PtCoFe Nanowire Cathodes Boost Short‐Circuit Currents of Ru(II)‐Based Dye‐Sensitized Solar Cells to a Power Conversion Efficiency of 12.29

PtCoFe nanowires with different alloying compositions are chemically prepared and acted as counter electrodes (CEs) in dye‐sensitized solar cells (DSSCs) with Ru(II)‐based dyes. Due to their superior I3− reduction activity, PtCoFe nanowires with rich (111) facets enhance the performance of DSSCs. Hence, N719 DSSCs with PtCoFe nanowires, respectively, produce better power conversion efficiency (PCE) of 8.10% for Pt33Co24Fe43 nanowire, 8.33% for Pt74Co12Fe14 nanowire, and 9.26% for Pt49Co23Fe28 nanowire in comparison to the PCE of Pt CE (7.32%). Further, the PRT‐22 DSSC with Pt49Co23Fe28 nanowire exhibits a maximum PCE of 12.29% with a certificated value of 12.0%, which surpass the previous PCE record of the DSSCs with Ru(II)‐based dyes. The photovoltaic and electrochemical results reveal the composition‐dependent activity along with a volcano‐shaped trend in the I−/I3− redox reaction. Theoretical work on the adsorption energies of I2, the desorption energies of I−, and the corresponding absolute energy demonstrates that the I3− reduction activity followed in the order of Pt49Co23Fe28(111) plane > Pt74Co12Fe14(111) plane > Pt33Co24Fe43(111) plane, proving Pt49Co23Fe28 nanowire to be a superior cathode material for DSSCs. PtCoFe nanowires with rich (111) planes are chemically prepared and act as the counter electrodes of dye‐sensitized solar cells (DSSCs). Evidently, Pt49Co23Fe28 nanowires demonstrate the superior catalytic properties with respect to the I−/I3− redox reactions. Thus, PRT‐22 DSSC based on Pt49Co23Fe28 nanowire produces an impressive power conversion efficiency of 12.29%.