Multi-scale cellulose based new bio-aerogel composites with thermal super-insulating and tunable mechanical properties

• Aerogels preparation by freezing drying.
• Multi-scale cellulose aerogels for super thermal–insulation properties.
• Reinforcing effect of CNF and CNC as ultra-thin films in aerogels.
• Effect of TEMPO oxidation time of CNF on the structure and properties of aerogels.

Bio-composite aerogels based on bleached cellulose fibers (BCF) and cellulose nanoparticles having various morphological and physico-chemical characteristics are prepared by a freeze-drying technique and characterized. The various composite aerogels obtained were compared to a BCF aerogel used as the reference. Severe changes in the material morphology were observed by SEM and AFM due to a variation of the cellulose nanoparticle properties such as the aspect ratio, the crystalline index and the surface charge density. BCF fibers form a 3D network and they are surrounded by the cellulose nanoparticle thin films inducing a significant reduction of the size of the pores in comparison with a neat BCF based aerogel. BET analyses confirm the appearance of a new organization structure with pores of nanometric sizes. As a consequence, a decrease of the thermal conductivities is observed from 28 mW m−1 K−1 (BCF aerogel) to 23 mW m−1 K−1 (bio-composite aerogel), which is below the air conductivity (25 mW m−1 K−1). This improvement of the insulation properties for composite materials is more pronounced for aerogels based on cellulose nanoparticles having a low crystalline index and high surface charge (NFC-2h). The significant improvement of their insulation properties allows the bio-composite aerogels to enter the super-insulating materials family. The characteristics of cellulose nanoparticles also influence the mechanical properties of the bio-composite aerogels. A significant improvement of the mechanical properties under compression is obtained by self-organization, yielding a multi-scale architecture of the cellulose nanoparticles in the bio-composite aerogels. In this case, the mechanical property is more dependent on the morphology of the composite aerogel rather than the intrinsic characteristics of the cellulose nanoparticles.