Carrier Modulation via Tunnel Oxide Passivating at Buried Perovskite Interface for Stable Carbon-Based Solar Cells

Carbon-based perovskite solar cells (C-PSCs) have the impressive characteristics of good stability and potential commercialization. The insulating layers play crucial roles in charge modulation at the buried perovskite interface in mesoporous C-PSCs. In this work, the effects of three different tunnel oxide layers on the performance of air-processed C-PSCs are scrutinized to unveil the passivating quality. Devices with ZrO₂-passivated TiO₂ electron contacts exhibit higher power conversion efficiencies (PCEs) than their Al₂O₃ and SiO₂ counterparts. The porous feature and robust chemical properties of ZrO₂ ensure the high quality of the perovskite absorber, thus ensuring the high repeatability of our devices. An efficiency level of 14.96% puts our device among the state-of-the-art hole-conductor-free C-PSCs, and our unencapsulated device maintains 88.9% of its initial performance after 11,520 h (480 days) of ambient storage. These results demonstrate that the function of tunnel oxides at the perovskite/electron contact interface is important to manipulate the charge transfer dynamics that critically affect the performance and stability of C-PSCs.