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Abstract A depolymerizable vitrimer that allows both reprocessability and monomer recovery by a simple and scalable one‐pot two‐step synthesis of vitrimers from cyclic lactones is reported. Biobased
δ ‐valerolactone with alkyl substituents (δ ‐lactone) has low ceiling temperature; thus, their ring‐opening‐polymerized aliphatic polyesters are capable of depolymerizing back to monomers. In this work, the amorphous poly(δ ‐lactone) is solidified into an elastomer (i.e.,δ ‐lactone vitrimer) by a vinyl ether cross‐linker with dynamic acetal linkages, giving the merits of reprocessing and healing. Thermolysis of the bulkδ ‐lactone vitrimer at 200 °C can recover 85–90 wt% of the material, allowing reuse without losing value and achieving a successful closed‐loop life cycle. It further demonstrates that the new vitrimer has excellent properties, with the potential to serve as a biobased and sustainable replacement of conventional soft elastomers for various applications such as lenses, mold materials, soft robots, and microfluidic devices.
