Stable Perovskite Solar Cells with Bulk-Mixed Electron Transport Layer by Multifunctional Defect Passivation

Multifarious electron transport layers (ETLs), especially fullerene derivatives, have been applied in organic-inorganic hybrid perovskite (OIHP) devices owing to their superior optoelectronic properties. However, a PCBM Lewis acid molecule can only passivate the iodine-rich defect sites, which cannot solve the problem of uncoordinated Pb²⁺ and water oxygen erosion due to the high volatility of halide I^- and the hydrophilicity of organic cation MA⁺. Herein, we introduce a Lewis base, TBA-Azo with an electron-donating Azo moiety, and hydrophobic long alkyl chains into the PCBM layer to form a multifunctional bulk-mixed electron transport layer (MBE). PCBM of MBE can combine with iodine-rich trap sites at the surface and grain boundaries of perovskite. TBA-Azo molecules of MBE can passivate uncoordinated Pb²⁺ by forming Lewis adducts and isolate water/oxygen at the perovskite surface with hydrophobic alkyl chains. It results in a decrease of trap densities with 1 order of magnitude, effectively inhibiting both bimolecular and trap-induced recombination and thus elongating the carrier lifetime. The passivation of MBE can effectively improve the open-circuit voltage from 1.05 to 1.10 V. Furthermore, three long carbon chain structures of TBA-Azo in MBE can improve the water-resistant ability of OIHP devices, which can maintain 90% of the original PCE after 500 h at the humidity of 50 ± 10%. We believe that the MBE with multifunctional defect passivation provides a strategy for simultaneously achieving high-performance and high-stability OIHP optoelectronic devices.