Scalable, Flexible, Magnetic-Field-Guided rULGO Sponge-BN-Cobalt Oxide-Based Supercapacitors: Mechanistic Insights into Multiple Charge Transfer Pathways by the Distribution of Relaxation Times

Scalable and flexible supercapacitors are in high demand from an application point of view. Through our exploration, we have attained promising performance of electrochemical energy storage under the influence of an external magnetic field for future energy-based applications. In this work, a commercial sponge is used as a template for ultra-large graphene oxide (rULGO) functionalization, followed by the incorporation of Co₃O₄:BN without the inclusion of binders or conductive additives. The fabricated electrodes, namely, <b>SPG-rULGO</b> and <b>SPG-rULGO-Co</b>_<b>3</b><b>O</b>_<b>4</b><b>:BN</b>, demonstrate superior performance with a potential window of 2.2 V at a magnetic field strength of 13.5 and 28 mT, respectively. A specific capacitance of 218 ± 5% F·g^-¹ and 312 ± 5% F·g^-¹, respectively, with retention rates of 80 and 88% over 5000 charge-discharge cycles are achieved. In contrast to the conventional fabrication of the asymmetric device, both electrodes are made using flexible substrates with <b>SPG-rULGO-Co</b>_<b>3</b><b>O</b>_<b>4</b><b>:BN</b> as the positive electrode and <b>SPG-rULGO</b> as the negative electrode eliminating the need to use activated carbon. This configuration yields a specific capacitance of 153 ± 5% F·g^-¹ at 1 Ag^-¹, leading to a high energy density of 103 ± 5% W·h·kg^-1 at a power density of 1.10 ± 5% kW kg^-1 with an 85% retention rate. The charge-discharge mechanism of bare and modified electrodes is probed by the distribution of relaxation time analysis of the coupled electrochemical impedance spectra. The integration of magnetic field with advanced electrode materials opens up other possibilities for optimizing energy storage systems and advancing the field of flexible and mechanically robust supercapacitors.