Interfacial recombination and limited ionic mobility remain major bottlenecks in advancing dye-sensitized solar cell (DSSC) performance. In this work, we develop a dual-material strategy that simultaneously enhances electronic and ionic transport by integrating a microwave-synthesized polythiophene–fullerene (PTh–C₆₀) nanocomposite counter electrode with a binary-cation ionic liquid polymer gel electrolyte (ILPGE). The optimized PTh–C₆₀ electrode exhibits a markedly improved electrical conductivity of 83.15 S cm⁻¹ , as confirmed by four-point probe analysis, supported by structural and morphological evidence from XRD and SEM. The ILPGE, formulated using LiI and TPAI within a polyacrylonitrile matrix and supplemented with an imidazolium-based ionic liquid, demonstrates a maximum ionic conductivity of 2.02 × 10⁻² mS cm⁻¹ and stable, reversible redox behavior over a wide electrochemical window (–1.5 V to +1.5 V). Molecular dynamics simulations reveal significantly enhanced ion diffusion in the dual-cation gel, while DFT calculations confirm favorable PTh–C₆₀ interaction energies that support efficient electrocatalytic interfaces. When integrated into a quasi-solid-state DSSC, the optimized materials deliver a power conversion efficiency of 7.87 %, surpassing the standard Pt-based device (7.45 %). Notably, the quasi-solid-state cell exhibits excellent long-term durability, retaining its performance beyond 25 days, whereas the standard device undergoes rapid degradation. This combined materials design offers a scalable and stable pathway for improving charge transport, interfacial kinetics, and operational lifetime in next-generation quasi-solid-state DSSCs.
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