The development of anti-solvent free, scalable and printable perovskite film is crucial to realizing the low-cost roll-to-roll development of perovskite solar cells (PSCs). Herein, we explored large-area perovskite film fabrication using a spray-assisted sequential deposition technique. We investigated how propylene carbonate (PC) solvent additive affects the transformation of PbI2 into perovskite at room temperature. Our result shows that PC-modified perovskite films exhibit a uniform, pinhole-free morphology with oriented grains compared with pristine perovskite films. The PC-modified perovskite film also has a prolonged fluorescence lifetime that indicates lower carrier recombination. The champion PSC devices based on PC-modified perovskite film realized a power conversion efficiency (PCE) of 20.5% and 19.3% at an active area (A) of 0.09 cm2 and 1 cm2, respectively. The fabricated PSCs are stable and demonstrated >85% PCE retention following 60 days of exposure to ambient conditions. Furthermore, we fabricated perovskite solar modules (A ~13 cm2) that yielded a PCE of 15.8%. These results are among the best reported for the state-of-art spray-coated PSCs. Spray deposition coupled with a PC additives is highly promising for economical and high-output preparation of PSCs.

https://doi.org/10.1002/smtd.202300237