Semiconductor is the main part of the photoanode in dye-sensitized solar cells (DSSCs). In this study, an evaluation was conducted on two different morphological shapes of TiO2/ZnO semiconductors, namely nanoparticles (NPs) and nanofibers (NFs), to enhance the efficiency of DSSCs. The nanofibrous semiconductors were fabricated using the electrospinning technique. Furthermore, a natural sensitizer, anthocyanin dye, was used to promote the environmental friendliness of the fabricated cells. These cells were then compared to those that used a synthetic dye known as N719 to determine their efficiencies. The UV-vis results confirmed the extraction of anthocyanin from black plum fruits (Syzygium cumini). The structural characteristics of the composites were examined using XRD, FE-SEM, and BET experiments. The XRD results revealed that the anatase phase of TiO2 was dominant in the crystal structure of the semiconductors, while the crystallite sizes of the composites were 25.04 nm and 12.24 nm in NPs and NFs forms, respectively. The FE-SEM analysis revealed the formation of quasi-spherical NPs with an average diameter of 48.26 ± 17.75 nm and NFs with an average diameter of 153.99 ± 26.18 nm. The BET results showed that the surface characteristics of the nanocomposite were enhanced by changing the shape from NPs to NFs. Photovoltaic studies showed that utilizing NFs semiconductors in the photoanodes of DSSCs resulted in increased conversion efficiency of light to electricity. The results of the sun simulator studies confirmed that the use of natural dye led to a decrease in the effectiveness of the DSSCs. This phenomenon can be attributed to the weaker binding of the natural dye to the photoanodes. Furthermore, the EIS investigations illustrated that the electron lifetime in the natural dye is more than twice that of N719, leading to a reduced rate of electron recombination in the Syzygium cumini extract. The TiO2/ZnO NFs photoanodes exhibited superior performance compared to their nanoparticle counterparts in DSSCs. Their high surface area promoted superior dye adsorption and light absorption. Moreover, the interconnected nanofiber network facilitated efficient electron transport, minimizing recombination losses. Increasing the binding strength of the chosen natural dye to the photoanode will also make the cells more environmentally friendly and improve their ability to produce electricity.
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