<i>o</i>-Methoxy Substituents in Spiro-OMeTAD for Efficient Inorganic–Organic Hybrid Perovskite Solar Cells

TLDR

The study compares three spiro‑OMeTAD derivatives as hole‑transporting materials in mesoporous TiO₂/CH₃NH₃PbI₃/HTM/Au perovskite solar cells. The authors synthesized and characterized three spiro‑OMeTAD derivatives with varied methoxy positions, then evaluated their optical, electronic, and hole‑transport properties by NMR, MS, UV–vis, and cyclic voltammetry before incorporating them into the solar‑cell architecture. The cell performance depends on methoxy placement, with the o‑OMe derivative achieving a record 16.7 % PCE (Jsc = 21.2 mA cm⁻², Voc = 1.02 V, FF = 77.6 %)—the highest reported for spiro‑OMeTAD‑based perovskite cells.

Abstract

Three spiro-OMeTAD derivatives have been synthesized and characterized by 1H/13C NMR spectroscopy and mass spectrometry. The optical and electronic properties of the derivatives were modified by changing the positions of the two methoxy substituents in each of the quadrants, as monitored by UV–vis spectroscopy and cyclic voltammetry measurements. The derivatives were employed as hole-transporting materials (HTMs), and their performances were compared for the fabrication of mesoporous TiO2/CH3NH3PbI3/HTM/Au solar cells. Surprisingly, the cell performance was dependent on the positions of the OMe substituents. The derivative with o-OMe substituents showed highly improved performance by exhibiting a short-circuit current density of 21.2 mA/cm2, an open-circuit voltage of 1.02 V, and a fill factor of 77.6% under 1 sun illumination (100 mW/cm2), which resulted in an overall power conversion efficiency (PCE) of 16.7%, compared to ∼15% for conventional p-OMe substituents. The PCE of 16.7% is the highest value reported to date for perovskite-based solar cells with spiro-OMeTAD.