Abstract

The uncoordinated lead cations are ubiquitous in perovskite films and severely affect the efficiency and stability of perovskite solar cells (PSCs). In this work, 15-crown-5 with various heteroatoms are connected to the organic semiconductor carbazole diphenylamine, and two new compounds, CDT-S and CDT-N, are developed to modify the Pb2+ defects in perovskite films through the anti-solvent method. Apart from the oxygen atoms, there are also N atoms on crown ether ring in CDT-N, and both S and N heteroatoms in CDT-S. The heteroatoms enhance the interaction between the crown ether-based semiconductors and the undercoordinated Pb2+ defect in perovskite. Particularly, the stronger interaction between S atoms and Pb2+ further enhances the defect passivation effect of CDT-S than CDT-N, thereby more effectively suppressing the non-radiative recombination of charge carriers. Finally, the efficiency of the device treated with CDT-S is up to 23.05 %. Moreover, the unencapsulated device based on CDT-S maintained 90.5 % of the initial efficiency after being stored under dark conditions for 1000 hours, demonstrating good long-term stability. Our work demonstrates that crown ethers are promising in perovskite solar cells, and the crown ether containing multiple heteroatoms could effectively improve both efficiency and stability of devices.

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