Inhibiting Ion Migration Through Chemical Polymerization and Chemical Chelation Toward Stable Perovskite Solar Cells

The migration of ions is known to be associated with various detrimental phenomena, including current density‐voltage hysteresis, phase segregation, etc., which significantly limit the stability and performance of perovskite solar cells, impeding their progress toward commercial applications. To address these challenges, we propose incorporating a polymerizable organic small molecule monomer, N‐carbamoyl‐2‐propan‐2‐ylpent‐4‐enamide (Apronal), into the perovskite film to form a crosslinked polymer (P‐Apronal) through thermal crosslinking. The carbonyl and amino groups in Apronal effectively interact with shallow defects, such as uncoordinated Pb2+ and iodide vacancies, leading to the formation of high‐quality films with enhanced crystallinity and reduced lattice strain. Furthermore, the introduction of P‐Apronal improves energy level alignment, and facilitates charge carrier extraction and transport, resulting in a champion efficiency of 25.09 %. Importantly, P‐Apronal can effectively suppress the migration of I− ions and improve the long‐term stability of the devices. The present strategy sets forth a path to attain long‐term stability and enhanced efficiency in perovskite solar cells. A polymerizable organic molecule monomer, N‐carbamoyl‐2‐propan‐2‐ylpent‐4‐enamide (Apronal), is introduced into the perovskite precursor to form a polymer (P‐Apronal) through thermal crosslinking, which can effectively interact with shallow defects, leading to enhance crystallinity and reduced lattice strain, especially inhibiting the migration of I−, thus resulting in enhanced long‐term stability and performance of devices.