Enhancing the Photoelectrochemical Performance of Ru(II)‐Sensitized Dye‐Sensitized Solar Cells Using Cyanopyridine‐Based Cosensitizers

The cosensitization approach is one of the widely adopted strategies for systematically enhancing photovoltaic performance of dye‐sensitized solar cells (DSSCs) by utilizing two or more dyes with distinct absorption spectra. This method achieves panchromatic absorption, improves intramolecular charge transfer performance, prevents dye aggregation, and increases dye loading capability. In this study, we investigated four previously reported push–pull‐type dianchored chromophores ( CP 1–4 ) featuring a cyanopyridine scaffold as cosensitizer to enhance the performance of Ru(II)‐based N3 ‐sensitized DSSCs. Both the co‐sensitized devices ( N3 + CP 1–4 ) and the N3 ‐only devices were fabricated using a fixed dye concentration of 0.2 mM for each sensitizer/cosensitizers, while the coadsorbent chenodeoxycholic acid (CDCA) was systematically varied between 0 and 20 mM. This systematic variation of CDCA concentration was designed to examine its role in suppressing dye aggregation and modulating interfacial charge dynamics. Among the Series, CP 4 , carrying a thiobarbituric acid anchoring/acceptor group, demonstrated superior performance at all CDCA concentrations, achieving power conversion efficiency of 6.67%, 6.79%, and 5.74%, compared to 6.02%, 6.10%, and 5.44% for devices sensitized with N3 alone. Further, electrochemical impedance spectroscopy measurements confirmed the improved charge transport and reduced recombination in these devices. These findings highlight the potential of rationally engineered cosensitizers and optimized coadsorbent concentrations for enhancing the performance of metal‐based sensitizers in DSSCs.