Enhancing Performance and Stability of Sn–Pb Perovskite Solar Cells with Oriented Phenyl-C61-Butyric Acid Methyl Ester Layer via High-Temperature Annealing

Phenyl-C₆₁-butyric acid methyl ester (PCBM) can be used as a passivation material in perovskite solar cells (PeSCs) in order to reduce the trap site of the perovskite. Here, we show that a thick PCBM layer can form a smoother surface on the SnO₂ substrate, improving the grain size and reducing the microstrain of the perovskite. High-temperature annealing treatment of PCBM layer not only increases its solvent resistance to perovskite precursor or antisolvent, but also enhances its molecular alignment, resulting in improved conductivity as an electron transport layer. High-temperature annealed PCBM (HT-PCBM) effectively minimizes trap-assisted nonradiative recombination by reducing trap density in perovskite and improving the electrical properties at the interface between SnO₂ and perovskite layers. This HT-PCBM process significantly enhances the performance of the PeSCs, including the open-circuit voltage (V_OC) from 0.39 to 0.77 V, fill factor from 52% to 65%, and power conversion efficiency (PCE) from 6.03% to 15.50%, representing substantial improvements compared to devices without PCBM. This PCE is the highest efficiency among conventional (n-i-p) Sn-Pb PeSCs reported to date. Moreover, passivating the trap sites of SnO₂ and separating the interface between the Sn-containing perovskite and the substrate effectively have improved the stability of the Sn-Pb perovskite in the n-i-p structure. The optimized best device with HT-PCBM has maintained an efficiency of over 90% for more than 300 h at 85 °C and 5000 h at room temperature in a glovebox atmosphere.