Expandable and scalable production of cellulose nanofibrils via highly efficient swelling-modification in deep
Shaoning Wang1,2, Lili Zhang1,2, Enqing Zhu1,2
1Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, Nanjing Forestry University, Nanjing, China.
Abstract:
The scalable production of chemically tailored cellulose nanofibrils (CNFs) remains challenging because native cellulose lacks sufficient chemical versatility for simultaneous fibrillation and functional regulation. Here, we develop a highly efficient swelling-modification strategy using a hydrated deep eutectic solvent (Zn(OAc)2/ChCl/H2O) to enable efficient CNF production and programmable chemical modification. Zn(OAc)2 regulates proton activity through buffering effects, suppressing excessive hydrolysis and preserving the crystalline structure of CNFs with an ultrathin diameter (3-4 nm), high aspect ratio (~1800), high degree of polymerization (600-900), and high yield (93%). By incorporating diverse cyclic anhydrides, this DES system is transformed into a multifunctional operating platform, enabling customizable CNFs with diverse chemical functionalities, including carboxyl groups, double bonds, bridged bicyclic structures, and aromatic rings. This highly efficient swelling-modification strategy provides a scalable and expandable route toward customized CNFs, advancing the design of cellulose-based functional nanomaterials.


