Elevated Efficiency and Stability of Hole-Transport-Layer-Free Perovskite Solar Cells Triggered by Surface Engineering

Surface engineering is one of the important strategies to enhance the power conversion efficiency (PCE) and stability of perovskite solar cells (PSCs). Herein, 2-chloro-1,3-dimethylimidazolidinium hexafluorophosphate (CIP) was introduced into PSCs to passivate the defects of the perovskite films. There are many F atoms in CIP molecules that have strong electronegativity and hydrophobicity. F groups can interact with Pb2+ defects, inhibit interface recombination, improve the interaction between the CIP ionic liquid and perovskite film, and reduce the defect density of perovskites, thus improving the stability of perovskite devices. Density functional theory calculation reveals that CIP can interact with uncoordinated Pb2+ in perovskites through coordination, reduce the defects of perovskite films, and inhibit nonradiation recombination. The ITO/SnO2/MAPbI3/CIP/carbon devices without hole transport layers possessed the highest PCE of 17.06%. Moreover, the unencapsulated device remains at 98.18% of the initial efficiency stored in 30–40% relative humidity for 850 h. This strategy provides an effective reference for enhancing the performance of PSCs.