The upcycling of discarded garments can help to mitigate the environmental impact of the textile industry. Here, we fabricated hybrid anisotropic foams having cellulose nanocrystals (CNCs), which were isolated from discarded cotton textiles and had varied surface chemistries as structural components, in combination with xanthan gum (XG) as a physical crosslinker of the dispersion used for foam preparation. All CNCs had crystallinity indices above 85 %, zeta potential values below -40 mV at 1 mM NaCl, and true densities ranging from 1.61 to 1.67 g center dot cm(-3). Quartz crystal microbalance with dissipation (QCM-D) measurements indicated weak interactions between CNC and XG, while rheology measurements showed that highly charged CNCs caused the XG chains to change from an extended to a helicoidal conformation, resulting in changes the in viscoelastic properties of the dispersions. The inclusion of XG significantly enhanced the compression mechanical properties of the freeze-casted foams without compromising their thermal properties, anisotropy, or degree of alignment. CNC-XG foams maintained structural integrity even after exposure to high humidity (91 %) and temperatures (100 degrees C) and displayed very low radial thermal conductivities. This research provides a viable avenue for upcycling cotton-based clothing waste into high-performance materials.

Lightweight and mechanically robust hybrid foams based on cellulose nanocrystals (CNC) and multi-walled carbon nanotubes (MWCNT) with an anisotropic structure are prepared by directional ice-templating. The anisotropic hybrid CNC-MWCNT foams displayed a combination of highly anisotropic thermal conductivity and an orientation-dependent electromagnetic interference (EMI) shielding with a maximum EMI shielding efficiency (EMI-SE) of 41–48 dB between 8 and 12 GHz for the hybrid foam with 22 wt% MWCNT. The EMI-SE is dominated by absorption (SE_A) which is important for microwave absorber applications. Modelling of the low radial thermal conductivity highlighted the importance of phonon scattering at the heterogeneous CNC-MWCNT interfaces while the axial thermal conductivity is dominated by the solid conduction along the aligned rod-like particles. The lightweight CNC-MWCNT foams combination of an anisotropic thermal conductivity and EMI shielding efficiency is unusual and can be useful for directional heat transport and EMI shielding. 

Nanoparticles extracted from plants or textile waste are promising candidates for the design of sustainable materials. In this thesis, I explored how nanoparticles extracted from trees and from Kevlar and cotton textile wastes can be processed to form lightweight composite foams. The heat transfer and other functional properties such as electromagnetic shielding have been related to the structure, composition, and processing of the composite foams. 

Specifically, upcycled aramid nanofibers (upANF_A) with a small diameter were derived from Kevlar yarn. The upANF_A could be combined with wood-based cellulose nanofibrils (CNF) to produce moisture-resilient anisotropic foams with a very low thermal conductivity perpendicular to the aligned nanofibrils. The very low radial thermal conductivity was related to the strong interfacial phonon scattering between the very thin upANF_A and CNF in the hybrid foam walls. 

Aqueous dispersions of multiwalled carbon nanotubes (MWCNT) and cellulose nanocrystals (CNC) were used to form anisotropic foams with an anisotropic heat transport and orientation-dependent electromagnetic interference shielding efficiency (EMI-SE). The low-density (31 kg m^–3) CNC-MWCNT hybrid foams with 22 wt% MWCNT were mechanically robust along the axial direction (Young’s Modulus of 1200 kPa). The foams displayed an absorption-dominated EMI-SE of up to 41–48 dB and transferred heat favorably along the axial direction compared to the radial, meaning that this material could be useful in devices that require directional heat management and electromagnetic shielding.

A novel wet-foaming with subsequent freeze-casting process was developed to produce air- and ice-templated foams based on methylcellulose, CNF, and tannic acid. The air- and ice-templated foams displayed a high specific compression stiffness compared with other CNF-based materials while maintaining good insulation properties. 

Hybrid foams based on CNC extruded from cotton textile waste and wood-based CNF were prepared by freeze-casting in combination with two different solvent removal routes: supercritical drying and freeze drying. The nanoparticles in the foam walls of the freeze-dried foams were more densely packed, and the foams were mechanically stiffer and more resistant to moisture, whereas the supercritically dried foams displayed a significantly larger surface area. This highlights how the processing techniques govern the structure of a material, which in turn affects its properties. 

Biopolymer-based functional materials are essential for reducing the carbon footprint and providing high-quality lightweight materials suitable for packaging and thermal insulation. Here, cellulose nanocrystals (CNCs) were efficiently upcycled from post-consumer cotton clothing by TEMPO-mediated oxidation and HCl hydrolysis with a yield of 62% and combined with wood cellulose nanofibrils (CNFs) to produce anisotropic foams by unidirectional freeze-casting followed by freeze drying (FD) or supercritical-drying (SCD). Unidirectional freeze-casting resulted in foams with aligned macropores irrespective of the drying method, but the particle packing in the foam wall was significantly affected by how the ice was removed. The FD foams showed tightly packed and aligned CNC and CNF particles while the SCD foams displayed a more network-like structure in the foam walls. The SCD compared to FD foams had more pores smaller than 300 nm and higher specific surface area but they were more susceptible to moisture-induced shrinkage, especially at relative humidities (RH) > 50%. The FD and SCD foams displayed low radial thermal conductivity, and the FD foams displayed a higher mechanical strength and stiffness in compression in the direction of the aligned particles. Better understanding how drying influences the structural, thermal, mechanical and moisture-related properties of foams based on repurposed cotton is important for the development of sustainable nanostructured materials for various applications.

Low-density foams and aerogels based on upcycled and bio-based nanofibers and additives are promising alternatives to fossil-based thermal insulation materials. Super-insulating foams are prepared from upcycled acid-treated aramid nanofibers (upANF_A) obtained from Kevlar yarn and tempo-oxidized cellulose nanofibers (CNF) from wood. The ice-templated hybrid upANF_A/CNF-based foams with an upANF_A content of up to 40 wt% display high thermal stability and a very low thermal conductivity of 18–23 mW m⁻¹ K⁻¹ perpendicular to the aligned nanofibrils over a wide relative humidity (RH) range of 20% to 80%. The thermal conductivity of the hybrid upANF_A/CNF foams is found to decrease with increasing upANF_A content (5–20 wt%). The super-insulating properties of the CNF-upANF_A hybrid foams are related to the low density of the foams and the strong interfacial phonon scattering between the very thin and partially branched upANF_A and CNF in the hybrid foam walls. Defibrillated nanofibers from textiles are not limited to Kevlar, and this study can hopefully inspire efforts to upcycle textile waste into high-performance products.

By forming and directionally freezing an aqueous foam containing cellulose nanofibrils, methylcellulose, and tannic acid, we produced a stiff and tough anisotropic solid foam with low radial thermal conductivity. Along the ice-templating direction, the foam was as stiff as nanocellulose–clay composites, despite being primarily methylcellulose by mass. The foam was also stiff perpendicular to the direction of ice growth, while maintaining λ_r < 25 mW m^–1 K^–1 for a relative humidity (RH) up to 65% and <30 mW m^–1 K^–1 at 80% RH. This work introduces the tandem use of two practical techniques, foam formation and directional freezing, to generate a low-density anisotropic material, and this strategy could be applied to other aqueous systems where foam formation is possible.