Cellulose nanofiber aerogels were used as preforms that were impregnated with a bio-epoxy resin via a widely used vacuum infusion process. The simple and straightforward nanocomposite processing approach resulted in an almost 70 % improvement in the storage modulus of the polymer with only an 11.7 wt% cellulose nanofiber content. The nanofibers were well dispersed in the polymer matrix and the fiber structures were anisotropically aligned. The impregnation time of the aerogels was also significantly lower than that of the more commonly used nanopapers. It was thus shown that environmentally friendly and mechanically robust nanocomposites could be produced by impregnating cellulose nanofiber aerogels with a thermosetting resin, using a processing approach that has a potential to be scaled up for commercial use.

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Finding renewable alternatives to the commonly used reinforcement materials in composites is attracting a significant amount of research interest. Nanocellulose is a promising candidate owing to its wide availability and favorable properties such as high Young’s modulus. This study addressed the major problems inherent to cellulose nanocomposites, namely, controlling the fiber structure and obtaining a sufficient interfacial adhesion between nanocellulose and a non-hydrophilic matrix. Unidirectionally aligned cellulose nanofiber filament mats were obtained via ice-templating, and chemical vapor deposition was used to cover the filament surfaces with an aminosilane before impregnating the mats with a bio-epoxy resin. The process resulted in cellulose nanocomposites with an oriented structure and a strong fiber–matrix interface. Diffuse reflectance infrared Fourier transform and X-ray photoelectron spectroscopy studies revealed the presence of silane on the filaments. The improved interface, resulting from the surface treatment, was observable in electron microscopy images and was further confirmed by the significant increase in the tan delta peak temperature. The storage modulus of the matrix could be improved up to 2.5-fold with 18 wt% filament content and was significantly higher in the filament direction. Wide-angle X-ray scattering was used to study the orientation of cellulose nanofibers in the filament mats and the composites, and the corresponding orientation indices were 0.6 and 0.53, respectively, indicating a significant level of alignment.

The next generation of green insulation materials is being developed to provide safer and more sustainable alternatives to conventional materials. Bio-based cellulose nanofiber (CNF) aerogels offer excellent thermal insulation properties; however, their high flammability restricts their application. In this study, the design concept for the development of a multifunctional and non-toxic insulation material is inspired by the natural composition of seaweed, comprising both alginate and cellulose. The approach includes three steps: first, CNFs were separated from alginate-rich seaweed to obtain a resource-efficient, fully bio-based, and inherently flame-retardant material; second, ice-templating, followed by freeze-drying, was employed to form an anisotropic aerogel for effective insulation; and finally, a simple crosslinking approach was applied to improve the flame-retardant behavior and stability. At a density of 0.015 g cm –3 , the lightweight anisotropic aerogels displayed favorable mechanical properties, including a compressive modulus of 370 kPa, high thermal stability, low thermal conductivity (31.5 mW m –1 K –1 ), considerable flame retardancy (0.053 mm s –1 ), and self-extinguishing behavior, where the inherent characteristics were considerably improved by crosslinking. Different concentrations of the crosslinker altered the mechanical properties, while the anisotropic structure influenced the mechanical properties, combustion velocity, and to some extent thermal conductivity. Seaweed-derived aerogels possess intrinsic characteristics that could serve as a template for the future development of sustainable high-performance insulation materials.