Wood adhesives play a critical role in the wood processing industry; however, traditional formaldehyde-based adhesives pose health risks and are reliant on non-renewable resources. This study aims to develop a bio-based wood adhesive with excellent water resistance, focusing on environmentally friendly solutions. The synthesis of an oxidized starch-lignin (OSTL) composite adhesive was accomplished by modifying starch via oxidation and subsequent cross-linking with lignin. Ammonium persulfate (APS) was employed for oxidation of starch, introducing aldehyde groups that upgrade its reactivity with lignin. Subsequently, the oxidized starch (OST) was cross-linked with the phenolic rings of lignin, resulting in a strong network structure. The oxidation of starch and its cross-linking mechanism with lignin were investigated using the Fourier transform infrared (FT-IR), proton nuclear magnetic resonance (1H-NMR), and X-ray photoelectron spectroscopy (XPS) techniques, proving the formation of aldehyde and carboxyl groups with subsequent reaction possibilities. The effects of oxidant dosage, oxidation time, and the ratio of starch to lignin on the adhesive properties were systematically studied. The results demonstrated that the OSTL adhesive, prepared under optimized conditions, exhibited outstanding adhesion strength (1.23 MPa in dry state) and water resistance (0.94 MPa after 24 h cold water immersion, 1.04 MPa after 3 h in hot water, and 0.69 MPa after 3 h in boiling water), significantly outperforming conventional wood adhesives in terms of cold water, hot water, and boiling water resistance. In addition, the thermal behavior of the OSTL adhesive was further validated using differential scanning calorimetry (DSC) as well as thermogravimetric analysis (TGA). This study presents new insights and technical support for the development of green, environmentally friendly, and highly water-resistant lignin-based bio-adhesives.

Wood adhesives play a critical role in the wood processing industry; however, traditional formaldehyde-based adhesives pose health risks and are reliant on non-renewable resources. This study aims to develop a bio-based wood adhesive with excellent water resistance, focusing on environmentally friendly solutions. The synthesis of an oxidized starch-lignin (OSTL) composite adhesive was accomplished by modifying starch via oxidation (ST) and subsequent cross-linking with lignin. Ammonium persulfate (APS) was employed for oxidation of starch, introducing aldehyde groups that upgrade its reactivity with lignin. Subsequently, the oxidized starch (OST) was cross-linked with the phenolic rings of lignin, resulting in a strong network structure. The oxidation of starch and its cross-linking mechanism with lignin were investigated using FT-IR, 1H-NMR, and XPS techniques, proving the formation of aldehyde and carboxyl groups with subsequent reaction possibilities.The effects of oxidant dosage, oxidation time, and the ratio of OST to lignin on the adhesive properties were systematically studied. The results demonstrated that the OSTL adhesive, prepared under optimized conditions, exhibited outstanding adhesion strength and water resistance in both dry and wet states, significantly outperforming conventional wood adhesives in terms of cold water, hot water, and boiling water resistance. In addition, the thermal behavior of the OSTL adhesive was further validated using differential scanning calorimetry (DSC) as well as thermogravimetric analysis (TGA). This study presents new insights and technical support for the development of green, environmentally friendly, and highly water-resistant lignin-based bio-adhesives.

To develop a fully green and non-toxic wood adhesive with improved water resistance and bonding performance for soybean meal (Glycine max (L.) Merr.)-based adhesives, oxidized tannin (OTN) was obtained by the laccase treatment of waxberry tannin (TN), a natural polyphenolic polymer, and then blended with soybean meal (SM) to prepare an oxidized tannin–soybean meal adhesive (OTS). Laccase-mediated oxidation converted the tannin polymer into quinone-rich oxidized polymeric structures, which reacted with amino groups in soybean meal proteins through Michael addition and Schiff base reactions to form a covalently crosslinked polymeric network. Under the optimal conditions of a laccase dosage of 10%, an oxidation time of 6 h, an OTN:SM mass ratio of 0.5:1, and a hot-pressing temperature of 160 °C, plywood bonded with OTS exhibited a wet shear strength of 0.85 MPa at 63 °C, representing a 136% increase over that of the neat soybean meal adhesive, and showed slightly higher bonding performance than the commercial urea-formaldehyde (UF) resin under boiling-water conditions. Structural analyses (FT-IR and XPS) verified quinone formation and carbon–nitrogen single and double bonds. Thermal analyses (DSC and TGA) revealed improved curing reactivity and significantly enhanced thermal stability compared with the neat soybean meal adhesive.