Decoupling cation segregation and volatile loss in formamidinium–caesium metal halide perovskite solar cells under high-temperature operating conditions
摘要
Formamidinium–caesium lead iodide (FAXCs1-XPbI3, 0 < x < 1) perovskites are pivotal for commercialization of perovskite solar cells owing to their superior stability. However, their upper stability limits under combined thermal and light stressors remain poorly understood. Through Arrhenius analysis of hundreds of p–i–n devices, we reveal two distinct degradation regimes: below 106 °C, cation segregation dominates, whereas above 106 °C, FAI loss dominates perovskite decomposition. Incorporating a compact tin oxide (SnO2) layer effectively suppresses FAI loss, maintaining cation-segregation-dominated degradation beyond 106 °C. Moreover, introducing trace CsI3 in perovskite precursor enhances cation homogeneity in as-prepared films, dramatically extending the device T90 (time to 90% of maximum efficiency) to ~2,700 h under continuous 1-sun illumination (1.0% UV) at 85 °C. The extrapolated T90 at 45 °C exceeds 50 years by assuming a same degradation pathway. These findings elucidate the temperature-dependent degradation pathways in formamidinium–caesium perovskites and provide practical strategies to enhance their operational stability.