Chen Keqiang, Liu Dan, Lu Weiqi, Zhuo Kaihuai, Li Guogang
Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, P. R. China.
Zhejiang Institute, China University of Geosciences, Hangzhou 311305, P. R. China.
Inorg Chem. 2024 Jan 29;63(4):2247-2256. doi: 10.1021/acs.inorgchem.3c04210. Epub 2024 Jan 17.
Shelling with chalcogenides on the surface of lead halide perovskite (LHP) nanocrystals (NCs) is believed to be an effective approach to increase their stability under high-moisture/aqueous conditions, which is important for LHP NC-based optoelectronic devices. However, it is still a challenge to prepare high-quality LHP/chalcogenide core/shell NCs with moisture/aqueous stability. In this work, a surface-defect-induced strategy is carried out to facilitate the adsorption of Br ions and subsequently Zn ions to preform a bipolar surface, which reduces the energy barrier at the CsPbBr/ZnS interface and promotes the epitaxial growth of the ZnS shell layer. The aqueous stability of the as-received NCs shows an increase of over 12 times compared to that of the original one. Likewise, Mn ions are introduced to further reduce the geometric symmetry mismatch and defect density at the CsPbBr/ZnS interface. Interestingly, aqueous stability characterizations illustrate negligible degradation even after 230 min of ultrasonication, suggesting their outstanding stability. This work proposes an effective approach to prepare high-quality LHP/chalcogenide core/shell NCs, which possess great potential in the fabrication of stable optoelectronic devices.
在卤化铅钙钛矿(LHP)纳米晶体(NCs)表面包覆硫族化物被认为是提高其在高湿度/水性条件下稳定性的有效方法,这对于基于LHP NCs的光电器件很重要。然而,制备具有湿度/水性稳定性的高质量LHP/硫族化物核壳NCs仍然是一个挑战。在这项工作中,实施了一种表面缺陷诱导策略,以促进Br离子随后Zn离子的吸附,从而预先形成双极表面,这降低了CsPbBr/ZnS界面处的能垒,并促进了ZnS壳层的外延生长。与原始NCs相比,所制备的NCs的水性稳定性提高了12倍以上。同样,引入Mn离子以进一步减少CsPbBr/ZnS界面处的几何对称性失配和缺陷密度。有趣的是,水性稳定性表征表明,即使在超声处理230分钟后,降解也可忽略不计,这表明它们具有出色的稳定性。这项工作提出了一种制备高质量LHP/硫族化物核壳NCs的有效方法,其在制造稳定的光电器件方面具有巨大潜力。