High-Lignin-Containing Cellulose Nanofibrils from Date Palm Waste Produced by Hydrothermal Treatment in the Presence of Maleic Acid.

Lignin-containing cellulose nanofibrils (LCNFs) have attracted great attention because the presence of lignin brought additional merits to cellulose nanofibrils including hydrophobicity, ultraviolet (UV)-shielding capacity, and reduced water sensitivity. In the present work, LCNFs with lignin content up to 21 wt % were prepared with a high yield exceeding 70 wt %, from neat date palm waste, by a hydrothermal treatment (HTT) at 120-150 °C in the presence of 20-30 wt % maleic acid, followed by high-pressure homogenization. The chemical composition, degree of polymerization, morphology, and colloidal and rheological properties of the LCNFs were investigated to understand how the HTT in the presence of MA affected the properties of the resulting LCNFs. Nanopapers prepared from the LCNF suspensions exhibited mechanical properties lower than those from lignin-free CNF-based nanopapers, yet with decreased hydrophilicity. A mechanism explaining how the HTT in the presence of MA facilitated the disintegration of the biomass into nanoscale material was proposed. Overall, the present work demonstrated a feasible and scalable approach for the sustainable production of LCNF suspensions from neat agricultural residues, with a high yield and a high lignin content, without any need to perform a preliminary partial delignification.

Lignin-Containing Cellulose Nanofibrils from TEMPO-Mediated Oxidation of Date Palm Waste: Preparation, Characterization, and Reinforcing Potential.

Lignin-containing cellulose nanofibrils (LCNFs) have emerged as a new class of nanocelluloses where the presence of residual lignin is expected to impart additional attributes such as hydrophobicity or UV-absorption. In the present work, LCNFs with a lignin content between 7 and 15 wt% were prepared via a TEMPO-mediated oxidation as chemical pretreatment followed by high-pressure homogenization. The impact of the carboxyl content (CC) on the properties of the resulting LCNF gel, in terms of lignin content, colloidal properties, morphology, crystallinity, and thermal stability, were investigated. It was found that lignin content was significantly decreased at increasing CC. In addition, CC had a positive effect on colloidal stability and water contact angle, as well as resulting in smaller fibrils. This lower size, together with the lower lignin content, resulted in a slightly lower thermal stability. The reinforcing potential of the LCNFs when incorporated into a ductile polymer matrix was also explored by preparing nanocomposite films with different LCNF contents that were mechanically tested under linear and non-linear regimes by dynamic mechanical analysis (DMA) and tensile tests. For comparison purposes, the reinforcing effect of the LCNFs with lignin-free CNFs was also reported based on literature data. It was found that lignin hinders the network-forming capacity of LCNFs, as literature data shows a higher reinforcing potential of lignin-free CNFs. Nonetheless, the tensile strength of the acrylic matrix was enhanced by 10-fold at 10 wt% of LCNF content.