To cope up with the sustainable energy storage goals for supercapacitors (SCs), the self-discharge in SC electrodes is a significant hurdle, and thereby, nickel sulfide (NS) with high conductivity is adopted as a test vehicle for understanding the morphological evolution effects for long-life SCs. Herein, honeycomb-like NS is hierarchically formed over hydrothermally grown nickel oxide (NO) via successive ionic layer adsorption reaction (SILAR) method. Their heterostructure shows a fivefold improvement in specific capacitance from 348 F g−1 to 2077 F g−1 at 1 mV s−1 over bare NO. Furthermore, the remarkable upliftment of capacitance retention is achieved from 60.7% to 92.3% even after 3000 cycles via morphological control of NS/NO hetero-structure with the help of highly conductive NS. More importantly, the self-discharge behaviors and synergistic role of leakage current associated with morphological evolution via NS overcoating are studied in detail. In particular, the self-discharge mitigation from 45% (NO) to 35% (NS20/NO) due to the NS/NO heterostructure and the behind mechanism are ascribed to the activated-controlled Faradaic reaction coupled with a charge redistribution. This study emphasizes the potential importance of composite heterostructure by tuning the electrical conductivity and morphological adjustment NO via consecutive overcoating of NS through SILAR as a novel strategy. This enhances charge storage, redox kinetics, and the mitigation of self-discharge properties of the active electrode materials. For practical validation on sustainable energy storage, NS20/NO supercapacitors illuminate the LED for 35% longer than NO after one-time charging, potentially beneficial for the next generation SCs.
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