Mechanoresponsive self‐powered piezoelectric energy‐generating composite hydrogels based on carbon nanotube‐reinforced fungal‐carboxymethyl chitosan‐bacterial cellulose nanofibers for wearable electronics

Abstract Developing conductive hydrogels with both enhanced mechanical properties and superior sensing capabilities for wearable, flexible electronics remains challenging. Here, we developed mechanoresponsive self‐powered piezoelectric energy‐generating composite hydrogels. These hydrogels were prepared by blending fungal‐derived carboxymethyl chitosan (FC), carboxylate‐bacterial cellulose nanofibers (CBC‐NFs), and carbon nanotubes (CNTs) within a covalently crosslinked polyacrylamide (PAM) network (CNT‐FBCNF). The resulting hydrogels showed remarkable mechanical properties due to the molecular interactions between polymer chains. The hydrogels showed a self‐recoverable property and high stability under compressive mechanical force at 40% of strain (2000 cycles). The maximum compressive load (N) of 27.8 N was obtained for the optimized hydrogel, CNT‐FBCNF (1% CNT content). This hydrogel exhibited a good conductivity of 1.3 S/m, which was attributed to the homogeneous dispersion of CNTs within the hydrogel matrix and sufficient biocompatibility with skin fibroblasts. The hydrogel also exhibited impressive performance as a strain sensor, boasting a wide strain range (10–40%), excellent stability, and repeatability. Furthermore, strategic cutting and assembly of the hydrogel generated a flexible strain sensor capable of accurately monitoring finger and thumb pressure in real‐time. This study will significantly accelerate the development of hydrogel‐based sensors within the rapidly advancing field of wearable soft electronics. Highlights CNT‐reinforced composite hydrogel was developed The optimized hydrogel showed good electrical conductivity (1.3 S/m) The optimized hydrogel showed good self‐recovery properties The optimized hydrogel exhibited impressive strain‐sensing capability between 10% and 40% strain