Additive-free, Cost-Effective Hole-Transporting Materials for Perovskite Solar Cells Based on Vinyl Triarylamines

A series of cost-effective hole-transporting materials (TOP-HTMs) for perovskite solar cells (PSCs) was designed and synthesized. The molecules, composed of multiple 4,4'-dimethoxytriphenylamines linked to a benzene core via trans-vinylene units, can be manufactured from inexpensive materials through a simple synthetic route. The photophysical, electrochemical, and thermal properties, as well as hole mobilities, were strongly influenced by the position and number of vinyl triarylamine substituents on the core benzene ring. CH₃NH₃PbI₃-based solar cells using the X-shaped TOP-HTM 3 with additives gave a high power conversion efficiency of 17.5% (forward scan)/18.6% (reverse scan). Crucially, TOP-HTMs gave high working device efficiency without the need for conduction-enhancing additives. The power conversion efficiency for the device with additive-free TOP-HTM 3 was 16.0% (forward scan)/16.6% (reverse scan). Device stability is also enhanced and is superior to the reference HTM, 2,2',7,7'-tetrakis(N,N-di-p-methoxyphenylamine)-9,9'-spirobifluorene (Spiro-OMeTAD).