| Summary: | This work highlights the use of Fe-modified MgAl-layered double hydroxides (LDHs) to replace dye and semiconductor complexes in dye-sensitized solar cells (DSSCs), forming a layered double hydroxide solar cell (LDHSC). For this purpose, a MgAl-LDH and a Fe-modified MgAl LDH were prepared. X-ray diffraction spectroscopy (XRD), scanning electron microscopy (SEM), and energy-dispersive X-ray (EDX) spectroscopy were used to analyze the structural properties, morphology, and success of the Fe-modification of the synthesized LDHs. Ultraviolet-visible (UV-Vis) absorption spectroscopy was used to analyze the photoactive behavior of these LDHs and compare it to that of TiO<sub>2</sub> and dye-sensitized TiO<sub>2</sub>. Current-voltage (I–V) solar simulation was used to determine the fill factor (FF), open circuit voltage (V<sub>OC</sub>), short circuit current (I<sub>SC</sub>), and efficiency of the LDHSCs. It was shown that the MgFeAl-LDH can act as a simultaneous photoabsorber and charge separator, effectively replacing the dye and semiconductor complex in DSSCs and yielding an efficiency of 1.56%.
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