Deep eutectic solvents (DESs) are beginning to attract interest as electrolyte alternatives to conventional organic solvents and ionic liquids within dye-sensitized solar cells (DSSCs). The precise roles played by DES components and whether they simply represent a benign medium for mobilizing charge carriers or present beneficial functionality that impacts device performance remain unclear. To begin to address this deficiency in understanding, we performed a comprehensive characterization of the three “canonical” choline chloride-based DESs (i.e., reline, ethaline, and glyceline) as DSSC electrolytes hosting the iodide–triiodide (I/I3) redox couple. The measurement of electrolyte viscosities, determination of triiodide diffusion coefficients, and photovoltaic performances assessed for water contents up to 40 wt. % allow the emergence of several important insights. A comparison to the observed photovoltaic performance arising from the individual components aids in further clarifying the impact of DES chemistry and solution viscosity on photovoltaic and charge carrier diffusion characteristics. Finally, we introduce the DES guaniline—consisting of a 1:1 molar ratio mixture of choline chloride with guanidinium thiocyanate—demonstrating it to be a superior DSSC electrolyte over those formulated from the three most widely studied canonical DESs at all water contents investigated.

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