Water‐Triggered Reconfigurable Glycerogels for Sustainable All‐Gel Supercapacitors

The polymeric structures of synthetic gels are typically static, which makes them damage-prone and nonrecyclable. Inspired by the dynamic reconfigurability of biological tissues, which eliminate old/damaged cells and regenerate new ones via biological triggers/signals, a reconfigurable biopolymer gel is presented based on a glycerol-mediated supramolecular gelation strategy. In response to an eco-friendly triggering agent water, this gel undergoes on-demand molecular-level reconfiguration. The versatility of the approach enables the development of reconfigurable gels with modulated functionality. As a proof-of-concept, a reconfigurable glycerogel electrode and electrolyte are developed and used to prototype an all-gel supercapacitor that exhibits exceptional self-healing, degradation, and rebuilding abilities. Furthermore, it can tolerate extreme mechanical deformations (e.g., stretching, bending, and twisting) and temperatures (-20 to 80 °C). The device exhibits excellent energy storage performance, with a maximum areal capacitance of 450 mF cm^-2 (at 0.035 mA cm^-2) and remarkable capacitance retention of 89% following 20 000 charge/discharge cycles (at 0.35 mA cm^-2). Moreover, following self-healing and rebuilding, the capacitance remains at 91% and 110% (at 0.35 mA cm^-2) of the original value, respectively. This generalized strategy for preparing multifunctional reconfigurable gels will facilitate the development of high-performance flexible and wearable devices with improved durability and recyclability.