The European Green Deal aims to transform the European economy into a sustainable, climate-neutral, and circular economy by 2050, driving research in polymer science. Beyond substituting fossil raw materials with biobased ones to reduce polymer material carbon footprints, attention shifts to thermoset circularity. Covalent adaptable networks (CANs) mark a vital development, incorporating reversible chemical bonds to merge the rapid processing advantages of thermoplastics with the durability and resistance inherent to thermosets. This study focuses on the development of sustainable CANs utilizing biomass-derived components, more specific lignin as the hard segment and a biobased diamine functionalized polymer as the soft segment. Associative vinylogous urethane CANs will be discussed with a lignin content up to 50%. Mechanical properties are tailored by adjusting the ratio of modified lignin to diamine, influencing the cross-linked network’s density. At temperatures above 100 °C, vinylogous urethane amine exchange reactions are activated, enabling recyclability without the need for additional catalysts. Rheology was used to study time- and temperature-dependent stress relaxation dynamics. A breakthrough was achieved since by the right structural modifications in the network, creep-free vinylogous urethane networks could be achieved. Furthermore, the study highlights the potential to use those CANs for the development of adhesives with superior adhesion properties, thermal repairability and on-demand removability, both thermally and with solvents.
This sustainable approach addresses challenges in recycling thermosets, emphasizing the significance of biomass-derived materials for eco-friendly and recyclable polymer systems.
References:Liu, J.; Pich, A.; Bernaerts, K. V., Preparation of lignin-based vinylogous urethane vitrimer materials and their potential use as on-demand removable adhesives. Green Chemistry 2024, 26, 1414-1429