This research has developed a novel adhesion promoter using organic-inorganic hybrid nanoparticles (ATS) to address existing limitations, such as the cumbersome separate coating and drying stages and insufficient adhesion. ATS was synthesized through hydrolysis-condensation reactions of an alkoxysilane-functionalized amphiphilic polymer (AFAP) precursor and 3-aminopropyltriethoxysilane (APTES). When directly mixed with resin part of polyurethane, ATS significantly enhanced the adhesion strength of 2 K PU to steel substrates without altering the mechanical properties or chemical structure of the polyurethane. An optimization process was conducted to determine the ideal mixing ratio of ATS with other components of 2 K PU, including different types of glycols (butylene glycol, propylene glycol, and ethylene glycol) and polyols to achieve the highest adhesive performance. The results showed that 2 K PU resin formed by using a mixture of polycaprolactone diol (PCD) and butylene glycol (BG) containing ATS (1−2) with nanoscale size (30.86 nm) exhibited superior adhesion performance over the other modified 2 K PUs and was 2.16 times higher than the common 2 K PU. These results were further validated via predictive model following response surface methodology to assess the precise impact of three parameters: the amount of AFAP (X1), amount of APTES (X2), and amount of BG (X3) on the adhesion strength of 2 K PU. The properties of different types of ATS and modified 2 K PU including particle size, degree of condensation, moisture content, molecular structure, molecular weight, hydrogen bonding intensity, microstructure morphology, and adhesion strength, were characterized.
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