Sustainable Dough‐Based Gel Electrolytes for Aqueous Energy Storage Devices

Abstract Polymer gel electrolytes are usually utilized in various energy storage devices due to their advantages of excellent ionic conductivity and outstanding mechanical properties. However, they are often not biodegradable and lose their flexibility and electrochemical performance during the dehydration/hydration process. Herein, sustainable dough‐based gel electrolytes with high biosafety and environmental friendliness are developed. In the dough electrolytes, gluten molecules connect with each other through disulfide bonds to construct gluten network and water that contains abundant ions adheres on it to achieve a continuous ion transport pathway. Therefore, the dough electrolytes possess outstanding mechanical properties and excellent ionic conductivities. More impressively, they also exhibit the ability to recover their electrochemical and mechanical performance after dehydration/hydration cycles as well as the self‐adhering, degradable, and edible behaviors. As a proof of concept, the dough electrolytes are used in supercapacitors and zinc‐ion batteries. The resultant devices display comparable electrochemical performance in comparison with the counterparts with polymer gel electrolytes. Furthermore, the multiple functions of dough electrolytes are also integrated into the supercapacitors and zinc‐ion batteries devices. This work provides a promising route to design highly sustainable gel electrolytes for different aqueous energy storage devices.