Methylamine-Dimer-Induced Phase Transition toward MAPbI3 Films and High-Efficiency Perovskite Solar Modules

钙钛矿(结构) 甲胺 化学 相(物质) 二聚体 化学工程 相变 化学物理 结晶学 凝聚态物理 有机化学 物理 工程类
作者
Xiaofeng Huang,Ruihao Chen,Guocheng Deng,Faming Han,Pengpeng Ruan,Fangwen Cheng,Jun Yin,Binghui Wu,Nanfeng Zheng
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:142 (13): 6149-6157 被引量:68
标识
DOI:10.1021/jacs.9b13443
摘要

Perovskite films prepared with CH3NH2 molecules under ambient conditions have led to rapid fabrication of perovskite solar cells (PSCs), but there remains a lack of mechanistic studies and inconsistencies with operability in their production. Here the crystal structure of CH3NH2-CH3NH3PbI3 was analyzed to involve hydrogen bonds (CH3NH2···CH3NH3+) and has guided the facile, reproducible preparation of high-quality perovskite films under ambient conditions. Hydrogen bonds within CH3NH2···CH3NH3+ dimers were found in the CH3NH2-CH3NH3PbI3 intermediates, accompanied by 1D-PbI3- chains (δ-phase). The weakly hydrogen-bonded CH3NH2 molecules were easily released from the CH3NH2-CH3NH3PbI3 intermediates, contributing to rapid, spontaneous phase transition from 1D-PbI3- (δ-phase) to 3D-PbI3- (α-phase). Further introduction of CH3NH3Cl into the CH3NH2-CH3NH3PbI3 intermediates led to interruption of 1D-PbI3- transition into 0D-Pb2I9-xClx5-(0 < x < 6), adjusting the phase transition route toward 3D-PbI3-. On the basis of the above understanding, CH3NH2 solution in ethanol and CH3NH3Cl were used for precursors and a best efficiency of 20.3% in PSCs was achieved. Large-scale modules (12 cm2 aperture area) fabricated by a dip-coating technology exhibited an efficiency up to 16.0% and outstanding stability over 10 000 s under continuous output. The developed preparation method of perovskite precursors and insightful research into the methylamine-dimer-induced phase transition mechanism have enabled the production of high-quality perovskite films with robust operability, showing great potential for large-scale commercialization.
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