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Organically modified sol-gel coatings have been investigated as potential replacements for chromate conversion coating of AA1050 and AA2024 aluminium alloys. The coatings were prepared by a combination of a completely hydrolysable precursor of tetra-n-propoxyzirconium (TPOZ), with a partially hydrolysable precursor of glycidoxypropyltrimethoxysilane (GPTMS). GPTMS contains organic functional groups, which are retained in the sol-gel coatings after the hydrolysis-condensation process. Different process parameters, e.g. GPTMS/TPOZ ratios, withdrawal speeds, solvent water concentrations, and curing temperatures were studied. Coatings produced using a low GPTMS/TPOZ ratio and a high withdrawal speed generated significant cracks due to the shrinkage of the coatings. It was found that increase of organic moieties reduced the shrinkage of the coatings and the tendency for crack formation. By controlling process parameters and ratios of organic and inorganic moieties, crack-free sol-gel coatings from 0.1 μm to 9 μm thick can be achieved. The sol-gel coatings formed are amorphous and contain organic epoxy-ether retained silicon oxide, silicon hydroxide, zirconium oxide, zirconium hydroxide, and zirconium acetate. The Si/Zr ratios of resultant sol-gel coatings are proportional to the initial GPTMS/TPOZ ratio. Cerium oxide nanoparticles were successfully incorporated into sol-gel coatings with a single layer and double layer sol-gel process. Through the dip coating process, crack-free sol-gel coatings, of varied thickness, were developed on different aluminium substrate, including electropolished superpure aluminium, magnetron sputtered aluminium with varied copper contents from 0 to 30 wt.%, and commercial AA1050 and 2024 aluminium alloys. Sol-gel coatings formed on commercial AA1050 and 2024 aluminium alloys revealed a significant passivation in 3.5 wt.% sodium chloride solution during anodic polarisation when the sol-gel coating is more than 1 µm thick and proper surface pretreatments of the alloys were used. Corrosion tests by immersion in 3.5 wt% sodium chloride solution and by salt spray in 5 wt.% sodium chloride solution revealed that sol-gel coatings successfully protected AA2024 aluminium alloy against the aggressive environment and have the potential to replace chromate containing coating systems.

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En general, un material tenderá a corroerse espontáneamente en un determinado medio si los productos de corrosión son más estables que el material de partida, o si bajo las condiciones de exposición la corrosión resulta favorecida. En la práctica, lo que se busca es extender la vida útil de estructuras, equipos o dispositivos, es decir, mejorar su durabilidad. / In general, a material will tend to corrode in a specific environment when the corrosion products are more stable than the starting material or, when exposed to certain conditions, a corrosion process results favored. In general practice, the goal is to extend the service life of structures, equipment or devices, that is, to improve their durability.

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The thesis aims to illustrate and highlight the potential of graphene-based fillers in reinforcing organic coatings deposited by cataphoresis. Thanks to particular surface modification processes of the graphene flakes, these have been properly distributed within the polymer matrix, providing the composite coating with remarkable protective performance. The optimization of the deposition process parameters, as well as the amount of filler, also allowed to improve the mechanical and conductivity properties of the cataphoretic matrix, suggesting the possibility of realizing multifunctional coatings. Finally, these ’smart’ coatings were made by combining two deposition techniques, creating two layers with distinct purposes, containing different types of graphene-based fillers. The cataphoretic primer provided the substrate with high corrosion protection, while the spray top coat possessed high properties of electrical conductivity and resistance to abrasion phenomena. Ultimately, graphene has proven to be an excellent resource as a reinforcing filler in multifunctional organic coatings.