Roxana Dinu

This paper evaluates the environmental sustainability of a carbon fibre reinforced composite panel manufactured using a bio-based, recyclable and reprocessable epoxy resin synthetized from phloroglucinol, compared to one produced with traditional epoxy, through life cycle assessment. Results show a 2.42% reduction in global warming potential and an 80.7% decrease in freshwater eutrophication, enabled by bioremediation from brown algae cultivation, the source of phloroglucinol. However, increases of 1.67% and 9.76% in human toxicity for carcinogenic and non-carcinogenic categories, respectively, were observed due to solvent use at laboratory scale, which still requires optimization. The findings highlight the potential of bio-refinery processes for carbon-neutral composites, identifying key challenges for future development and scale-up.

The non-toxic and biodegradable nature of chitosan makes it a valuable resource offering promising opportunities in the development of bio-based materials with enhanced mechanical and thermal properties. In this work, the combination of epoxidized linseed oil, oxalic or citric acids, and chitosan (CHI) as a curing accelerator presents an attractive strategy to create bio-based and sustainable thermosetting materials. This article aims to provide a comprehensive exploration of the systems reactivities, characteristics, and performance evaluation of the designed bio-thermosets. Both the nature of the two carboxylic acids and the presence of chitosan are shown to have a big impact on the thermomechanical properties of the developed networks. While oxalic acid favours the formation of elastic networks, with low T_g values (increasing with CHI content between 0.7 and 8.5 °C) and relatively low Young’s modulus (~2.5 MPa), citric acid promotes the formation of very dense networks with lower mass of the segments between the crosslinks, having 20 times higher T_g values (from 36 to 45 °C) and ~161 times higher Young’s modulus (from 94 MPa up to 404 MPa in these systems). The CHI has a strong impact on the curing reaction and on the overall properties, by increasing the materials’ performance.

There is an imperative need to find sustainable ways to produce bisphenol A free, high performance thermosets for specific applications such as the space or aerospace areas. In this study, an aromatic tris epoxide, the tris(4-hydroxyphenyl)methane triglycidyl ether (THPMTGE), was selected to generate high crosslinked networks by its copolymerization with anhydrides. Indeed, the prepared thermosets show a gel content (GC) ~99.9% and glass transition values ranged between 167–196 °C. The thermo-mechanical properties examined by DMA analyses reveal the development of very hard materials with E′ ~3–3.5 GPa. The thermosets’ rigidity was confirmed by Young’s moduli values which ranged between 1.25–1.31 GPa, an elongation at break of about 4–5%, and a tensile stress of ~35–45 MPa. The TGA analyses highlight a very good thermal stability, superior to 340 °C. The Limit Oxygen Index (LOI) parameter was also evaluated, showing the development of new materials with good flame retardancy properties.

A bio-based polymeric matrix was developed by the copolymerization of a vegetable oil-based epoxy, epoxidized linseed oil (ELO), with dodecenyl succinic anhydride (DDSA). To obtain eco-friendly bio-composites, this matrix was combined with a natural filler: spruce bark powder (SB) with its hydrochar (HC) in various proportions ranged from 1 to 30 wt.%. The reactivities of these formulations were studied by DSC analysis that highlighted that both fillers have a high catalytic effect on the ELO–DDSA crosslinking reaction. The complementary studies by TGA, DMA, tensile tests, water absorption and Shore tests had shown that both HC and SB bring improvements to the mechanical properties of the composites, fulfilling multiple roles: (i) Both act as co-reactants in the copolymerization mechanism; (ii) HC acts as reinforcement, consolidating the network and providing stiffness and rigidity; and (iii) SB acts as plasticizer for reducing the brittle character of the epoxy resins.