Improving the Efficiency, Stability, and Adhesion of Perovskite Solar Cells Using Nanogel Additive Engineering

Additive engineering has been applied widely to improve the efficiency and/or stability of perovskite solar cells (PSCs). Most additives used to date are difficult to locate within PSCs as they are small molecules or linear polymers. In this work, we introduce, for the first time, carboxylic acid-functionalized nanogels (NGs) as additives for PSCs. NGs are swellable sub-100 nm gel particles. The NGs consist of poly(2-(2-methoxyethoxy) ethyl methacrylate)-co-methacrylic acid-co-ethylenegylcol dimethacrylate (PMEO₂MA-MAA-EGD) particles prepared by a scalable synthesis, which have a diameter of 40 nm. They are visualized in the perovskite films using SEM and are located at the grain boundaries. X-ray photoelectron and FTIR spectroscopy reveal that the NGs coordinate with Pb²⁺ via the -COOH groups. Including the NGs within the PSCs increased the grain size, decreased nonradiative recombination, and increased the power conversion efficiency (PCE) to 20.20%. The NGs also greatly increase perovskite stability to ambient storage, elevated temperature, and humidity. The best system maintained more than 80% of its original PCE after 180 days of storage under ambient conditions. Tensile cross-cut tape adhesion tests are used to assess perovskite film mechanical integrity. The NGs increased both the adhesion of the perovskite to the substrate and the mechanical stability. This study demonstrates that NGs are an attractive alternative to molecularly dispersed additives for providing performance benefits to PSCs. Our study indicates that the NGs act as a passivator, stabilizer, cross-linker, and adhesion promoter.