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Electron transport layers (ETLs) are crucial for achieving efficient and stable planar perovskite solar cells (PSCs). Reports on versatile inorganic ETLs using a simple film fabrication method and applicability for both low‐cost planar regular and inverted PSCs with excellent efficiencies (>22%) and high stability are very limited. Herein, we employ a novel inorganic ZnSe as ETL for both regular and inverted PSCs to improve the efficiency and stability using a simple thermal evaporation method. The TiO2‐ZnSe‐FAPbI3 heterojunction could be formed, resulting in an improved charge collection and a decreased carrier recombination further proved through theoretical calculations. The optimized regular PSCs based on TiO2/ZnSe have achieved 23.25% efficiency with negligible hysteresis. In addition, the ZnSe ETL can also effectively replace the unstable bathocuproine (BCP) in inverted PSCs. Consequently, the ZnSe‐based inverted device realizes a champion efficiency of 22.54%. Moreover, the regular device comprising the TiO2/ZnSe layers retains 92% of its initial PCE after 10:00 h under 1 Sun continuous illumination and the inverted device comprising the C60/ZnSe layers maintains over 85% of its initial PCE at 85 °C for 10:00 h. This highlights one of the best results among universal ETLs in both regular and inverted perovskite photovoltaics. [ABSTRACT FROM AUTHOR]

Understanding the function of moisture on perovskite is challenging since the random environmental moisture strongly disturbs the perovskite structure. Here, we develop various N2-protected characterization techniques to comprehensively study the effect of moisture on the efficient cesium, methylammonium, and formamidinium triple-cation perovskite (Cs0.05FA0.75MA0.20)Pb(I0.96Br0.04)3. In contrast to the secondary measurements, the established air-exposure-free techniques allow us directly monitor the influence of moisture during perovskite crystallization. We find a controllable moisture treatment for the intermediate perovskite can promote the mass transportation of organic salts, and help them enter the buried bottom of the films. This process accelerates the quasi-solid-solid reaction between organic salts and PbI2, enables a spatially homogeneous intermediate phase, and translates to high-quality perovskites with much-suppressed defects. Consequently, we obtain a champion device efficiency of approaching 24% with negligible hysteresis. The devices exhibit an average T80-lifetime of 852 h (maximum 1210 h) working at the maximum power point. Perovskite structure is disturbed by environmental moisture, limiting the device performance. Here, Wei et al. monitor the effect of moisture during the growth by N2-protected characterization techniques, and obtain an operationally stable perovskite solar cell with efficiency approaching 24%. [ABSTRACT FROM AUTHOR]