Localized Electron Density Engineering for Stabilized B-γCsSnI₃-Based Perovskite Solar Cells with Efficiencies >10%

Black orthorhombic (B-γ) CsSnI3 with low toxicity and excellent optoelectronic properties is a promising candidate for perovskite solar cell (PSC). However, the performance of the B-γCsSnI3-based PSCs is much lower than their lead-based or organotin-based counterparts due to the heavy self-doping of Sn2+ to form Sn4+ under ambient-air conditions. Here, this undesirable oxidation in CsSnI3 is restricted by engineering the localized electron density with phthalimide (PTM) additive. The lone electron pairs of NH and two CO units of PTM are designed to form trigeminal coordination bonding with Sn2+, resulting in reduced defect density and relatively grain-ordered perovskite film. The champion efficiencies of 10.1% and 9.6% are obtained for the modified rigid and flexible B-γCsSnI3-based PSCs, respectively. These encapsulated devices maintain 94.3%, 83.4%, and 81.3% of their initial efficiencies under inert (60 days), ambient (45 days), and 1 Sun continuous illumination at ∼70 °C (2000 min) conditions, respectively.