Cut from the Same Cloth: Enamine-Derived Spirobifluorenes as Hole Transporters for Perovskite Solar Cells.

To attain commercial viability, perovskite solar cells (PSCs) have to be reasonably priced, highly efficient, and stable for a long period of time. Although a new record of a certified power conversion efficiency (PCE) value over 25% was achieved, PSC performance is limited by the lack of hole-transporting materials (HTMs), which extract positive charges from the light-absorbing perovskite layer and carry them to the electrode. Here, we report spirobifluorene-based HTMs with finely tuned energy levels, high glass-transition temperature, and excellent charge mobility and conductivity enabled by molecularly engineered enamine arms. HTMs are synthesized using simple condensation chemistry, which does not require costly catalysts, inert reaction conditions, and time-consuming product purification procedures. Enamine-derived HTMs allow the fabrication of PSCs reaching a maximum PCE of 19.2% and stability comparable to spiro-OMeTAD. This work demonstrates that simple enamine condensation reactions could be used as a universal path to obtain HTMs for highly efficient and stable PSCs.