Multifunctional Metal‐Organic Frameworks Capsules Modulate Reactivity of Lead Iodide toward Efficient Perovskite Solar Cells with UV Resistance

Abstract The two‐step sequential deposition process is demonstrated as a reliable technology for the fabrication of efficient perovskite solar cells (PVSCs). However, the complete conversion of dense PbI₂ to perovskite in planar PVSCs is tough without mesoporous titanium dioxide as support. Herein, multifunctional capsules consisting of zeolitic imidazolate framework‐8 (ZIF‐8) encapsulant and formamidinium iodide (FAI) are introduced between tin oxide (SnO₂) and lead iodide (PbI₂) layer. Intriguingly, the capsule dopant interlayer benefits the formation of porous PbI₂ film due to the porous nanostructure of ZIF‐8 that is favorable for the subsequent intercalation reaction. Furthermore, the constituent of the perovskite precursor in ZIF‐8 pores can convert into the crystal nuclei of perovskite by reacting with PbI₂ first, thereby promoting further perovskite crystallization. Significantly, the incorporation of ZIF‐8 can enhance the resistance of perovskite against UV illumination due to down‐conversion effect. Consequently, the modified device achieves a champion power conversion efficiency (PCE) of 24.08% and displays enhanced UV stability, which can sustain 83% of its original PCE under 365 nm UV illumination for 300 h. Moreover, the unencapsulated device maintains 90% of initial PCE after 1500 h storage in dark ambient conditions with a relative humidity range of 50%–70%.