Buried Interface Engineering for Scalable Processing of High‐Performance Inverted Perovskite Solar Modules

Abstract Achieving high efficiency over large areas remains a significant bottleneck in commercializing perovskite solar cells (PSCs). Recent advancements in passivation technology, especially using self‐assembled monolayers (SAMs) to address buried interface defects, have been instrumental in boosting the efficiency of PSCs. However, SAMs' compactness, uniformity, and wettability are crucial factors influencing the quality of perovskite films. This study presents a buried interface layer based on NiO x /mesoporous Al 2 O 3 sponge as a carrier for SAM solution adsorption, combined with a dip coating process, successfully developing a large‐area preparation technology for SAM layers. The results indicate that the compact SAM layer deposited by this approach effectively passivates buried interface defects on a large scale, while the enhanced wettability of the Al 2 O 3 layer aids in eliminating interfacial voids. The modified PSCs with an active area of 0.09 cm 2 achieve a power conversion efficiency (PCE) of 25.46%. The device attains a champion PCE of 22.66%, marking one of the highest efficiencies reported for p‐i‐n PSMs prepared via large‐area coating in mini‐modules (10–200 cm 2 ) under air ambient conditions. Moreover, encapsulated devices retain 93.8% of their initial PCE after 1000 h of continuous operation under one‐sun equivalent intensity at 65 °C in an air environment.