摘要
During the crystallization of perovskite films,defects at Pb and I sites are generated,causing lattice mismatch and adversely affecting the performance of perovskite solar cells(PSCs).Herein,we introduced aπ-conjugated molecule with a dual-ring structure,namely CCA(3,4-ethylenedioxythiophene-2,5-dicarboxylic acid),as an additive to regulate the crystallization of perovskite films and passivate defects.As a bidentate Lewis base,CCA coordinates the bidentate carboxyl groups with free Pb^(2+)through the delocalized electrons of its conjugated ring.This coordination regulates lattice stress,repairs the 3D[PbI6]octahedra,stabilizes the perovskite framework,and guides the vertical orientation growth of grains.Simultaneously,the addition of CCA shifts the perovskite’s band structure towards p-type,achieving better energy-level alignment with the doped hole-transport layer(HTL)and suppressing non-radiative recombination.Consequently,the prepared CCA-doped single-junction devices exhibit an outstanding power conversion efficiency(PCE)of 24.90%,with a high open-circuit voltage(VOC)of 1.195,a high fill factor(FF)of 84.60%,and low FF loss.The optimized films and devices show enhanced long-term stability,retaining 80.1%of the initial efficiency after continuous illumination for 560 h.Additionally,a PCE of 21.6%was achieved in devices with a bandgap of 1.68 eV,which were further extended to perovskite/silicon tandem devices,achieving high-performance devices with PCEs of 30.96%(aperture area:1.05 cm^(2))and 25.96%(aperture area:20.06 cm^(2)).
基金
the generous financial support provided by Sichuan Science and Technology Program(2024ZDZX0030)
Chengdu Science and Technology Program(2024-JB00-00010-GX)。
