Metal oxide carrier transporting layers have been investigated widely in organic/inorganic lead halide perovskite solar cells (PSCs). Tin oxide (SnO2) is a promising alternative to the titanium dioxide commonly used in the electron transporting layer (ETL), due to its tunable carrier concentration, high electron mobility, amenability to low-temperature annealing processing, and large energy bandgap. In this study, a facile method was developed for the preparation of a room-temperature-processed SnO2 electron transporting material that provided a high-quality ETL, leading to PSCs displaying high power conversion efficiency (PCE) and stability. A novel physical ball milling method was first employed to prepare chemically pure ground SnO2 nanoparticles (G-SnO2), and a sol–gel process was used to prepare a compact SnO2 (C-SnO2) layer. The effects of various types of ETLs (C-SnO2, G-SnO2, composite G-SnO2/C-SnO2) on the performance of the PSCs are investigated. The composite SnO2 nanostructure formed a robust ETL having efficient carrier transport properties; accordingly, carrier recombination between the ETL and mixed perovskite was inhibited. PSCs incorporating C-SnO2, G-SnO2, and G-SnO2/C-SnO2 as ETLs provided PCEs of 16.46, 17.92, and 21.09%, respectively. In addition to their high efficiency, the devices featuring the composite SnO2 (G-SnO2/C-SnO2) nanostructures possessed excellent long-term stability—they maintained 89% (with encapsulation) and 83% (without encapsulation) of their initial PCEs after 105 days (>2500 h) and 60 days (>1400 h), respectively, when stored under dry ambient air (20 ± 5 RH %).
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