Biobased Cyclic Enoate Monomers: Enabling Intrinsically Crystalline, Chemically Recyclable, Ultratough Polymers

Area of Science:

• Polymer Chemistry
• Materials Science
• Sustainable Chemistry

Background:

• Petroleum-based plastics pose significant environmental challenges due to poor recyclability.
• Designing circular polymers faces trade-offs between polymerizability, depolymerizability, performance, crystallinity, and ductility.

Purpose of the Study:

• To introduce a novel monomer design strategy for creating high-performance, chemically recyclable polymers.
• To overcome the inherent trade-offs in circular polymer design.

Main Methods:

• Utilized renewable cyclic enoates for monomer synthesis.
• Employed regioselective and stereoselective ring-opening metathesis polymerization (ROMP).
• Modulated ring-chain equilibrium to control polymerization and depolymerization.

Main Results:

• Achieved highly regioselective (head-to-tail) and stereoselective (E-selective) ROMP.
• Synthesized polyolefins/polyesters with high crystallinity and full chemical recyclability.
• Demonstrated near-quantitative conversion for both polymerization and depolymerization.

Conclusions:

• The developed strategy successfully defies traditional trade-offs in circular polymer design.
• These polymers exhibit an exceptional combination of intrinsic crystallinity, chemical recyclability, high thermal stability, mechanical strength, ductility, and toughness.
• This work provides a pathway for designing advanced sustainable polymers.