Orientation Regulation of Phenylethylammonium Cation Based 2D Perovskite Solar Cell with Efficiency Higher Than 11%

Increasing the power conversion efficiency (PCE) of the two-dimensional (2D) perovskite-based solar cells (PVSCs) is really a challenge. Vertical orientation of the 2D perovskite film is an efficient strategy to elevate the PCE. In this work, vertically orientated highly crystalline 2D (PEA)2(MA)n-1PbnI3n+1 (PEA= phenylethylammonium, MA = methylammonium, n = 3, 4, 5) films are fabricated with the assistance of an ammonium thiocyanate (NH4SCN) additive by a one-step spin-coating method. Planar-structured PVSCs with the device structure of indium tin oxide (ITO)/poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)/(PEA)2(MA)n-1PbnI3n+1/[6,6]-phenyl-C61-butyric acid methyl ester/bahocuproine/Ag are fabricated. The PCE of the PVSCs is boosted from the original 0.56% (without NH4SCN) to 11.01% with the optimized NH4SCN addition at n = 5, which is among the highest PCE values for the low-n (n < 10) 2D perovskite-based PVSCs. The improved performance is attributed to the vertically orientated highly crystalline 2D perovskite thin films as well as the balanced electron/hole transportation. The humidity stability of this oriented 2D perovskite thin film is also confirmed by the almost unchanged X-ray diffraction patterns after 28 d exposed to the moisture in a humidity-controlled cabinet (Hr = 55 ± 5%). The unsealed device retains 78.5% of its original PCE after 160 h storage in air atmosphere with humidity of 55 ± 5%. The results provide an effective approach toward a highly efficient and stable PVSC for future commercialization.