Antisolvent‐Free Fabrication of Efficient and Stable Sn–Pb Perovskite Solar Cells

Pb‐based perovskite solar cells (PSCs) have shown great potential in next‐generation photovoltaics. However, the toxicity of Pb remains a big concern. Partial replacement of Pb with Sn is shown to reduce the toxicity of PSCs without considerably compromising the device performance. Currently, Sn–Pb single‐junction PSCs have realized a champion power conversion efficiency (PCE) of 21.7%, whereas all perovskite tandem PSCs with a Pb–Sn device as the bottom cell have achieved a PCE of 25.5%. However, the fabrication process of Sn–Pb PSCs is still not ecofriendly due to the use of hazardous organic solvents and antisolvents. Herein, for the first time, a one‐step antisolvent‐free method is developed to fabricate a high‐quality Sn–Pb perovskite film using methylammonium acetate (MAAc) ionic liquid as a green solvent. The crucial effects of multiple organic halides (MOHs) on the crystallization process and characteristics of the Sn–Pb film are comprehensively investigated. After optimizing the film fabrication parameters, PSCs with a champion PCE of 15.42% can be achieved. Moreover, the device exhibits robust stability that shows negligible PCE loss after being stored in N 2 for 720 h. A new avenue to promote the ecofriendly fabrication of efficient Sn–Pb PSCs is opened up.