Zhao Qiangqiang, Zhang Bingqian, Hui Wei, Su Zhenhuang, Wang Han, Zhang Qi, Gao Kun, Zhang Xiaoxu, Li Bo-Han, Gao Xingyu, Wang Xiao, De Wolf Stefaan, Wang Kai, Pang Shuping
Institute of Flexible Electronics (IFE), Northwestern Polytechnical University, Xi'an, Shanxi 710072, P. R. China.
Key Laboratory of Photoelectric Conversion and Utilization of Solar Energy, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, P.R. China.
J Am Chem Soc. 2024 Jul 17;146(28):19108-19117. doi: 10.1021/jacs.4c03783. Epub 2024 Jun 7.
Previous findings have suggested a close association between oxygen vacancies in SnO and charge carrier recombination as well as perovskite decomposition at the perovskite/SnO interface. Underlying the fundamental mechanism holds great significance in achieving a more favorable balance between the efficiency and stability. In this study, we prepared three SnO samples with different oxygen vacancy concentrations and observed that a low oxygen vacancy concentration is conducive to long-term device stability. Iodide ions were observed to easily diffuse into regions with high oxygen vacancies, thereby speeding up the deprotonation of FAI, as made evident by the detection of the decomposition product formamide. In contrast, a high oxygen vacancy concentration in SnO could prevent hole injection, leading to a decrease in interfacial recombination losses. To suppress this decomposition reaction and address the trade-off, we designed a bilayer SnO structure to ensure highly efficient carrier transport still while maintaining a chemically inert surface. As a result, an enhanced efficiency of 25.06% (certified at 24.55% with an active area of 0.09 cm under fast scan) was achieved, and the extended operational stability maintained 90% of their original efficiency (24.52%) after continuous operation for nearly 2000 h. Additionally, perovskite submodules with an active area of 14 cm were successfully assembled with a PCE of up to 22.96% (20.09% with an aperture area).
先前的研究结果表明,SnO中的氧空位与电荷载流子复合以及钙钛矿/ SnO界面处的钙钛矿分解之间存在密切关联。其基本机制对于在效率和稳定性之间实现更有利的平衡具有重要意义。在本研究中,我们制备了三种具有不同氧空位浓度的SnO样品,并观察到低氧空位浓度有利于器件的长期稳定性。观察到碘离子容易扩散到具有高氧空位的区域,从而加速了FAI的去质子化,这通过检测分解产物甲酰胺得以证实。相反,SnO中高氧空位浓度会阻止空穴注入,导致界面复合损失减少。为了抑制这种分解反应并解决权衡问题,我们设计了一种双层SnO结构,以确保在保持化学惰性表面的同时仍能实现高效的载流子传输。结果,实现了25.06%的增强效率(在快速扫描下,活性面积为0.09 cm²时认证效率为24.55%),并且在连续运行近2000小时后,扩展的操作稳定性保持了其原始效率(24.52%)的90%。此外,成功组装了活性面积为14 cm²的钙钛矿子模块,其光电转换效率高达22.96%(孔径面积下为20.09%)。