Managing Secondary Phase Lead Iodide in Hybrid Perovskites via Surface Reconstruction for High-Performance Perovskite Solar Cells with Robust Environmental Stability

Rationally managing the secondary-phase excess lead iodide (PbI₂) in hybrid perovskite is of significance for pursuing high performance perovskite solar cells (PSCs), while the challenge remains on its conversion to a homogeneous layer that is robust stable against environmental stimuli. We herein demonstrate an effective strategy of surface reconstruction that converts the excess PbI₂ into a gradient lead sulfate-silica bi-layer, which substantially stabilizes the perovskite film and reduces interfacial charge transfer barrier in the PSCs device. The perovskite films with such bi-layer could bear harsh conditions such as soaking in water, light illumination at 70 % relative humidity, and the damp-thermal (85 °C and 30 % humidity) environment. The resulted PSCs deliver a champion efficiency up to 24.09 %, as well as remarkable environmental stability, e.g., retaining 78 % of their initial efficiency after 5500 h of shelf storage, and 82 % after 1000 h of operational stability testing.