In recent years, the demand for renewable resource-derived polymers has surged, particularly for thermosetting materials. These crosslinked polymers, while offering superior mechanical and thermal properties due to their aromatic monomers, are typically non-recyclable and often rely on harmful chemical precursors. Addressing these challenges, our team has developed platforms of bio-based, non-toxic, and sustainable aromatic monomers derived from natural phenols such as tannins, lignin-based vanillin, eugenol, and cardanol. These monomers, functionalized with polymerizable groups like epoxy, highly reactive amines, cyclic carbonate leading to non-isocyanate polyurethanes, alcohol, isocyanate, and (meth)acrylate, have enabled the synthesis of diverse polymers tailored for various applications. Hence, we have proposed the replacement of bisphenol A by biobased vanillin in epoxy resins. Recently we have synthesized fully biobased polyurethanes and demonstrated upscaling to industrial scale . Additionally, we have explored cardanol-based additives to replace conventional plasticizers in PVC. Beyond synthesis, our efforts extend to the end-of-life stage, where we achieved chemical recycling of thermosetting biobased polyurethane foams and closed the recycling loop for epoxy composites, recovering bio-based monomers and fibers.

In the ongoing energy, materials and feedstock transition, the development of sustainable resins, polymers and coatings with high percentages of biobased content is a highly desirable goal. Our group has shown that biobased butenolides are promising monomers for the paints and coatings industry. The synthesis of this class of biobased monomers starts from the platform chemical furfural, which is derived from hemicellulosic biomass. Photo-oxidation of furfural with singlet oxygen affords hydroxy butenolide, with minimal waste in matter and energy. This efficient process can be performed both in batch and flow setups. Hydroxy butenolide can be further derivatized through its acetal moiety, for instance by condensation with a variety of (potentially bio-based) alcohols. These substituted butenolides can be co-polymerized with electron-rich vinyl co-monomers, such as vinyl ethers, vinyl esters and vinyl lactams, under solventborne conditions. Here, we show the first step towards aqueous poly-butenolide dispersions using high molecular weight polyurethanes as colloidal stabilizing moiety.

Aromatic synthetic molecules are widely employed for the production of rigid and thermally stable materials. In the green chemistry framework, the exploitation of green synthesis and polymerization techniques together with biomass polyphenols is growing [1].
The current work investigated the methacrylic grafting of gallic and tannic acids through microwave-assisted technology to achieve photocrosslinkable monomers [2,3]. The solvent-free and catalyst-free microwave-assisted technology ensured enhanced reaction rate (10 min at 130°C) with product yields of approximately 90%. To confirm the successful functionalization, the structures of methacrylated gallic acid (MGA) and tannic acid (MTA) were characterized by ¹H NMR and ³¹P NMR, respectively, and ATR-FTIR spectroscopies.
The radical UV-photopolymerization of MGA and MTA was deeply investigated by real-time FTIR, photo-DSC and photo-rheological analyses. High conversion degrees (89% for MGA and 80% for MTA) and low gel point values (5 s for MGA and 2.5 s for MTA) demonstrated the high photo-reactivity of both monomers. The UV-cured MGA and MTA exhibited a good thermal stability and high glass transition temperature (120-130°C), implying a significant crosslinking density.
The suitability of MGA for light-assisted 3D printing was proven. A honeycomb and a hollow cube were 3D printed with an outstanding accuracy in small scale [2]. Instead, MTA was demonstrated a promising anticorrosive coating on plasma pre-treated steel surface, as proved by the electrochemical impedance spectroscopy [3].
The exploitation of the reactivity of polyphenolic groups toward the UV-curable moieties incorporation via greener methods have proved a noteworthy potential to broader the innovative eco-friendly applications of natural polyphenols.

Microfibers are defined as fibers with a fineness of 1 dTex or less [1]. Their high surface-area-to-volume ratio enhances their functionality in applications requiring extensive interaction with the environment [2]. Therefore, they are mainly suited for uses such as thermoregulating clothing, filtration systems, medical devices as scaffolds for cell proliferation, and cleaning textiles [3].
Most commercial microfibers are bicomponent fibers made of poly(ethylene terephthalate) (PET) and polyamide 6.6 (PA 6.6), typically in a 80/20 ratio [4]. Bicomposition is a requirement of the process used to manufacture those fibers: by using a pie-wedge cross-section during bicomponent melt spinning, the filaments obtained can then be split into multiple finer fibers through an alkali treatment (involving caustic soda or NaOH) [4]. Overall, the main route for obtaining microfibers generates two environmental pressures as it involves additional chemical products, and results in bicomponent textiles that complexify their recycling.
To reduce these impacts, this study explores a new processing strategy that relies on the substitution of one polymer with a water-soluble counterpart. In this approach, water solubilization leads to split yet fully monocomponent fibers without requiring any chemicals. Several candidates have been evaluated based on their thermal and mechanical properties, solubility, and compatibility with PET, retained as the primary polymer due to its predominant presence in conventional microfibers. Once the optimal polymer was selected, process conditions were optimized to ensure proper spinning. The resulting filaments were characterized in terms of morphology, mechanics, and structure, validating the feasibility of this approach for sustainable microfiber production.