Side chain-engineered pseudocapacitive semiconducting polymer electrodes for symmetrical supercapacitors operable at wide potentials

Pseudocapacitive electrodes based on inorganic metal oxides exhibit superior capacitance. However, they suffer from limited operational voltage, resulting in low energy and power densities. To address these issues, redox semiconducting polymer (SP)-based pseudocapacitive electrodes, integrating electron donor and acceptor functionalities, offer a promising solution. In this study, we introduce two novel pseudocapacitive SP electrodes composed of highly planar electron-donating building blocks 4,8-bis ((5-octylthiophen-2-yl)ethynyl)benzo[1,2-b:4,5-b'] dithiophene (TBDT) with an electron-accepting building blocks benzo[c][1,2,5]thiadiazole (BT) and its side chain manipulated counterpart, i.e., OBT, denoted as SP1 and SP2, respectively. Among them, SP2 demonstrates a maximum specific capacitance of 117 F/g at 1 A/g. Furthermore, a symmetric supercapacitor fabricated for full-cell applications exhibits a significant energy density, reaching 29.1 Wh kg⁻¹, and a maximum power density of 12.4 kW kg⁻¹ within the wide operating potential window of 2.5 V. The exceptional performance of the pseudocapacitive electrode can be attributed to its highly planar backbone, nanoporous morphology, low crystallinity, and low lowest unoccupied molecular orbital levels. Overall, this new class of pseudocapacitive polymer electrode holds great potential for diverse sustainable energy storage technologies, addressing the limitations of traditional inorganic metal oxide-based electrodes by offering wide potentials window.