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An ionic liquid, 1-methyl-3-propylimidazolium iodide (MPII), was solidified with an organic hole-transporting material, 4,4′,4″-tris[(3-methylphenyl)phenylamino]triphenylamine (m-MTDATA), and the resulting solid-state redox mediator (RM) (m-MTDATA-solidified MPII) was employed in solar devices to realize solid-state dye-sensitized solar cells (sDSSCs). Solar devices with only MPII or m-MTDATA as an RM showed almost 0 mA/cm2 of short-circuit current (Jsc) and thus 0% power conversion efficiency (PCE). However, an sDSSC with the m-MTDATA-solidified MPII exhibited 4.61 mA/cm2 of Jsc and 1.80% PCE. It was found that the increased Jsc and PCE were due to the formation of I3−, which resulted from a reaction between the iodie (I−) of MPII and m-MTDATA cation. Further enhancement in both Jsc (9.43 mA/cm2) and PCE (4.20%) was observed in an sDSSC with 4-tert butylpyridine (TBP) as well as with m-MTDATA-solidified MPII. We attributed the significant increase (about 230%) in PCE to the lowered diffusion resistance of I−/I3− ions in the solid-state RM composed of the m-MTDATA-solidified MPII and TBP, arising from TBP’s role as a plasticizer.

The leakage and volatilization of liquid electrolytes limit the commercialization of dye-sensitized solar cells (DSCs). As solid-state (ss) hole-transporting materials, free from leakage and volatilization, biscarbazole-based polymers with different molecular weights (PBCzA-H (21,200 g/mol) and PBCzA-L (2450 g/mol)) were applied in combination with additives to produce ssDSCs. An ssDSC with PBCzA-H showed a better short-circuit current (Jsc), open-circuit voltage (Voc), and fill factor (FF) than a device with PBCzA-L, resulting in 38% higher conversion efficiency. Compared to the PBCzA-L, the PBCzA-H with a higher molecular weight showed faster hole mobility and larger conductivity, leading to elevations in Jsc via rapid hole transport, Voc via rapid hole extraction, and FF via lowered series and elevated shunt resistances. Thus, it is believed that PBCzA-H is a useful candidate for replacing liquid electrolytes.