Tetraphenylbutadiene-Based Symmetric 3D Hole-Transporting Materials for Perovskite Solar Cells: A Trial Trade-off between Charge Mobility and Film Morphology

Two three-dimensional symmetric tetraphenylbutadiene derivatives decorated with diphenylamine or triphenylamine fragments are first prepared for use as hole-transporting materials (HTMs) in perovskite solar cells (PSCs). The HTMs are acquired using straightforward synthetic methods and facile purification techniques. The thermal stability, photophysical properties, electrochemical behaviors, computational study, hole mobility, X-ray diffraction, hole transfer dynamics, hydrophobicity, surface morphology, and photovoltaic performances of the HTMs are discussed. The highest power conversion efficiency (PCE) of CJ-04-based cell is 13.75%, which is increased to 20.06% when CJ-03 is used as HTM, superior to the PCE of the cell based on 2,2′,7,7′-tetrakis­(N,N-di-p-methoxyphenylamine)-9,9′-spirobifluorene (spiro-OMeTAD) (18.90%). The preparation cost of CJ-03 accounts for merely 23.1% of the price of commercial spiro-OMeTAD, while the concentration of CJ-03 solution used in the device fabrication (60.0 mg mL^–1) is lower compared with that of the spiro-OMeTAD solution (72.3 mg mL^–1). These results corroborate that the screw-like HTMs with a highly distorted configuration are facilely available and promising candidates for PSCs. More importantly, a practical solution is proposed to achieve moderate charge mobility and good film-formation ability of the HTMs simultaneously.