Tailored Supramolecular Interactions in Host–Guest Complexation for Efficient and Stable Perovskite Solar Cells and Modules

• Published in: Angewandte Chemie International Edition Vol. 63; no. 40; pp. e202410454 - n/a
• Main Authors: Yang, Guangyue, Liu, Xin, Wang, Linqin, Dong, Kaiwen, Zhang, Bingqian, Jiang, Xiaoqing, Yin, Yanfeng, Wang, Minhuan, Niu, Wenzhe, Zheng, Likai, Yu, Shitao, Liu, Shiwei, Zakeeruddin, Shaik M., Guo, Xin, Pang, Shuping, Sun, Licheng, Grätzel, Michael, Wei, Mingyang
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 01.10.2024
• Edition: International ed. in English
• Subjects: Cations; Complexation; Crown ether; Crown ethers; Defect passivation; Dipole moments; Ethers; Host-guest complexation; Modules; Perovskite; Perovskites; Photovoltaic cells; Solar Cells; Surface defects; Crown ether; Perovskite; Host-guest complexation; Defect passivation; Solar Cells
• ISSN: 1433-7851; 1521-3773; 1521-3773
• DOI: 10.1002/anie.202410454

Host‐guest complexation offers a promising approach for mitigating surface defects in perovskite solar cells (PSCs). Crown ethers are the most widely used macrocyclic hosts for complexing perovskite surfaces, yet their supramolecular interactions and functional implications require further understanding. Here we show that the dipole moment of crown ethers serves as an indicator of supramolecular interactions with both perovskites and precursor salts. A larger dipole moment, achieved through the substitution of heteroatoms, correlates with enhanced coordination with lead cations. Perovskite films incorporating aza‐crown ethers as additives exhibited improved morphology, reduced defect densities, and better energy‐level alignment compared to those using native crown ethers. We report power‐conversion efficiencies (PCEs) exceeding 25 % for PSCs, which show enhanced long‐term stability, and a record PCE of 21.5 % for host–guest complexation‐based perovskite solar modules with an active area of 14.0 cm2. Dipole moment of crown ethers indicates their supramolecular interactions with perovskites. Higher dipole moments enhance coordination with lead cations, improving film morphology and optoelectronic properties. Optimized host–guest complexation led to perovskite solar modules reaching a 21.5 % efficiency over 14.0 cm2.