The use of hydrogels in wound dressings, which is pivotal for effective wound treatment, has been widely applied to diverse medical wound conditions. However, formulating natural hydrogels that combine robust strength and self-healing capabilities is a significant challenge. To overcome this, we successfully designed a natural nanocellulose self-healing hydrogel that can quickly self-heal and restore the complete hydrogel structure after injury to fill the injured area and protect the wound from external damage. Our study utilized modified natural polymer carboxymethyl chitosan (CMC), hydrazide-modified carboxymethyl cellulose nanofibers (HCNF), and cellulose nanocrystals modified by dialdehyde (DACNC) to fabricate the hydrogel. The amides containing more amino groups and HCNF in CMC can be used as cross-linking nodes, and the high aspect ratio and specific surface area of DACNC are favorable for the connection of many active hydrogels. The hydrogel is crosslinked by the dynamic imide bond and hydrazone bond between the amino group of CMC, the amide of HCNF, and the aldehyde of DACNC and has a double network structure. These connections can be readily reassembled when disrupted, enabling fast self-healing of hydrogels within five minutes. Moreover, HCNF and DACNC were incorporated as nano-reinforced fillers to bolster the hydrogel's strength while preserving its high liquid absorption capacity (381% equilibrium swelling rate).
Keywords: cellulose nanocrystals; cellulose nanofibrils; self-healing hydrogel.