Solution-processed hole contact materials, as an indispensable
component in perovskite solar cells (PSCs), have been widely studied
with consistent progress achieved. One bottleneck for the commercialization
of PSCs is the lack of hole contact materials with high performance,
cost-effective preparation, and green-solvent processability. Therefore,
the development of versatile hole contact materials is of great significance.
Herein, we report two novel donor–acceptor (D–A)-type
hole contact molecules (FMPA–BT-CA and 2FMPA–BT-CA)
with low cost and alcohol-based processability by utilizing a fluorination
strategy. We showed that the fluorine atoms lead to the lowered highest
occupied molecular orbital (HOMO) energy levels and larger dipole
moments for FMPA–BT-CA and 2FMPA–BT-CA. Moreover, fluorination
also improves the buried interfacial interaction between hole contacts
and perovskite. As a result, a remarkable power conversion efficiency
(PCE) of 22.37% along with good light stability could be achieved
for green-solvent-processed FMPA–BT-CA-based inverted PSC devices,
demonstrating the great potential of environmentally compatible hole
contacts for highly efficient PSCs