Photo-assisted energy storage systems, by which solar energy can be both converted and stored, have been of interest in the past few years. Novel energy conversion and storage technology is offered by photo-supercapacitors through the combination of an energy collecting unit and a supercapacitor. This dual-application system effectively generates and stores power in a single device, which makes it appropriate for various purposes. In this work, the electrochemical anodization-electrodeposition has been employed to fabricate manganese-nickel sulfide (Mn-Ni-S) nanostructures on titania nanotubes (TNs) and used them as photoelectrodes in photo-supercapacitors. The high surface area and improved properties make TNs considerably important for energy production and storage. Photoelectrochemical analysis was carried out in a three-electrode system under a xenon (Xe) lamp irradiation using the film prepared as the photoelectrode. The highest photocurrent and photovoltage were shown by MnNiS-3/TN electrode, indicating its superior photosensitivity. Upon illumination under a 0.7 mA/cm(2) current density, the area-specific capacitance of MnNiS-3/TN electrode increased from 388.3 to 723.3 mF/cm(2), which is 2.0, 3.6, and 12.8 times higher than the corresponding values for NiS/TN, MnS/TN, and bare TN electrodes under similar conditions, respectively. This indicates the considerable enhancement of the capacitance of this electrode induced by light. The desirable light-sensitive properties of MnNiS/TN make it capable of simultaneous solar energy harvesting and storage. Light sensitivity makes it possible to charge MnNiS/TN optically. More importantly, upon light irradiation, the capacity can be increased from 374.7 to 630.2 mF/cm(2) (current density 0.5 mA/cm(2)) compared to the corresponding value in the dark. Using MnNiS-3/TN as the best photoelectrode and MnS/FTO, NiS/FTO, MnNiS-1/FTO, MnNiS-2/FTO, and MnNiS-3/FTO as the counter electrodes, photo-charged through light illumination on their surfaces, five asymmetric solid-state photo-supercapacitors (ASSPS) were prepared. MnNiS-3/TN//MnNiS-3/FTO device showed the largest CV curve area, which indicated its highest areal capacitance. High capacitance gain under irradiation (155.7% at 2.0 mA/cm(2)) and outstanding capacitance maintenance (97.9% over 10000 cycles) were shown by this ASSPS. Furthermore, a great energy density of 4855.4 mWh/cm(2) was shown by the MnNiS-3/TN//MnNiS-3/FTO device under light irradiation. This research introduces a novel approach to the development of powerful solar energy conversion/storage devices.
