Suppressed Voltage Deficit and Degradation of Perovskite Solar Cells by Regulating the Mineralization of Lead Iodide

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 quality of perovskite film. The interplay of size effect and adequate bonding strength between 3‐AzTca and uncoordinated Pb2+ regulates the mineralization of PbI2 and generates low‐dimensional PbI2 phase, thereby boosting the crystallization of perovskite. The decreased defect states result in suppressed nonradiative recombination and reduced VOC loss. The power conversion efficiency (PCE) of modified PSC is improved to 22.79% with a high VOC of 1.22 V. Moreover, the decomposition of PbI2 and perovskite films is also retarded, yielding enhanced device stability. This study provides an effective method to minimize the concentration of uncoordinated Pb2+ and improve the PCE and stability of PSCs. The introduction of 3‐AzTca regulates the mineralization of PbI2 and perovskite by strengthening the metallic Pb frame, thereby reducing the defects and improving the environmental stability of PbI2 and perovskite film. The champion perovskite solar cell achieves a low voltage deficit of 0.37 V, an efficiency of 22.79%, and enhanced stability.