2D Polymers with Lead Anchoring Groups Enable Perovskite Solar Cells with Over 24% Efficiency

The hygroscopic dopants used in Spiro‐OMeTAD hole‐transport materials (HTMs) in n –i– p perovskite solar cells (PSCs) inevitably cause device degradation. Herein, two polymer interface materials based on lead anchoring groups are developed. It is found that 2D polymers 2DP‐BT and 2DP‐Por can form dense films and exhibit excellent hydrophobicity. Importantly, 2DP‐Por can passivate the surface defects through noncovalent interactions, reducing nonradiative recombination loss. After introducing these polymer interface materials between the perovskite layer and the HTM layer, the optimized devices using 2DP‐Por and 2DP‐BT achieve champion power conversion efficiency of 24.12% and 23.29%, respectively, and the stability is significantly improved. These results indicate that developing polymer interface materials containing lead anchoring groups can improve PSC efficiency and stability and elucidate critical molecular design rules for interface materials.