High‐Pressure Nitrogen‐Extraction and Effective Passivation to Attain Highest Large‐Area Perovskite Solar Module Efficiency

Slot-die coating holds advantages over other large-scale technologies thanks to its potential for well-controlled, high-throughput, continuous roll-to-roll fabrication. Unfortunately, it is challenging to control thin.film uniformity over a large area while maintaining crystallization quality. Herein, by using a high-pressure nitrogen-extraction (HPNE) strategy to assist crystallization, a wide processing window in the well-controlled printing process for preparing high-quality perovskites is achieved. The yellow-phase perovskite generated by the HPNE acts as a crucial intermediate phase to produce large-area high-quality perovskite film. Furthermore, an ionic liquid is developed to passivate the perovskite surface to reduce surface defect density and to suppress carrier recombination, resulting in significantly increased efficiency to 22.7%, the highest for large-area fabrication. The strategies are successfully extended to large-area device fabrication, making it possible to produce a 40 × 40 mm2 module with stabilized PCE as high as 19.4%, the highest-efficiency for a large-area module to date.