Interfacial adhesion of <i>in silico</i> developed functionalized linseed oil based green pressure-sensitive adhesives

The rising demand for sustainable pressure-sensitive adhesives (PSAs) in healthcare and food packaging necessitates a deeper understanding of their interfacial adhesion mechanisms. This study employs molecular dynamics (MD) simulations to investigate the adhesion behavior of low-<i>T_g</i> acrylated epoxidized linseed oil (AELO) and acrylated epoxidized methyl ester (AEME) PSAs on a corneocyte lipid envelope (CLE) and polypropylene (PP), which are representative of human skin and packaging substrates, respectively. Model validation was achieved through the accurate prediction of bulk properties (density, solubility parameter, and <i>T_g</i>) and the surface energies of CLE and PP. The AELO-based PSA exhibited superior adhesion, which was driven predominantly by van der Waals interactions. These forces facilitated significant molecular rearrangement, enhancing acrylate and hydroxyl group mobility toward the interfaces over time. The work underscores the potential of AELO and AEME as bio-based PSA monomers, offering a renewable alternative for high-performance adhesion in biomedical and packaging applications.