Facile synthesis and application of nano-sized semiconductor metal oxides for optoelectronic devices have always affected fabrication challenges since it involves multi-step synthesis processes. In this regard, semiconductor oxides derived directly from metal–organic frameworks (MOFs) routes have gained a great deal of scientific interest owing to their high specific surface area, regular and tunable pore structures. Exploring the application potential of these MOF-derived semiconductor oxides systems for clean energy conversion and storage devices is currently a hot topic of research. In this study, titanium-based MIL-125(Ti) MOFs were used as a precursor to synthesize cobalt-doped TiO2-based dye-sensitized solar cells (DSSCs) for the first time. The thermal decomposition of the MOF precursor under an air atmosphere at 400 °C resulted in mesoporous anatase-type TiO2 nanoparticles (NPs) of uniform morphology, large surface area with narrow pore distribution. The Co2+ doping in TiO2 leads to enhanced light absorption in the visible region. When used as photoanode in DSSCs, a good power conversion efficiency (PCE) of 6.86% with good photocurrent density (Jsc) of 13.96 mA cm−2 was obtained with the lowest recombination resistance and the longest electron lifetime, which is better than the performance of the pristine TiO2-based photoanode.

The enduring effort toward stabilizing and improving the efficiency of dye-sensitized solar cells (DSSCs) has stirred the solar research community to follow innovative approaches. Current research centered on electrode materials design, which improves photoanodes' light-harvesting efficiency (LHE). Metal–Organic Frameworks (MOFs) are a new family of materials that can be used as competent materials due to their desirable qualities, including high porosity, flexible synthesis methodology, high thermal and chemical stability, and good light-harvesting capabilities. MOF-derived porous photoanodes can effectively adsorb dye molecules and improve LHE, resulting in high power conversion efficiency (PCE). Doping is a prospective methodology to tune the bandgap and broaden spectral absorption. Hence, a novel and cost-effective synthesis of high surface area transition metal (TM) doped TiO2 nanocrystals (NCs) via the metal–organic framework route for DSSCs is reported here. Among the TM dopants (i.e., Mn, Fe, Ni), a remarkable PCE of 7.03% was obtained for nickel-doped samples with increased Jsc (14.66 mA/cm2) due to the bandgap narrowing and porous morphology of TiO2. The findings were further confirmed using electrochemical impedance spectroscopy (EIS) and dye-desorption experiments. The present study expedites a promising way to enhance the LHE for many innovative optoelectronic devices.

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