Mechanically robust and recyclable CO2-derived poly(carbonate) vitrimers: The role of crosslinking density in mechanical and rheological properties

Abstract

Effective CO2 fixation into valuable products has become a top priority in addressing global warming. Herein, we designed CO2-derived vitrimers with mechanically robust and recyclable through chemical and physical methods. We fabricated poly(carbonate) vitrimers (PCVs) capable of storing 6.6 mmol center dot g(-1) of CO2, by synthesizing CO2-derived poly(1,2-glycerol carbonate) and a bis(6-membered cyclic carbonate) (BCC) crosslinker. The mechanical properties were tunable by varying the crosslinking density, yielding PCVs with elastic moduli ranging from 335 to 1,360 MPa and elongations at break from 3.9 to 29%, comparable to industrial polymers. Dynamic analysis demonstrated the influence of crosslinking density on mechanical and rheological properties. Furthermore, the PCVs exhibited recyclability through both physical and chemical methods. Fragmented PCVs were physically recycled into films using hot pressure, while end-of-life PCVs could be chemically degraded into monomers for the re-synthesis into new PCVs. In addition, PCVs demonstrated shape memory properties, where deformed structures could be temporarily fixed and subsequently recovered upon heating above their glass transition temperature. This characteristic, combined with their recyclability and tunable mechanical performance, highlights the potential of PCVs as sustainable CO2-derived materials for advanced polymer applications. CO2-derived PCVs show significant potential for sustainable CO2 utilization and closed-loop polymer lifecycles, offering a promising solution for developing next-generation recyclable polymer materials.