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 (FA0.7MA0.3Sn0.5Pb0.5I3) 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.