A High‐Throughput Approach to Identifying Environment‐Friendly Artificial Antisolvents for Efficient Perovskite Solar Cells

Abstract Rapid crystallization facilitated by antisolvents is widely employed for producing high‐quality perovskite films, but constrained by the limited variety and high toxicity of conventional solvents, underscoring the need for sustainable and low‐toxicity solvent systems for large‐scale production. In this study, a systematic screening of over 40 antisolvents is conducted using a high‐throughput platform, uncovering a significant correlation between the antisolvent properties within Hansen solubility space and the structural and optoelectronic characteristics of the resultant perovskite films. A Hansen solubility sphere is subsequently constructed, pinpointing a specific region within this space that is most conducive to the formation of high‐quality perovskite films. The underlying mechanism is further elucidated: antisolvents situated outside this optimal region either induce a rapid extraction of N,N‐dimethylformamide (DMF), thereby limiting grain growth due to insufficient crystallization time or fail to adequately extract DMF. Since no ideal low‐toxicity single antisolvent is found, a general concept based on solvent combinations with ultra‐low‐toxicity is introduced to solve the issues. The design rule for environment‐friendly “artificial” solvents, which is validated for different perovskite compositions, paves the way for sustainable development and production of perovskite‐based optoelectronic technologies.