Department of Chemistry, Physics, and Atmospheric Sciences, Jackson State University, Jackson, Mississippi 39217, United States.
Department of Chemistry, University of South Florida, 4202 E Fowler Avenue, Tampa, Florida 33620, United States.
ACS Appl Mater Interfaces. 2023 May 31;15(21):25495-25505. doi: 10.1021/acsami.3c02571. Epub 2023 May 18.
Homogeneous and pinhole-free large-area perovskite films are required to realize the commercialization of perovskite modules and panels. Various large-area perovskite coatings were developed; however, at their film coating and drying stages, many defects were formed on the perovskite surface. Consequently, not only the devices lost substantial performance but also their long-term stability deteriorated. Here, we fabricated a compact and uniform large-area MAPbI-perovskite film by a slot-die coater at room temperature () and at high relative humidity (RH) up to 40%. The control slot-die-coated perovskite solar cell (PSC) produced 1.082 V open-circuit voltage (), 24.09 mA cm short current density (), 71.13% fill factor (FF), and a maximum power conversion efficiency (PCE) of 18.54%. We systematically employed a multi-functional artificial amino acid (F-LYS-S) to modify the perovskite defects. Such amino acids are more inclined to bind and adhere to the perovskite defects. The amino, carbonyl, and carboxy functional groups of F-LYS-S interacted with MAPbI through Lewis acid-base interaction and modified iodine vacancies significantly. Fourier transform infrared spectroscopy revealed that the C═O group of F-LYS-S interacted with the uncoordinated Pb ions, and X-ray photoelectron spectroscopy revealed that the lone pair of -NH coordinated with the uncoordinated Pb and consequently modified the I vacancies remarkably. As a result, the F-LYS-S-modified device demonstrated more than three-fold charge recombination resistance, which is one of the primary requirements to fabricate high-performance PSCs. Therefore, the device fabricated employing F-LYS-S demonstrated remarkable PCE of 21.08% with superior photovoltaic parameters of 1.104 V , 24.80 mA cm , and 77.00%. FF. Concurrently, the long-term stability of the PSCs was improved by the F-LYS-S post-treatment, where the modified device retained 89.6% of its initial efficiency after storing for 720 h in air ( ∼ 27 °C and RH ∼ 50-60%).
为了实现钙钛矿模块和组件的商业化，需要制备具有均匀性和无针孔的大面积钙钛矿薄膜。为此，人们开发了各种大面积钙钛矿涂层方法；然而，在薄膜涂层和干燥阶段，钙钛矿表面会形成许多缺陷。因此，不仅器件的性能显著下降，而且其长期稳定性也恶化。在这里，我们在室温（）和高达 40%的高相对湿度（RH）下，通过狭缝涂布器制备了致密且均匀的大面积 MAPbI 钙钛矿薄膜。所制备的控制狭缝涂布钙钛矿太阳能电池（PSC）具有 1.082 V 的开路电压（）、24.09 mA cm 的短路电流密度（）、71.13%的填充因子（FF）和 18.54%的最大功率转换效率（PCE）。我们系统地采用了一种多功能人工氨基酸（F-LYS-S）来修饰钙钛矿的缺陷。这种氨基酸更倾向于与钙钛矿缺陷结合和附着。F-LYS-S 的氨基、羰基和羧基官能团通过路易斯酸碱相互作用与 MAPbI 相互作用，并显著修饰碘空位。傅里叶变换红外光谱显示，F-LYS-S 的 C═O 基团与未配位的 Pb 离子相互作用，X 射线光电子能谱显示，-NH 的孤对电子与未配位的 Pb 配位，并显著修饰 I 空位。结果表明，F-LYS-S 修饰的器件具有超过三倍的电荷复合电阻，这是制备高性能 PSCs 的主要要求之一。因此，采用 F-LYS-S 制备的器件表现出显著的 21.08%的功率转换效率，具有优越的光伏参数：1.104 V 的开路电压（）、24.80 mA cm 的短路电流密度（）和 77.00%的填充因子（FF）。同时，通过 F-LYS-S 后处理提高了 PSCs 的长期稳定性，修饰后的器件在空气中（ ∼ 27°C 和 RH ∼ 50-60%）储存 720 h 后保留了初始效率的 89.6%。
