallization of PVA, while the system with a high degree of alcoholysis shows significant characteristics of preferred crystal growth.

Multi-component polymer systems exhibit exceptional versatility and structural diversity, making them indispensable in the polymer industry as well as in advanced and high performance applications. However, constructing accurate phase diagrams for these systems remains challenging due to inhomogeneous structures arising from the introduction of block copolymer components. Here, we present a unified and model-agnostic framework for computing phase equilibria in multi-component polymeric systems based on the concept of “effective chemical potential”. This approach directly connects key thermodynamic variables in the canonical ensemble to other ensembles, unifying phase coexistence determination without requiring the reformulation of self-consistent field theory (SCFT) calculations across different ensembles. By decoupling phase equilibrium determination from specific ensemble formulations, our approach enables the reuse of existing SCFT solvers. Moreover, it provides a useful framework to develop highly efficient phase equilibrium solvers for multi-component polymer systems.

Understanding the mechanisms that influence the formation of stereocomplex crystals (SCs) in poly(lactic acid) (PLA) is critical for achieving effective regulation of SC content. In the current simulations, we constructed polymer blends with different initial chain conformations and then obtained four groups of polymer blend systems with similar segment miscibility but different chain extension degrees by controlling the high-temperature relaxation time. The simulation results indicate that the fraction of SCs formed in these systems is closely correlated with the average mixing parameters during the crystallization process rather than the initial chain extension degrees. In other words, the average segment miscibility in the crystallization process is the key factor controlling the formation ability of SCs.