“Built to Last”: Plant-based Eco-friendly Durable Antibacterial Coatings

The demand for effective and long-term durable antibacterial surfaces has been ever-growing in the past decades. A wide variety of long-lasting antibacterial surfaces developed from release-killing, active-killing, and anti-fouling strategies have demonstrated the desired effectiveness and durability so far. Most of these successful designs were developed from toxic and fossil-based materials, which failed to comply with the green design criteria. Furthermore, the longevity of these surfaces remained an unaddressed challenge. Herein, we present a disruptive paradigm that emphasizes both eco-friendliness and long-lasting antibacterial properties. A bio-based active-killing essential oil, namely carvacrol, and nonfouling carboxybetaine zwitterionic moieties were combined and incorporated into a highly bio-based polyurethane (BPU). The long-lasting active-killing property for this antibacterial BPU coating was enabled through the extended release of the bounded carvacrol via hydrolysis in an aqueous environment and compared to unbound carvacrol by liquid infusion. Also, the release of carvacrol generates zwitterionic moieties to prevent further bacterial attachment at the release site, resulting in a "kill and defend" synergistic antibacterial function in the BPU. The kinetics of the extended-release property were investigated and compared with unbound carvacrol BPU coatings; unbound carvacrol infused into BPU was quickly exhausted after 2 days of immersion in water, while the extended-release surface exhibited a nearly constant release rate of ∼128 ng cm^-2 h^-1 even after 45 days. The in vitro antibacterial efficiency of the BPUs was quantitatively evaluated using the modified ISO standard for cross-laboratory comparison. As a result, approximately 98.9 and 98.7% of Escherichia coli and Staphylococcus aureus were eliminated from the coating surfaces, and only a negligible variance in the antibacterial efficiency was observed after 5 cycles of test. The feasibility for practical application was also demonstrated by challenging the BPU coatings in everyday settings. This "built-to-last" design theory provided insights for future development of greener antibacterial coatings with long-term performance.