Highly Efficient and Stable Perovskite Solar Cells Incorporating Chlorinated-Tin Oxide Electron Transport Layers Prepared via Coordination of Diacyl-Metal Cations

The surface passivation of metal oxide electron-transport layers (ETLs) is a powerful strategy for realizing high-performance perovskite solar cells. The surface properties of ETLs strongly influence carrier injection and transfer dynamics; therefore, control of the carrier trap density is crucial. Semiconducting small molecules are considered suitable materials for surface passivation. However, they are expensive and vulnerable to humid atmospheres. Ultrathin polymer layers can have poor surface coverage owing to their spinodal dewetting. In this study, we employ adipoyl chloride as an organic ligand for the chemically robust and efficient surface passivation of SnO 2 ETLs. Through the strong coordination of diacyl-metal cations, acyl groups are adsorbed onto the SnO 2 surfaces, and the density of oxygen vacancies is significantly reduced. Furthermore, the changing surface properties of the SnO 2 ETLs also contribute to the improvement of perovskite morphologies. The deeper energy levels and reduced defect density of the ETLs promote electron injection and transfer at the perovskite and ETL interface. The enlarged perovskite grains are accompanied by improved electron mobility and reduced grain-boundary density. The resulting power conversion efficiency (PCE) increases from 19.36 to 21.41%. The normalized PCE is retained at 90.4% of the initial value for 720 h under 1 sun illumination without the encapsulation of the devices.