Bio-Based Nanocellulose Cryogels Modified with Tannin and Vanillin: Intermolecular Interactions and Functional Properties

Sustainable lightweight materials based on renewable resources have attracted increasing attention as alternatives to synthetic materials. However, developing nanocellulose cryogels with adequate structural integrity and efficient retention of phenolic compounds remains challenging, often requiring furanic and dialdehyde-based additives associated with environmental and health concerns. In this context, tannin-containing nanocellulose cryogels were produced using vanillin and hydrogen peroxide as sustainable modification agents. The effects of the additives on the structural, morphological, colorimetric, mechanical, thermal, and leaching properties of the cryogels were investigated. FTIR and colorimetric analyses revealed the presence of phenolics and the effect of hydrogen peroxide. SEM analysis showed that tannin promoted structural densification, whereas peroxide induced fragmentation of the cryogel network and pore reorganization. These changes influenced density and mechanical performance, with nanocellulose-tannin exhibiting the highest compressive strength and elastic modulus. Thermal conductivity values remained within the range reported for highly porous lignocellulosic materials (38.93–43.79 (mW/m·K)). Tannin leaching demonstrated that peroxide significantly improved tannin retention, especially in the system including vanillin which exhibited only 13,61% tannin release. Overall, vanillin and hydrogen peroxide modified the supramolecular organization and functional properties of the cryogels, highlighting their potential as additives in porous materials for thermal insulation and adsorption applications.