Triiodide/iodide (I3-/I-) redox couple-mediated solar cells, batteries, and electrochromic devices require highly efficient and stable electrocatalysts for I3- reduction reaction (IRR) to overcome performance limitations, whereas the widely used platinum (Pt) cathode for IRR has limitations of high price and unfavorable durability. In this work, we present a halogen element (chlorine) doping strategy to design low-cost perovskite-type electrocatalysts with enhanced IRR activity and stability. The dye-sensitized solar cell (DSSC) assembled by the LaFeO2.965-δCl0.035 cathode delivers an attractive power conversion efficiency (PCE) of 11.4% with a remarkable PCE enhancement factor of 23% compared with Pt, which is higher than most of the reported non-Pt DSSC cathodes. Attractively, LaFeO2.965-δCl0.035 displays superior IRR activity/stability and structural stability in the I3-/I--based electrolyte compared to pristine LaFeO3 because chlorine doping facilitates the creation of oxygen vacancies (active sites) and enhances surface acidity simultaneously. This study provides a new way for designing outstanding IRR electrocatalysts, which could be applied to many redox couple-mediated photo/electrochemical devices.
Keywords: anion doping; cathode; dye-sensitized solar cell; electrocatalyst; perovskite oxide.