High-performance chemically recyclable multifunctional polyolefin-like biomass-derived polyester materials

Polyolefins are the most widely used and produced petroleum-based plastics. Unfortunately, the enormous production and usage of traditional polyolefins, coupled with the lack of effective disposal or recycling options, have led to significant fossil fuel depletion and severe environmental pollution. To foster sustainable societal development, there is an urgent need to design high-performance and inherently recyclable polyolefin-like bio-derived materials by innovative structural and molecular designs. Here, inspired by a copolymerization molecular design approach that simultaneously confers recyclability and superior properties to materials, high-performance recyclable polyolefin-like bio-derived polyesters (PBC_<i>x</i>S) enabled by a novel judicious combination of building blocks are reported. PBC_<i>x</i>S display excellent mechanical (40.6 MPa, 498.4%) and gas barrier properties (O₂ 0.09 barrer, H₂O 1.70 × 10^-13 g cm cm^-2 s^-1 Pa^-1), even greater than those of bio-based materials and most aliphatic polyester. Meanwhile, PBC_<i>x</i>S also exhibit multifunctionality with excellent biocompatibility properties and ultra-high processability (thermoforming, extrusion spinning, and 3D printing processing). Notably, PBC_<i>x</i>S undergo depolymerization in the absence of any additional organic solvents, regenerating 92.0% of the high-purity (98.3%) original monomers, even with polyolefin blend plastics. Repolymerized polyesters still maintain their exceptional mechanical and thermal qualities. The successful application of this approach in polyesters opens up exciting possibilities for designing high-performance and recyclable bio-derived polyolefin-like materials.