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Rapidly Adaptive Aromatic–Aliphatic Polyester Networks Enabled by TBD-Catalyzed Bond Exchange
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DOI：10.1002/pola.70248.png)
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Abstract
En 中文
Aromatic–aliphatic polyester covalent adaptable networks (CANs) were synthesized from dimethyl terephthalate (DMT), 1,4-butanediol (BDO), and pentaerythritol (PER) by organocatalyst-assisted transesterification. Network structure tuning via systematically varying the ratio of difunctional and multifunctional monomers was possible, allowing us to establish a direct relationship between cross-link density and macroscopic properties. Rigid aromatic terephthalate moieties increase mechanical resistance and modulus, while flexible BDO moieties preserve the mechanical deformability of the polymer network. Increased cross-linking, as confirmed by dynamic mechanical analysis, is reflected in the storage modulus and effective cross-link density (νe = 2.5 × 103 mol/m3). Analysis of stress relaxation demonstrates bond exchange at elevated temperature, characteristic of CANs, with an activation energy of about 86 kJ/mol. Significantly higher reactivity of TBD promotes bond-exchange reactions in CANs, providing opportunities for thermal reprocessing and welding, as well as self-healing (UTS: ≥ 95%), which are not observed in catalyst-free controls with inferior mechanical properties and dynamic behavior. High thermal stability (~200°C) enables easy, safe processing and healing of the material below its degradation temperature.
Keywords:
elastomers
network topology
organic polymer
reprocessable thermosets
self-healable materials
sustainable polymer
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