中国科学院大连化物所郭鑫团队报道了用于高效稳定钙钛矿太阳能电池的芳香族酮的空间构象工程。相关研究成果于2024年12月9日发表在国际顶尖学术期刊《美国化学会杂志》。

最先进的混合卤化铅钙钛矿太阳能电池（PSCs）中使用的含羰基材料，表现出强烈的结构依赖性电子供体效应，在缺陷钝化中占主导地位。然而，分子空间构象对含羰基钝化剂效能的影响仍然不明确，阻碍了钝化材料分子设计的进步。

该文中，研究表明，将芳香酮的空间扭转角从扭曲构型改变为平面构型，如二苯甲酮（BP，27.2°）、蒽酮（AR，15.3°）和9-芴酮（FO，0°）所示，会导致羰基周围的电子云密度显著增加，从而提高了铅基缺陷的钝化能力。

因此，PSCs性能还取决于芳香酮的扭转角，共面FO基PSCs实现了25.13%的最高功率转换效率（PCE），并在连续1个标准光照（ISOS-L-1I）下以最大功率点运行1000小时后保持了92%的初始效率。此外，含有FO的钙钛矿微型模块（14.0 cm²）的PCE为20.19%。

研究结果突出了分子构象对羰基钝化效果的影响，为芳香酮作为高效稳定PSC钝化剂的设计和开发提供了更深入的见解。

附：英文原文

Title: Spatial Conformation Engineering of Aromatic Ketones for Highly Efficient and Stable Perovskite Solar Cells

Author: Xiaoqing Jiang, Lina Zhu, Bingqian Zhang, Likai Zheng, Linqin Wang, Pingping Li, Minhuan Wang, Guangyue Yang, Kaiwen Dong, Suying Li, Shiwei Liu, Yanfeng Yin, Haiyuan Wang, Shaik. M. Zakeeruddin, Shuping Pang, Licheng Sun, Michael Grtzel, Xin Guo

Issue&Volume: December 9, 2024

Abstract: Carbonyl-containing materials employed in state-of-the-art hybrid lead halide perovskite solar cells (PSCs) exhibit a strong structure-dependent electron donor effect that predominates in defect passivation. However, the impact of the molecular spatial conformation on the efficacy of carbonyl-containing passivators remains ambiguous, hindering the advancement of molecular design for passivating materials. Herein, we show that altering the spatial torsion angle of aromatic ketones from twisted to planar configurations, as seen in benzophenone (BP, 27.2°), anthrone (AR, 15.3°), and 9-fluorenone (FO, 0°), leads to a notable increment of the electron cloud density around the carbonyl group, thus improving the passivation ability for lead-based defects. Consequently, the PSC performance also relies on the torsion angle of the aromatic ketones, with the coplanar FO-based PSC achieving a highest power conversion efficiency (PCE) of 25.13% and retaining 92% of its initial efficiency after 1000 h of operation at the maximum power point under continuous 1-sun illumination (ISOS-L-1I). Moreover, a perovskite mini-module (14.0 cm2) containing FO exhibits a PCE of 20.19%. Our findings highlight the influence of molecular conformation on the passivation effect of the carbonyl group, offering deeper insight into the design and development of aromatic ketones as passivators for highly efficient and stable PSCs.

DOI: 10.1021/jacs.4c13866

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c13866