Metal ion and hydrogen bonding synergistically mediated carboxylated lignin/cellulose nanofibrils composite film

In order to alleviate the resource and environmental problems caused by plastic film materials, the development of biodegradable cellulose-based films is crucial. Inspired by the strengthening mechanism of cellulose-lignin network from wood, carboxylated lignin (CL) was isolated using maleic acid (MA) pretreatment catalyzed by metal chlorides. Compared with pure MA, the presence of metal ions yielded CL with high carboxyl content (0.34 mmol/g), small size and good dispersibility. CL was then composited with CNF to prepare various CL/ cellulose nanofibrils (CNF) composite films. When the addition of ferric chloride was 0.3 mmol/g maleic acid, the corresponding composite films exhibited highest tensile strength (180.0 MPa), Young's modulus (13.0 GPa) and excellent ultraviolet blocking rate (97.0 %). Meanwhile, the interaction forces measured by atomic force microscope showed that the binding between CNF and various CLs (276-406 nN) was higher than that between pure CNFs (202 nN), verifying that CL enhanced the mechanical properties of composite films. In summary, this work constructs a super-strong network between CL and CNF synergistically mediated by metal ion crosslinking and hydrogen bonding, which can be a promising alternative to replace conventional plastics in multiple areas.