Boosting MA-based two-dimensional Ruddlesden-Popper perovskite solar cells by incorporating a binary spacer

Two-dimensional Ruddlesden-Popper (2DRP) perovskite exhibits excellent stability in perovskite solar cells (PSCs) due to introducing hydrophobic long-chain organic spacers. However, the poor charge transporting property of bulky organic cation spacers limits the performance of 2DRP PSCs. Inspired by the A-site cation alloying strategy in 3D perovskites, 2DRP perovskites with a binary spacer can promote charge transporting compared to the unary spacer counterparts. Herein, the superior MA-based 2DRP perovskite films with a binary spacer, including 3-guanidinopropanoic acid (GPA) and 4-fluorophenethylamine (FPEA) are realized. These films (GPA_0.85FPEA_0.15)₂MA₄Pb₅I₁₆ show good morphology, large grain size, decreased trap state density, and preferential orientation of the as-prepared film. Accordingly, the present 2DRP-based PSC with the binary spacer achieves a remarkable efficiency of 18.37% with a V_OC of 1.15 V, a J_SC of 20.13 mA cm⁻², and an FF of 79.23%. To our knowledge, the PCE value should be the highest for binary spacer MA-based 2DRP (n ≤ 5) PSCs to date. Importantly, owing to the hydrophobic fluorine group of FPEA and the enhanced interlayer interaction by FPEA, the unencapsulated 2DRP PSCs based on binary spacers exhibit much excellent humidity stability and thermal stability than the unary spacer counterparts.