Starch‐Based Organogel Polyelectrolyte with Dual Cross‐Linked Networks for Self‐Powered Energy and Sensing Applications

Abstract Polysaccharide polyelectrolytes with tunable cross‐linked structures and intrinsic conductivity and antibiosis address the energy consumption and high carbon emissions of wearable electronic devices. However, it is a great challenge to fabricate polysaccharide ionohydrogels with high conductivity and low stress loss for new energy generation and storage and other multiple occasion applications. Herein, a novel organogel polyelectrolyte (OST/P(AM‐co‐DMAEA‐Q)/ZA) based on conjoined double cross‐linked networks with high intrinsic conductivity, robust adhesion, and antibacterial properties is successfully prepared using oxidized starch (OST) and poly(ionic liquid) electrolyte (P(AM‐co‐DMAEA‐Q)). The organogel polyelectrolyte exhibits 446% mechanical stretchability, 136 mS m −1 conductivity and 100% antibacterial efficacy against E. coli . A series of self‐powered polyelectrolyte‐based energy and sensing devices are constructed and the assembled triboelectric nanogenerators (TENGs) harvest performance with an open‐circuit voltage of 118 V, while the supercapacitors (SCs) possess a high energy storage capacity of 87.84 mF cm −2 and long‐term durability. Furthermore, the organogel polyelectrolyte demonstrates moisture‐electric generation by utilizing ambient moisture to generate electricity. Additionally, the strain sensors effectively reproducibility detect human motions and serve as temperature sensors with a rapid response rate. This work develops a starch organogel polyelectrolyte for self‐powered energy and sensing applications via the designed dual cross‐linked networks.