Coupling of Supramolecular Chemistry with Dynamic Covalent Chemistry for Circular Polymers

• • Catalyst-free, solvent-free depolymerization: The semicrystalline poly(disulfide) reverts to monomeric crystals at 120 °C for 24 h with >90% purity and quantitative yield, eliminating the need for harsh conditions or catalysts, thus reducing energy consumption and waste. • • Exceptional mechanical performance: Sc-poly(TAA) exhibits a Young's modulus of 3.9 GPa, comparable to Nylon 6, and maintains its modulus and crystallinity after aging at 80% relative humidity for six days, indicating superior durability for structural applications. • • Ultra-long relaxation time: Rheological and creep analyses show a network relaxation time exceeding 90 years at room temperature, demonstrating exceptional dimensional stability and resistance to creep, critical for long-term load-bearing applications. • • Low carbon footprint: Life-cycle assessment reveals a carbon footprint of only 0.36 kg CO2 per kg product for the solid-state recycling process, significantly lower than conventional recycling methods, offering a sustainable pathway for plastic circularity.