Strong and tough bio-based biomimetic-multiphase composite polyesters with superior barrier and chemically closed-loop performances

Abstract

Development of bio-based polyester packaging materials that adheres to the principles of green chemistry demands the simultaneous achievement of high performance and facile recycling performance but remains challenging. In this work, we fabricated a novel mica single-sheet (MSS)-modified furan-based biomimetic composite polyester (denoted as BCP), achieving strong, tough, and high-barrier films that exhibit a unique nature of aromatic ring and multi-phase architectures. BCP showed many beneficial structural characteristics: heterogeneous-induced nucleation and crystallization, multi-scale energy dissipation, strain-induced alignment and orientation, and multi-effect physical barrier effects. Benefitting from these features, the resultant BCP films showed a superior integration of high tensile strength (about 76 MPa), toughness (about 397%), and exceptional gas barrier properties (O₂ 0.0183 barrer, CO₂ 0.0244 barrer, and H₂O 1.49 × 10^–14 g cm cm⁻² s⁻¹ Pa⁻¹), which are greater than those of most engineering plastics. More importantly, BCP also displayed impressive UV-shielding properties, solvent resistance, and easy physical and chemical recycling performance. Hence, the current work presents novel insights for the design and fabrication of strong, tough, high-barrier, and sustainable bio-based polyester materials that comply with the principles of green chemistry.