Spontaneous Formation of Upper Gradient 2D Structure for Efficient and Stable Quasi-2D Perovskites

Highly efficient and stable quasi-2D hybrid perovskite solar cells (PSCs) using hydrophobic 4-(trifluoromethyl) benzylamine (4TFBZA) as the spacer cation are successfully demonstrated. It is found that the incorporation of hydrophobic 4TFBZA into MAPbI₃ can effectively induce a spontaneous upper gradient 2D (SUG-2D) structure, passivate the trap states, and restrain the ion motion. Meanwhile, the strong hydrogen bonding of F···HN between 4TFBZA ions and methylamine ions can effectively suppress the decomposition of perovskite, which gives the device a better thermal stability. Besides, due to the SUG-2D structure with hydrophobic 4TFBZA, the device also exhibits a better moisture stability. The SUG-2D-structure-based device exhibits a power conversion efficiency of 17.07% with a high open-circuit voltage of 1.10 V and a notable fill factor of 71%. This work provides a new strategy for constructing efficient and stable quasi-2D PSCs, and it is an inspiration for the packaging strategy of perovskites.