Blading Phase‐Pure Formamidinium‐Alloyed Perovskites for High‐Efficiency Solar Cells with Low Photovoltage Deficit and Improved Stability

Currently, blade-coated perovskite solar cells (PSCs) with high power conversion efficiencies (PCEs), that is, greater than 20%, normally employ methylammonium lead tri-iodide with a sub-optimal bandgap. Alloyed perovskites with formamidinium (FA) cation have narrower bandgap and thus enhance device photocurrent. However, FA-alloyed perovskites show low phase stability and high moisture sensitivity. Here, it is reported that incorporating 0.83 molar percent organic halide salts (OHs) into perovskite inks enables phase-pure, highly crystalline FA-alloyed perovskites with extraordinary optoelectronic properties. The OH molecules modulate the crystal growth, enhance the phase stability, passivate ionic defects at the surface and/or grain boundaries, and enhance the moisture stability of the perovskite film. A high efficiency of 22.0% under 1 sun illumination for blade-coated PSCs is demonstrated with an open-circuit voltage of 1.18 V, corresponding to a very small voltage deficit of 0.33 V, and significantly improved operational stability with 96% of the initial efficiency retained under one sun illumination for 500 h.