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Two‐dimensional perovskite solar cells (PSCs) with high moisture resistance are a key topic in the photovoltaic field. However, their lower power conversion efficiencies (PCEs) in comparison to 3 D PSCs is still an urgent problem to be solved. It is vital to understand the impact of constituent ratios and ammonium salt sizes on the photovoltaic performance and humidity stability. Based on the formula of (RNH3)2(MA)n−1PbnI3n+1 (n=1, 3, 5, 7, 9, and 11), a series of 2 D perovskites is prepared by introducing varisized ammonium salts of ethylammonium iodide (EAI), propylammonium iodide (PAI), and butylammonium iodide (BAI). The effects of the constituent ratios and varisized ammonium salts on the properties of the 2 D perovskites were studied. 2 D perovskite devices based on larger n and smaller ammonium salt size are found to exhibit better performances. However, the moisture resistance of the 2 D perovskite devices is higher when n is smaller and the ammonium salt size is larger. Therefore, the EA2MA10Pb11I34 (n=11) 2 D perovskite device displays the best photovoltaic performance, with the highest PCE of 16.93 %, whereas BA2MA2Pb3I10 (n=3) 2 D perovskite, with the largest contact angle of 79.8°, can retain over 85 % of the initial PCE after 1440 h aging at 50 % relative humidity. This work indicates the PCE and stability of 2 D perovskites can be conveniently and effectively adjusted by controlling the 2 D constituent ratios and ammonium salt sizes, so as to obtain efficient 2 D PSCs with high stability. [ABSTRACT FROM AUTHOR]

2D/3D Perovskites: Introduction of Hydrophobic Ammonium Salts with Halogen Functional Groups for High-Efficiency and Stable 2D/3D Perovskite Solar Cells (Adv. Funct. In article number 1807565, Xu Pan, Songyuan Dai, and co-workers design novel type 2D/3D perovskites by firstly introducing hydrophobic ammonium salt cations with halogen functional groups into 3D perovskite. Owing to the notable hydrophobicity of alkylammonium cations with halogen functional groups and the formed 2D/3D perovskite structure, the highly efficienct 2D/3D perovskite solar cells exhibit superior moisture resistance and thermal stability. [Extracted from the article]

2D perovskites have attracted extensive attention due to their excellent stability compared with 3D perovskites. However, the intrinsic hydrophilicity of introduced alkylammonium salts effects the humidity stability of 2D/3D perovskites. Devices based on longer chain alkylammonium salts show improvement in hydrophobicity but lower efficiency due to the poorer charge transport among various layers. To solve this issue, two hydrophobic short‐chain alkylammonium salts with halogen functional groups (2‐chloroethylamine, CEA+ and 2‐bromoethylamine, BEA+) are introduced into (Cs0.1FA0.9)Pb(I0.9Br0.1)3 3D perovskites to form 2D/3D perovskite structure, which achieve high‐quality perovskite films with better crystallization and morphology. The optimal 2D/3D perovskite solar cells (PSCs) with 5% CEA+ display a power conversion efficiency (PCE) as high as 20.08% under 1 sun irradiation. Because of the notable hydrophobicity of alkylammonium cations with halogen functional groups and the formed 2D/3D perovskite structure, the optimal PSCs exhibit superior moisture resistance and retain 92% initial PCE after aging at 50 ± 5% relative humidity for 2400 h. This work opens up a new direction for the design of new‐type 2D/3D PSCs with improved performance by employing proper alkylammonium salts with different functional groups. [ABSTRACT FROM AUTHOR]