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.

In this work, a highly branched polyurea (HBP-NH₂) similar to urea structure was introduced to phenol-formaldehyde (PF) resin to accelerate itscuring speed The results of gel time and bonding strength were combined to obtain a good modified additional stage and amount of HBP-NH₂. The relative molar mass changes of HBP-NH₂-modified PF resin were investigated by gel permeation chromatography (GPC). The effects of HBP-NH₂ on the curing of PF resin were investigated by differential scanning calorimetry (DSC) and dynamic mechanical analysis (DMA). The effect of HBP-NH₂ on the structure of PF resin was also investigated by nuclear magnetic resonance carbon spectroscopy (¹³C-NMR). The test results show that the gel time of the modified PF resin was reduced by 32% and 51% at 110 °C and 130 °C, respectively. Meanwhile, the addition of HBP-NH₂ increased the relative molar mass of PF resin. The bonding strength test showed that the bonding strength of modified PF resin increased by 22% after soaking in boiling water (93 °C ± 2) for 3 h. The DSC and DMA analysis indicated that the curing peak temperature decreased from 137 °C to 102 °C, and the curing rate of the modified PF resin was also faster than that of the pure PF resin. The ¹³C-NMR results showed that HBP-NH₂ in the PF resin reacted to produce a co-condensation structure. Finally, the possible reaction mechanism of HBP-NH₂ for the modification of PF resin was given.

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.