Closed-loop recyclability of a biomass-derived epoxy-amine thermoset by methanolysis

Closed-loop recyclability of a biomass-derived epoxy-amine thermoset by methanolysis

2024 | Xianyuan Wu, Peter Hartmann, Dimitri Berne, Mario de Bruyn, Florian Cuminet, Zhiwen Wang, Johannes Matthias Zechner, Adrian Daniel Boese, Vincent Placet, Sylvain Caillol, et al.
A biomass-derived epoxy-amine thermoset (DGF/MBCA) was synthesized and demonstrated to be recyclable through methanolysis. The thermoset, made from dimethyl ester of 2,5-furandicarboxylic acid (DMFD), 4,4'-methylenebis(cyclohexylamine) (MBCA), and glycidol, exhibits excellent thermal and mechanical properties (Tg = 170°C, E'25°C = 1.2 GPa). It undergoes methanolysis without a catalyst, regenerating 90% of the original DMFD. Subsequently, the diamine MBCA and glycerol can be reformed via acetolysis, enabling closed-loop recycling. The material can be used in glass and wood fiber composites, demonstrating its potential for sustainable applications. The study highlights the development of inherently recyclable thermosets from renewable resources, addressing environmental concerns associated with traditional thermosets. The low-temperature methanolysis process allows for the recovery of all original building blocks, making the material suitable for circular economy applications. The thermoset's performance is comparable to commercial, fossil-based thermosets, and its stability in various solvents and under hydrolysis conditions further supports its potential for use in coatings, biomedical devices, and sustainable transportation. The research provides a sustainable solution for the recycling of thermosets, contributing to the development of a circular and bio-based economy.A biomass-derived epoxy-amine thermoset (DGF/MBCA) was synthesized and demonstrated to be recyclable through methanolysis. The thermoset, made from dimethyl ester of 2,5-furandicarboxylic acid (DMFD), 4,4'-methylenebis(cyclohexylamine) (MBCA), and glycidol, exhibits excellent thermal and mechanical properties (Tg = 170°C, E'25°C = 1.2 GPa). It undergoes methanolysis without a catalyst, regenerating 90% of the original DMFD. Subsequently, the diamine MBCA and glycerol can be reformed via acetolysis, enabling closed-loop recycling. The material can be used in glass and wood fiber composites, demonstrating its potential for sustainable applications. The study highlights the development of inherently recyclable thermosets from renewable resources, addressing environmental concerns associated with traditional thermosets. The low-temperature methanolysis process allows for the recovery of all original building blocks, making the material suitable for circular economy applications. The thermoset's performance is comparable to commercial, fossil-based thermosets, and its stability in various solvents and under hydrolysis conditions further supports its potential for use in coatings, biomedical devices, and sustainable transportation. The research provides a sustainable solution for the recycling of thermosets, contributing to the development of a circular and bio-based economy.
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