Defect Passivation Effect of Chemical Groups on Perovskite Solar Cells

Defect passivation is a key strategy to prepare high-performance perovskite solar cells (PVSCs). Even though abundant passivation molecules have been applied, the absence of detailed researches with regard to different functional groups in polymer additives may inevitably impede the establishment of passivation molecules selection rules. In this work, three passivation molecules including poly(vinyl alcohol) (PVA), polymethyl acrylate (PMA), and poly(acrylic acid) (PAA) are employed to systematically analyze the passivation effect from hydroxyl, carbonyl, and carboxyl groups. In general, PVA (-OH) can form hydrogen bonds with perovskite and PMA (-C═O) can complex with uncoordinated Pb²⁺. Specifically, PAA (-COOH) can interact selectively with MA⁺ and I^- ions via hydrogen bonding and complex with uncoordinated Pb²⁺ to passivate defects more effectively. Hence, the PAA-incorporated PVSCs based on MAPbI₃ achieve the champion power conversion efficiency (PCE) of 20.29% with open-circuit voltage up to 1.13 V. In addition, PAA cross-linking perovskite grains can relieve mechanical stress, as well as occupy the major channels to suppress ion migration and water/oxygen erosion. The corresponding unencapsulated devices demonstrate a superior light soaking stability, retaining more than 80% of the original PCE under one sun illumination for 1000 h.