Sustainable and Scalable Polyphenolic Bioadhesives for Hemostasis and Surface Functionalization

Abstract

Adhesive polyphenolic materials, inspired by mussel underwater adhesion, are promising candidates for versatile medical and industrial adhesives. Yet, most synthetic routes remain chemically intensive, energy-demanding, and poorly suited to sustainability and industrial-scale productivity. Conventional EDC/NHS carbodiimide coupling tethering polyphenolic moieties to polymer backbones require costly reagents, multi-step purifications, and extensive dialysis, waste, and scale-up inefficiency. Here, we introduce rapid, simple, coupling agent-free synthetic approach to produce adhesive polyphenolic conjugates entirely from renewable resources. Specifically, chitosan-1,2,4-benzenetriol (CHI-B) conjugates were synthesized via spontaneous conjugation between fructose-derived biomass, 1,2,4-benzenetriol (BTO), and crustacean-derived chitosan without heating or carbodiimide coupling agents, achieving rapid reaction within 30 minutes at scales reaching tens of liters in a laboratory setting. CHI-B effectively functionalizes challenging substrates such as PTFE and glass, transforming them into large-area superhydrophilic surfaces. Furthermore, CHI-B demonstrated potent hemostatic efficacy in a mouse liver bleeding model, highlighting its potential for biomedical and sustainable industrial applications.