Efficient Carbon‐Based Hole‐Conductor‐Free Printable Mesoscopic Perovskite Solar Cells via a Multifunctional Fluorinated Molecule

Abstract Benefiting from their simple and cost‐effective fabrication procedures, printable mesoscopic perovskite solar cells (p‐MPSCs) exhibit substantial potential for large‐scale production. In p‐MPSCs, the thickness of the perovskite filled in the TiO₂ and ZrO₂ mesoporous layers is ≈3 µm. Therefore, the perovskite crystallization process is more intricate and challenging in the mesoporous structure than the general planar thin film (0.3–0.5 µm). In this work, a multifunctional fluorinated molecule is applied to work as an additive to improve the perovskite crystallization, enhance the device efficiency, and elevate the operational stability. This additive forms robust coordination between its carbonyl groups and uncoordinated Pb²⁺, thereby effectively passivating defects. The hydrophobic properties of the fluorinated molecule contribute to the device's water‐resistant capability and long‐term operational stability. With these synergistic effects, the power conversion efficiency (PCE) of small‐area cells (0.1 cm²) reaches 20.15% under 1 sun illumination. Large‐area modules (56.4 cm²) are fabricated and exhibit a PCE of 15.41%.