Balancing crystallization rate in a mixed Sn–Pb perovskite film for efficient and stable perovskite solar cells of more than 20% efficiency

Abstract

In the journey to obtain well-crystallized mixed tin (Sn)–lead (Pb) iodide perovskite films for solar cell application, great difficulties have been presented due to very different crystallization rates between Sn- and Pb-based perovskite components. Herein, we report a new strategy to grow highly crystallized Sn–Pb perovskite (FA_0.7MA_0.3Sn_0.5Pb_0.5I₃) for perovskite solar cells (PSCs). An iso-pentylammonium tetrafluoroborate ([PNA]BF₄) ionic salt layer is introduced on top of poly(3,4-ethylenedioxythiophene)-poly-(styrenesulfonate) (PEDOT:PSS) to function as anchoring agent to bond Pb²⁺ to the surface of PEDOT:PSS, which can facilitate a quick crystallization of Pb-containing perovskite components and homogeneously distribute Sn/Pb elements inside the perovskite film in a vertical direction, uncovered by focused ion beam time-of-flight secondary ion mass spectrometry. Additionally, greatly reduced surface residual stress was also confirmed by X-ray diffraction. Lastly, these ionic salt molecules are able to encapsulate the acidic and hygroscopic surface of PEDOT:PSS to further ensure device stability. As a result, our strategies enabled a champion PCE of 20.11% for mixed Sn–Pb PSCs with improved thermal stability at 85 °C over 240 hours and shelf storage stability over 1200 hours. This work provides a new strategy to regulate the crystallization process of mixed Sn–Pb perovskites for both high performance and stability.