Exploring DSSC Efficiency Enhancement: SQI-F and SQI-Cl Dyes with Iodolyte Electrolytes and CDCA Optimization

This investigation delves into the potential use of halogen bonding to enhance both the short-circuit current (J_SC) and overall efficiency of dye-sensitized solar cells (DSSCs). Specifically, we synthesized two distinct dyes, SQI-F and SQI-Cl, and characterized them using FT-IR, ¹HNMR, ¹³C NMR, and mass spectroscopy. These dyes are based on the concept of incorporating halogen atoms within unsymmetrical squaraine structures with a donor-acceptor-donor (D-A-D) configuration. This strategic design aims to achieve optimal performance within DSSCs. We conducted comprehensive assessments using DSSC devices and integrated these synthesized dyes with iodolyte electrolytes, denoted as Z-50 and Z-100. Further enhancements were achieved through the addition of CDCA. Remarkably, in the absence of CDCA, both SQI-F and SQI-Cl dyes displayed distinct photovoltaic characteristics. However, through sensitization with three equivalents of CDCA, a significant improvement in performance became evident. The peak of performance was reached with the SQI-F dye, sensitized with three equivalents of CDCA, and paired with iodolyte Z-100. This combination yielded an impressive DSSC device efficiency of 6.74%, an open-circuit voltage (V_OC) of 0.694 V, and a current density (J_SC) of 13.67 mA/cm². This substantial improvement in performance can primarily be attributed to the presence of a σ-hole, which facilitates a robust interaction between the electrolyte and the dyes anchored on the TiO₂ substrate. This interaction optimizes the critical dye regeneration process within the DSSCs, ultimately leading to the observed enhancement in efficiency.