Mechanically strong, self‐healing and pH‐responsive lignocellulose nanofibril‐based hydrogels towards drug delivery applications

Abstract Employing lignocellulosic nanofibers (LCNF) with natural, high specific mechanical performance and abundant functional groups to design a hydrogel as a drug-sustained release carrier, which conforms to the concept of green and sustainable development. Herein, we facilely extracted carboxylated lignocellulose nanofibrils (CLCNF) from bagasse via a deep eutectic solvent (DES) and mechanical defibrillation-based strategy. The CLCNF crosslinked with poly(vinyl alcohol) (PVA) to obtain a nanocomposite hydrogel (PVA/CLCNF/B) whereupon the mechanical strength and drug release behavior were improved in the process. Consequently, the lignocellulose nanocomposite hydrogel presented a high compression modulus (3.92 MPa) and significant sustained‐release effect with a release rate of 80.73% after 36 h. TH delivery behavior of the PVA/CLCNF/B composite hydrogel could be controlled by acidic pH conditions. The TH release kinetics of PVA/CLCNF/B hydrogel in different phosphate buffer saline (PBS) followed the Korsmeyer‐Peppas model better, and the release of TH through the Fickian diffusion mechanism. Importantly, the vitro cytotoxicity tests showed PVA/CLCNF/B hydrogel had good biocompatibility. Overall, adding CLCNF to hydrogel may present great potential in drug release and therapy as a drug delivery carrier.