Biomacromolecules, 2025, 26 (4), 2720-2732.

Developing new biodegradable polyesters with well-defined structures is of interest. We reported an attractive two-component aliphatic polyester-based thermoset, which was prepared via the esterification of biomass-derived L-malic acid (LMA) oligomers and three-arm poly(ε-caprolactone) (3a-PCL) triols. Chemical network formed via the ester bonding and physical network caused by the crystallization of 3a-PCL arm chain coexist in the thermoset, and the competition of the two characteristic networks leads to a negative correlation between the degree of covalent crosslinking and the degree of crystallization, thereby the mechanical state of the thermosets can be easily tuned: from plastic to elastomer state. Moreover, the crystallization temperature and melting point of the thermosets range in 30 oC~50 oC and -7 oC~18 oC, respectively, which are favorable of shape morphing as the thermosets are used as shape memory materials. This work also provides valuable information on tailoring the mechanical and thermal properties of star-shaped polyester-based thermosets.

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