Promoting Large-Area Slot-Die-Coated Perovskite Solar Cell Performance and Reproducibility by Acid-Based...

Homogeneous and pinhole-free large-area perovskite films are required to realize the commercialization of perovskite modules and panels. Various large-area perovskite coatings were developed; however, at their film coating and drying stages, many defects were formed on the perovskite surface. Consequently, not only the devices lost substantial performance but also their long-term stability deteriorated. Here, we fabricated a compact and uniform large-area MAPbI₃-perovskite film by a slot-die coater at room temperature (T) and at high relative humidity (RH) up to 40%. The control slot-die-coated perovskite solar cell (PSC) produced 1.082 V open-circuit voltage (V_oc), 24.09 mA cm^-2 short current density (J_sc), 71.13% fill factor (FF), and a maximum power conversion efficiency (PCE) of 18.54%. We systematically employed a multi-functional artificial amino acid (F-LYS-S) to modify the perovskite defects. Such amino acids are more inclined to bind and adhere to the perovskite defects. The amino, carbonyl, and carboxy functional groups of F-LYS-S interacted with MAPbI₃ through Lewis acid-base interaction and modified iodine vacancies significantly. Fourier transform infrared spectroscopy revealed that the C═O group of F-LYS-S interacted with the uncoordinated Pb²⁺ ions, and X-ray photoelectron spectroscopy revealed that the lone pair of -NH₂ coordinated with the uncoordinated Pb²⁺ and consequently modified the I^- vacancies remarkably. As a result, the F-LYS-S-modified device demonstrated more than three-fold charge recombination resistance, which is one of the primary requirements to fabricate high-performance PSCs. Therefore, the device fabricated employing F-LYS-S demonstrated remarkable PCE of 21.08% with superior photovoltaic parameters of 1.104 V V_oc, 24.80 mA cm^-2 J_sc, and 77.00%. FF. Concurrently, the long-term stability of the PSCs was improved by the F-LYS-S post-treatment, where the modified device retained ca. 89.6% of its initial efficiency after storing for 720 h in air (T ∼ 27 °C and RH ∼ 50-60%).