Design of tough, strong and recyclable plant protein-based adhesive via dynamic covalent crosslinking chemistry

Abstract

Conventional covalent crosslinked protein adhesives are brittle and cannot be reprocessed effectively, which restricts their practical application and limits the recyclability of wood-based panels. Inspired by biological cartilage and mussels, a tough, strong, and recyclable soybean protein isolate (SPI)-based adhesive, SPI/BP@mica, was designed in this study by co-assembly of mica and SPI via dynamic boron-nitrogen (B-N) coordinated catechol-derived boronic ester (B-O) interfacial bonding. The dynamic covalent B-O, imine, and hydrogen bonds significantly improve the cohesive strength and energy dissipation capacity of SPI/BP@mica adhesive for high mechanical strength and toughness. The maximum wet shear strength and adhesion of SPI/BP@mica adhesive bonded plywood reach 1.05 MPa and 518.8 MJ, respectively, at increases of 94.4 % and 601.2 % over the original SPI adhesive. More importantly, we achieved a breakthrough in the recyclability of protein-based wood adhesives. Due to the synergistic triple dynamic mechanism and B-N coordination depolymerization of B-O bonds, second-generation particleboard prepared by recycling via hot-pressing and solvent-assisted repolymerization showed a rupture modulus of 12.1 MPa; to this effect, we fabricated a next-generation sustainable, reusable adhesive. The SPI/BP@mica adhesive showed excellent mold resistance (50-day shelf life) and flame retardancy (LOI = 29.7 %). Further, the cost of SPI/BP@mica adhesive is equivalent to the price of the phenol formaldehyde resin adhesive commonly used for wood-based panel. The proposed design strategy may promote the functional modification of composites and provide workable guidance for constructing robust, recyclable protein-based materials.