Colloidal Processing and Alignment of Wood-Based Dispersions and Hybrid Functional Foams

Abstract: This thesis presents novel methods and approaches for designing, preparing/fabricating, and characterizing wood-based nanomaterials. It investigates how modifications in structure, process variables, and composition can enhance functional properties. It employs advanced characterization techniques to analyze process-structure-property relationships and utilizes innovative colloidal processing approaches such as controlled nanoparticle incorporation, Layer-by-Layer self-assembly, and unidirectional ice-templating to improve the functional properties of wood-based nanomaterials.A novel approach has been developed to fabricate lightweight, highly porous hybrid foams using iron oxide nanoparticles (IONP) and TEMPO-oxidized cellulose nanofibers (TOCNF). The addition of tannic acid (TA) and the application of a magnetic field-enhanced unidirectional ice-templating technique (MFUIT) enhanced processability, mechanical, and magnetic characteristics of the foams. The hybrid foam containing 87% IONPs exhibited a saturation magnetization of 83.2 emu g–1, which is equivalent to 95% of the magnetization value observed in bulk magnetite.Hybrid, anisotropic foams have been prepared by incorporation of reduced graphene oxide (rGO) onto the macropore-walls of anisotropic TOCNF foams using a liquid-phase Layer-by-Layer self-assembly method. These hierarchical rGO-TOCNF foams exhibit lower radial thermal conductivity (λr) across a wide range of relative humidity compared to control TOCNF foams.The shear-induced orientations and relaxations of multi-component dispersions containing cellulose nanocrystals (CNC) and montmorillonite nanoplatelets (MNT) have been studied by rheological small-angle X-ray scattering (Rheo-SAXS). The addition of MNT resulted in gelation and changes in flow behavior, shear responses, and relaxation dynamics. Rheo-SAXS measurements showed that CNC and MNT aligned under shear, creating aligned structures that relaxed upon shear removal. Gaining insights into shear-induced orientations and relaxation dynamics can aid in the development of advanced wood-based nanocomposite materials.Transmission Electron Microscopy (TEM) was employed to characterize lignin oleate nanoparticles (OLNPs) derived from abundant lignin waste. TEM analysis revealed that the OLNPs had a spherical shape and a core-shell structure. Upon drying, the particles tended to agglomerate due to the loss of electrostatic repulsion forces. This agglomeration behavior indirectly supports the hypothesis that oleate chains act as a hydration barrier, preventing water permeation into the particles. Finally, a comprehensive study showed that TEMPO-oxidized lignocellulose nanofibers (TOLCNF)-based foams made from unbleached pulp can be used to prepare anisotropic, light-weight ice-templated foams with high mechanical strength. TOLCNF foams utilize lignin and hemicellulose to enhance properties while require less energy for production compared to TOCNF-based foams. This study emphasizes the potential for developing sustainable wood-based nanomaterials using TOLCNF.The results presented in this thesis offer valuable insights for further advancements of wood-based nanomaterials.