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Both the uncoordinated Pb2+ and excess PbI2 in perovskite film will create defects and perturb carrier collection, thus leading to the open‐circuit voltage (VOC) loss and inducing rapid performance degradation of perovskite solar cells (PSCs). Herein, an additive of 3‐aminothiophene‐2‐carboxamide (3‐AzTca) that contains amide and amino and features a large molecular size is introduced to improve the...