Replacing petroleum-derived monomers with bio-based alternatives offers a promising route to reducing the environmental footprint of plastics. However, only a few polymeric materials designed in this way can selectively recover valuable petroleum-derived segments. Herein, we report a novel strategy to construct petroleum/bio-based hybrid plastics with high tensile strength and chemical recyclability, by cross-linking thioctic acid and aromatic petroleum-derived epoxy monomers through dynamic imine, disulfide, and hydrogen bonds, denoted as TAE. Benefiting from the reversibly cross-linked network, TAE exhibits excellent mechanical properties (Young's modulus of ∼2.52GPa, tensile strength of ∼82.1MPa) and remarkable water stability. TAE was further combined with carbon fibers (CFs) to produce CF-TAE composites with outstanding mechanical performance comparable to commercial CF-epoxy thermoset composites. The dynamic imine bonds can be broken by immersing the TAE plastic sheets in a mixed solvent of a polar organic solvent and acidic solution, enabling the non-destructive recovery of CFs and the petroleum-derived monomer. Meanwhile, the residual bio-based components can be safely discarded without environmental concerns. This work addresses critical challenges in the design of sustainable polymeric materials, providing a promising strategy toward next-generation recyclable plastics and fiber-reinforced composites.

Polymer composites possessing high dielectric permittivity (ε), low dielectric loss (tanδ) and outstanding breakdown strength (Eb) hold vast application potential in electronic devices and electrical equipment. To achieve synergistic enhancement of ε and Eb in CCTO (copper calcium titanate)/PVDF (polyvinylidene fluoride), raw CCTO particles were coated with SiO2 (silica) and PDA (polydopamine), respectively, and the modified CCTO were blended with PVDF to probe the double-shell' effect on the morphology and dielectric performances of the composites. The results reveal that the CCTO@SiO2@PDA/PVDF achieves improved ε and Eb alongside reduced tanδ compared with CCTO/PVDF composites. The enhanced ε originates from the constructed double-shell that facilitates intra-particle polarization while limiting inter-particle polarization, and creates deep traps to restrain tanδ and conductivity. This double-shell is capable of reinforcing interfacial bonding between CCTO and PVDF while mitigating interfacial dielectric mismatch. Local electric field distortion gets weakened and electrical tree growth becomes suppressed accordingly, which finally boosts the Eb. Theoretical calculations and simulations disclose the multiple polarization mechanisms and modified charge transport behaviors within the CCTO@SiO2@PDA/PVDF. This work puts forward a strategy to fabricate polymer composites with high Eb and ε, low tanδ, displaying extensive applications in pulse power devices and electrical insulating fields.

The sodium salt of resorufin (RSF), an inexpensive, water-soluble, commercially available phenoxazinone dye, serves as an efficient photocatalyst for low-copper dual-catalysis PhotoATRP across the visible spectrum. RSF loadings as low as 1ppm catalyzed PhotoATRP of acrylates in the presence of CuBr2/Me6TREN, yielding polymers with low dispersities (Đ∼ 1.07) and high initiation efficiencies. Control was maintained under blue, green, orange, and red irradiation. The living character of the system was confirmed by linear first-order kinetics, light-on/off temporal control, chain extension, and molecular weights that tracked targeted degrees of polymerization up to 1200. The system was also effective for the ATRP of oligo(ethylene oxide) methacrylate (OEOMA500) in aqueous media using CuBr2/TPMA and was tolerant to residual oxygen. Fluorescence-quenching experiments identified oxidative quenching as the predominant pathway for photocatalytic activator (re)generation.

Cellulose-based adhesives offer sustainable alternatives to petroleum-derived products but face bottlenecks regarding organic solvent reliance, slow curing efficiency, and moisture sensitivity. Here, a solvent-free, UV-curable cellulosic adhesive (UCA) is developed via a supramolecular-covalent hybrid strategy. Utilizing a cellulose acetate butyrate/thymol eutectic platform, multi-component functionalization with silane, photoactive acrylic moieties, and fluorinated monomer yields a transparent, photocurable prepolymer. The cured UCA exhibits a lap-shear strength of 6.73MPa on PMMA, high optical transparency, and broad temperature tolerance. Synergistic surface hydrophobicity, interfacial coupling, and dense photocrosslinking impart strong water resistance, retaining 5.86MPa shear strength after 3-day water immersion and 5.12MPa after 1h in 100°C boiling water. The adhesive also withstands strong acids, bases, and organic solvents. This work provides a practical route for engineering high-performance bio-based adhesives.

Mechanical property characterization of supramolecular viscoelastic materials, particularly low-molecular-weight gelator (LMWG)-derived hydrogels, has predominantly relied on small-amplitude oscillatory shear (SAOS) measurements, although these experiments probe network dynamics only at short timescales and fail to capture the full spectrum of network rearrangements that drive bulk mechanical behavior. A key challenge is unveiling how transient non-covalent interactions in LMWGs and covalent polymeric components collectively modulate viscoelasticity across multiple timescales. Herein, we investigate an LMWG-polymer hybrid hydrogel to demonstrate how the progressive integration of a covalent polymer into a self-assembled network regulates the bulk mechanical response, using short-timescale SAOS and long-timescale stress-relaxation and creep/creep-recovery experiments. Notably, frequency-sweep and stress-relaxation measurements reveal that the storage modulus and characteristic relaxation time exhibit distinct sensitivities to polymer concentration, with comparable stiffnesses occurring alongside noticeably different relaxation times in the intermediate polymer composition range. Creep/Creep-recovery measurements further show enhanced resistance to irreversible deformation and improved elastic recovery at low polymer loadings, whereas higher polymer concentrations primarily promote faster recovery dynamics through a transition from dual to single retardation behavior. These findings demonstrate that polymer incorporation can differentially modulate the stiffness and relaxation dynamics of LMWG-derived supramolecular networks, providing a framework for tuning viscoelastic behavior across multiple timescales.

In chemically driven soft materials, polymer architecture can shape how chemical reactions are transduced into material-level dynamic behavior. However, the relationship between polymer architecture and the resulting dynamics remains insufficiently understood. Here, using Arrhenius analysis, we perform a cross-hierarchical comparison of the temperature dependence of Belousov-Zhabotinsky (BZ) reaction-driven oscillatory dynamics across three structurally related systems: molecular Ru(bpy)3Cl2, a linear self-oscillating polymer (SOP), and a self-oscillating microgel (SOMG). In these systems, Ru(bpy)3 complex is present in solution as a molecular catalyst or covalently incorporated into either a linear polymer or a crosslinked microgel network. The resulting apparent activation energies Ea, app are used to quantify the overall temperature dependence of their oscillatory dynamics. In the SOP, the redox and coacervation/dissolution oscillations exhibit similar Ea, app values, indicating that periodic liquid-liquid phase separation had only a limited effect on the overall temperature dependence. In contrast, in the SOMG, the flocculation/dispersion oscillation exhibits a substantially higher Ea, app than the redox oscillation. Moreover, the relative order of Ea, app between the SOP and SOMG is reversed between the redox and structural oscillatory modes. These results indicate that Ea, app is modulated by both the underlying polymer architecture and the architecture-dependent structural dynamics accompanying BZ-driven oscillations.

The cover illustrates how shear, nanoscale confinement, and homoepitaxial templating compete to direct crystallization in poly(ethylene oxide) thin films. Pseudo-polyrotaxane nanosheets selectively promote flat-on lamellae through matrix-filler interactions, whereas shear favors edge-on ordering and strong confinement drives reorientation. This mechanistic framework enables predictable control of crystalline orientation for advanced thin-film technologies. More details can be found in the Research Article by Kohzo Ito and co-workers (DOI: 10.1002/marc.70367).