The interest in the development of biobased adhesives has increased due to environmental concerns. Moreover, as the production of engineered wood products (EWPs) is expected to grow, the wood adhesives market needs to transit toward formaldehyde-free products. Cellulose nanoparticles (CNPs) are a material with unique properties and advantages for producing hybrid materials as biobased wood adhesives. Besides their traditional use as reinforcing additives, CNPs can be incorporated at the beginning of the polymerization reaction to form in situ polymerized hybrid adhesives with better mechanical and physicochemical properties than the neat adhesive. Despite their outstanding characteristics, CNPs are still an emerging nanomaterial in the wood adhesive field, and the studies are incipient. This review explores the utilization of CNPs in heterogeneous polymerization for the production of polyvinyl acetate, polymeric isocyanates, waterborne polyurethane systems, and other waterborne polymer latexes. The main challenges are discussed, and some recommendations are set down for the manufacture of these novel hybrid nanocomposites.
This study explored mycelium-based composites (MBCs) as a sustainable alternative to conventional materials, focusing on the role of lignocellulosic substrates in optimizing their physical, mechanical, and biodegradability properties. It also addressed the valorization of agroforestry by-products, particularly European hazelnut shells (HZ) and radiata pine sawdust (SW), in an effort to reduce waste and minimize environmental impacts. The MBCs were obtained using two formulations (HZ100 and HZ75-SW25) of local agroforestry by-products bound together with natural growth of fungal mycelium from Ganoderma sp. We examined the physical and mechanical properties of these novel materials, including the density, shrinkage, water absorption, hydrophobicity, moduli of rupture and elasticity, and internal bond strength. Additionally, we assessed the biodegradability of the MBCs in soil to estimate the time required for complete degradation. The results clearly indicated differences in performance between the MBCs from HZ100 and HZ75-SW25. In general, HZ75-SW25 demonstrated superior mechanical performance compared to HZ100. Water absorption was low in both cases, suggesting a degree of hydrophobicity on the surface. The biodegradation results indicated that the fabricated MBCs could fully decompose in less than one year when buried in soil, confirming that these biocomposites are entirely biodegradable.
The valorization of agro-industrial byproducts as sources of functional polysaccharides is a promising strategy for developing sustainable materials. In this study, cellulose was extracted and purified from rice husk and apple pomace through sequential alkaline and bleaching treatments. Then it was chemically modified via TEMPO-mediated oxidation to obtain cellulose nanofibers (TOCNFs) with cellulose yields ranging from 23.8 to 32.4% for rice husk and 9.3–13.8% for apple pomace. Owing to its higher recovery and structural regularity, rice husk was selected for surface modification with 3-aminopropyltriethoxysilane (APTES). The resulting TOCNFs exhibited an average width of 8 nm and a carboxyl content of 0.48 mmol g−1. Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), and nitrogen determination (1.72 mg g−1) confirmed the presence of aminosilane functionalities. APTES-modified TOCNFs were incorporated as active components to develop hybrid poly(vinyl acetate) (PVA) adhesives synthesized via in situ heterogeneous water-based polymerization. The influence of TOCNF surface chemistry and sodium dodecyl sulfate (SDS) on latex particle size, rheological behavior, and adhesive performance was systematically investigated. Latex particle size increased from 193 nm (PVA-SDS) to 625 nm with TOCNF-APTES and decreased to 247 nm upon SDS addition. Rheological analysis revealed pronounced shear-thinning behavior associated with the formation of percolated nanofibrillar networks, with low-shear viscosity increasing up to 477 Pa·s for TOCNF–APTES and decreasing to 370 Pa·s with SDS. Lap-shear testing (ASTM D905) showed substantial improvements in adhesive strength, reaching up to 250 kPa compared to PVA-SDS. These results demonstrate that surface-modified CNFs act not only as mechanical reinforcements but also as interfacially active components governing polymerization behavior, rheology, and adhesive performance. This exploratory study provides a proof-of-concept for the development of sustainable wood adhesives from agro-industrial byproducts.