Carboxylic Acid-Assisted Synthesis of Tin(II) Iodide: Key for Stable Large-Area Lead-Free Perovskite Solar Cells

Despite significant progress in tin-based perovskites, the development of stable and high-performance tin-based perovskite solar cells (TPSCs) remains a challenge. In this pursuit, a multitude of strategies have been explored, encompassing the use of reducing agents, antioxidants, bulky cations, and customized solvent systems. We propose an improved approach for synthesizing SnI2 from elemental tin and iodine. Here, we generate tin nanoparticles grafted with a carboxylic acid in situ from tin powder–carboxylic acid-assisted synthesis (CAAS). This methodology not only improves the synthesis process of SnI2 but also enhances precursor stability against oxidation. We use 119Sn MAS NMR to study the atomic-level structure of the resulting FASnI3 thin films and find that the CAAS approach leads to highly pure and unoxidized material. We report remarkable reproducibility in fabricating large-area (1 cm2) flexible TPSCs with significant improvement in open-circuit voltage leading to the champion device showing a power conversion efficiency of 8.35%.