Ion-Mediated Molecular Bridging at Buried Interface Enhances Perovskite Solar Cell Durability

Engineering heterointerfaces via molecular bridging has been crucial for achieving perovskite solar cells (PSCs) featuring optimal power conversion efficiencies (PCEs) and environmental durability. However, the challenge remains in ensuring interfacial mechanical reliability to enhance the long-term durability of PSCs. Herein, an ion-mediated molecular bridging strategy is intentionally exploited to improve the mechanical integrity between the perovskite bottom and electron-transport layers (ETLs) through balancing interfacial toughness and strength. As a demonstration of the concept, a zwitterionic guanylurea phosphate additive is preburied onto the SnO₂ ETL, in which the guanylurea with bifacial NH₂ groups servers as a molecular bridge connecting the perovskite and ETL through electrostatic coupling, while the phosphate can interact with charged species at the heterointerface to strengthen the mechanical contact. Benefiting from the robust heterointerfaces, the mechanical durability of flexible PSCs is significantly enhanced, retaining 91.3% of the original efficiency following 6000 bending cycles (bending radius = 3 mm). Additionally, the enhanced mechanical integrity at the buried interface also benefits the charge transfer and chemical stability in rigid PSCs, contributing to PCEs of over 25% as well as thermal stability with <i>T</i>₈₆ of 1200 h under aging at 85 °C.