A self-healing, recyclable and conductive gelatin/nanofibrillated cellulose/Fe3+hydrogel based on multi-dynamic interactions for a multifunctional strain sensor

Conductive hydrogels have emerged as promising material candidates for multifunctional strain sensors, attributed to their similarity to biological tissues, good wearability, and high accuracy of information acquisition. However, it is difficult to simultaneously manufacture conductive hydrogel-based multifunctional strain sensors with the synergistic properties of reliable healability for long-term usage and environmental degradability/recyclability for decreasing the electronic waste. This work reports a facile strategy to engineer a self-healing, recyclable and conductive strain sensor by virtue of molecular-level multi-dynamic interactions (MMDIs) including Schiff base complexes, hydrogen bonds, and coordination bonds, which were fabricated using a dialdehyde TEMPO (2,2,6,6-tetramethylpiperidine-1-oxyl)-oxidized nanofibrillated cellulose (DATNFC) pre-reinforced gelatin nanocomposite hydrogel (gelatin/DATNFC hydrogel, GDH) followed by dipping in an Fe3+ aqueous solution. The MMDI strategy allows synchronous regulation of both bulk and interfacial interactions to obtain exciting properties that outperform those of conventional hydrogels, including extraordinary compressive stress (1310 kPa), intriguing self-healing abilities, and remarkable electrical conductivity. With these outstanding merits, the as-prepared gelatin/DATNFC/Fe3+ hydrogel (GDIH) is developed to be a multifunctional strain sensor with appealing strain sensitivity (GF = 2.24 under 6% strain) and compressive sensitivity (S = 1.14 kPa-1 under 15 kPa), which can be utilized to manufacture electronic skin and accurately discern subtle bodily motions, handwriting and personal signatures. Notably, this GDIH-based sensor also exhibited reliable self-healing properties for long-term usage, environmental degradability and complete recyclability for decreasing the electronic waste. In consideration of the extremely facile preparation process, biocompatibility, satisfactory functionalities, remarkable self-healing properties and recyclability, the emergence of the GDIH-based sensor is believed to propose a new strategy for the development of sustainable-multifunctional strain sensors and healthcare monitoring.