Multidentate Coordination Induced Crystal Growth Regulation and Trap Passivation Enables over 24% Efficiency in Perovskite Solar Cells

Abstract Crystal growth regulation has become an effective solution to reduce the defects at grain boundaries (GBs) and surfaces of perovskite films for better photovoltaic performances. Oxime acid materials are maturely used as selective collectors in the flotation separation of oxide minerals. Such materials, showing a strong coordination effect and high selectivity with lead, may have great potential in controlling the crystal growth and passivating the defect of perovskite film, which are rarely applied in perovskite solar cells (PerSCs). Herein, an oxime acid‐based material with multi‐coordination sites, ethyl 2‐(2‐aminothiazole‐4‐yl)‐2‐hydroxyiminoacetate (EHA), is incorporated into the PbI₂ precursor solution to fabricate high‐performance PerSCs using a two‐step method. The multidentate coordination effect of EHA can link and integrate the PbI₂ colloidal clusters to achieve pre‐aggregation in the PbI₂ precursor solution, facilitating the sequent crystal growth progress of perovskite film. Meanwhile, EHA can connect grains and fill GBs, which is favorable for charge transfer and passivating both Pb‐I anti‐site and iodine vacancy defects. As a result, the optimal devices show an enhanced efficiency of 24.1% and excellent humidity and thermal stability. This work affords a promising strategy to fabricate efficient and stable PerSCs via multidentate coordination‐induced crystallization control and GB passivation.