Regulating the Self‐Discharge of Flexible All‐Solid‐State Supercapacitors by a Heterogeneous Polymer Electrolyte

Abstract

Supercapacitors with high power density and an ultralong cyclic lifetime have been intensively investigated. However, the crucial challenge of their rapid self-discharge process is often neglected in most cases. A heterogeneous interface formed between two layers of polymer electrolytes is designed, in which a polyanion and a polycation are added into a common matrix of polymer electrolyte, respectively. By using the heterogeneous polymer electrolyte (HPE) as the separator simultaneously, the resultant supercapacitors exhibit comparable electrochemical performance to that of devices based on traditional polymer electrolytes. The HPE-based supercapacitors using both electric double-layer capacitive and pseudocapacitive electrodes show at least one time longer self-discharge time than that of devices based on homogenous polymer electrolyte, especially for the electrode in an electrolyte containing polyanion served as a positive pole during the charging process. Because of the same polymer matrix used, the heterojunction structure of the HPE exhibits excellent stability without obvious phase separation during thousands of charge/discharge and repeated bending cycles. This novel strategy by interface engineering of electrolyte to suppress the self-discharge behavior of supercapacitors is very meaningful to promote their practical applications.