Abstract :
[en] Today, adhesive bonding is a widespread technology many fields including automotive,
aeronautic, surgery, packaging, electronic devices or in the building sector. It enables designing novel (lightweight) materials/products with performances comparable to the ones of systems fixed by mechanical adhesion. Glues, adhesives exist as a large variety of compositions such as cyanoacrylates (superglue ®), (meth)acrylate or epoxy resins, polyesters, polyurethanes… that fit on-demand to the specificity of the glued assembly (nature of the substrate, the thermo- mechanical performances, the resistance against water, acids, bases or solvents…). Due to their easy tunable and versatile properties (soft and flexible to rigid materials, high bonding adhesion, compatibility with numerous substrates…) polyurethanes (PUs) are reference systems. PUs are produced from toxic isocyanates that cause severe health concerns (asthma, skin irritation, DNA mutation). To surpass these issues, the quest for novel isocyanate-free PUs glues and adhesives formulations is essential. This thesis responds to this current trend which aims to develop well-designed innovative sustainable PU adhesives (and coatings) free of isocyanates. It explores the potential of poly(hydroxyurethane)s (PHU) made by step-growth polymerization of CO2-sourced bis- or multi-functional cyclic carbonates with di- or polyamines to construct novel PU glues/adhesives for various substrates (metals, wood, glass, plastics). Three main research axes were investigated and focused i) on the establishment of solvent-free petro-based PHU formulations and their corresponding nanocomposites thermoset PHUs (native or functional silica or ZnO fillers) to tailor high performance adhesives for various substrates; ii) on the increase of the sustainability of the PHU nanocomposites glues by incorporation of renewable monomers (vegetable oils) within the formulations and iii) the development of biomimetic PHU glues inspired from mussels (incorporation of dopamine). All formulations were benchmarked with commercial Terpmix-6700 and Araldite®2000 PU glues and results highlight that these PHU glues represent promising and competitive alternatives to conventional PU glues prepared from the toxic isocyanate chemistry. We believe that this work opens a realistic route to the next generation of PU adhesives.
