If perovskite solar cells (PSCs) with high power conversion efficiencies (PCEs) are to be commercialized, they must achieve long-term stability, which is usually assessed with accelerated degradation tests. One of the persistent obstacles for PSCs has been successfully passing the damp-heat test (85°C and 85% relative humidity), which is the standard for verifying the stability of commercial photovoltaic (PV) modules. We fabricated damp heat–stable PSCs by tailoring the dimensional fragments of two-dimensional perovskite layers formed at room temperature with oleylammonium iodide molecules; these layers passivate the perovskite surface at the electron-selective contact. The resulting inverted PSCs deliver a 24.3% PCE and retain >95% of their initial value after >1000 hours at damp-heat test conditions, thereby meeting one of the critical industrial stability standards for PV modules.

To produce mesoscopic carbon-electrode-based solar cells free of a hole-conduction layer, we developed a simple one-step drop-cast method (temperature 20 °C, relative humidity 50%) to grow uniform and compact perovskite nanocrystals via slow crystallization (SC). X-ray diffraction (XRD) results indicated that perovskite nanocrystals produced inside the mesoporous TiO₂/Al₂O₃/C layers according to our SC approach with N-methyl-2-pyrrolidone (NMP) as a precursor solvent showed a preferred orientation at facet (004) with large crystalline grains, whereas those produced with other solvents or via thermal annealing (TA) methods showed greater intensity at facet (220) with small crystals. After the SC (NMP) procedure was completed, additional TA treatment would change the preferred orientation from (004) back to facet (220), which would break the connectivity and lose the uniformity of the crystals, causing the grains to become significantly smaller. Transient photoluminescence (PL) decay profiles of the SC devices made with four precursor solvents, NMP, γ-butyrolactone (GBL), dimethylformamide (DMF) and dimethyl sulfoxide (DMSO), were recorded to show the trend of charge separation kinetics of the perovskite crystals inside the mesoporous films, which is consistent with the trend of the corresponding device performance showing the same order. The SC (NMP) device attained the best efficiency of power conversion (PCE), 15.0%, with average value (13.9 ± 0.5%), which is much superior to those devices from either the traditional one-step TA (DMF) method (5.2 ± 1.0%) or the traditional sequential TA method (10.1 ± 0.7%). This work emphasizes the significance of the control of preferred orientation of perovskite nanocrystals using the SC approach, to obtain high-performance carbon-based mesoscopic solar cells with excellent reproducibility and stability.