Methylammonium‐Free Ink for Blade‐Coating of Pure‐Phase α‐FAPbI₃ Perovskite Films in Air

The α-c (α-FAPbI₃) has been extensively employed in the fabrication of high-efficiency perovskite solar cells, yet heavily relied on multiple additives in upscalable fabrication in air. In this work, a simple α-FAPbI₃ ink is developed for the blade-coating fabrication of phase-pure α-FAPbI₃ in ambient air free from any additives containing extrinsic ions. The introduction of 2-imidazolidinone (IMD) to the FAPbI₃ precursor inks leads to the formation of intermediate phases that change the phase transition pathway from δ-FAPbI₃ to α-FAPbI₃ by tilting the PbI₆ octahedrons with strong coordination to Pb²⁺. Furthermore, the IMD ligands in the intermediate phase gradually escape from the perovskite film during the annealing, leaving a phase-pure α-FAPbI₃ film vertically grown with large grains. Consequently, the small-sized PSCs fabricated with blade-coated α-FAPbI₃ film achieve an efficiency of up to 23.14%, and the corresponding mini-module yields an efficiency of 19.66%. The device performance is among the highest reported for phase-pure α-FAPbI₃ PSCs fabricated in the air without non-native cations or chloride additives, offering a simple and robust fabrication approach of phase-pure α-FAPbI₃ films for PV application.