Abstract

In this work, a solvent-free, photocurable vitrimer based on dynamic imine bonds and functionalized silica nanoparticles was developed. The resulting materials exhibit good dispersion, strong adhesion to steel, enhanced scratch resistance, and rapid self-healing (within 5 minutes at 80 °C). They also provide excellent corrosion protection and can be fully removed and recycled via transimination reactions. Three systems were investigated: a pristine vitrimer without silica nanoparticles; a vitrimer containing 2 wt% functionalized silica nanoparticles (2% w/w SB-NPs); and a vitrimer containing 5 wt% functionalized silica nanoparticles (5% w/w SB-NPs). The silica nanoparticles (NPs) were functionalized through a two-step process. First, SiNPs were treated with 3-(aminopropyl)-triethoxysilane (APTES) to introduce amine functionalities, yielding NH₂-NPs. In the second step, a Schiff base reaction with methacrylated vanillin was carried out, producing the final functionalized nanoparticles (SB-NPs). The dataset includes the following characterization data: Attenuated Total Reflectance - Fourier Transform Infrared (ATR-FTIR) spectroscopy: to confirm the chemical structure of the samples Thermogravimetric analysis (TGA): to characterize the nanoparticles after each functionalization step and to evaluate the thermal stability of the three systems Differential scanning calorimetry (DSC): to assess the thermal transitions of the samples Dynamic mechanical analysis (DMA): to investigate the stress-relaxation behavior of the three systems. Atomic force microscopy (AFM): to analyze morphology and surface roughness of the systems in the presence of nanoparticles, as well as the effect of curing. Scanning electron microscopy (SEM): to examine the morphology of the three systems and the dispersion of the nanoparticles. Mechanical testing: to evaluate the adhesion of the systems when applied as coatings on metal substrates. Corrosion tests data: to assess the corrosion resistance properties of the three systems applied as coatings on metal substrates, as well as the recovery of the corrosion properties after the closure of a previously introduced scratch. This comprehensive dataset supports the findings presented in the manuscript and provides detailed insights into the design, characterization, and recyclability of the proposed systems