Biobased poly(amido-imide) CANs catalyzed by lanthanide triflates: High creep resistance and superior reprocessability

Abstract

Here, we report the preparation of a series of dynamic covalent poly(amido-imide) materials where the network architecture and the addition of external catalysts were carefully selected through an in-depth study to fine-tune the thermomechanical properties of the final materials and maximize their possible applicability.

The use of bioderived tricarballylic acid in combination with different proportions of commercially available amines enabled tailoring the thermal and mechanical properties of the final materials. This approach allowed to obtain materials with T_gs ranging from 90 °C to 130 °C, high thermal stability (T_1% > 248 °C) and robust mechanical properties at room temperature (σ_break > 85 MPa, Young Modulus > 3.1 GPa). Moreover, the addition of lanthanide triflates significantly enhanced the dynamicity of the networks by almost one order of magnitude, while still maintaining excellent structural integrity and high creep resistance at service temperatures. This achievement represents a significant step towards highly crosslinked materials with fast reprocessing capabilities and good thermomechanical performance.

The materials also showcased excellent self-welding and shape-memory capabilities, highlighting their versatility, which we envision will open up new advancements in the field of reprocessable thermosetting materials.