Zhu Hua, Kick Matthias, Ginterseder Matthias, Krajewska Chantalle J, Šverko Tara, Li Ruipeng, Lu Yongli, Shih Meng-Chen, Van Voorhis Troy, Bawendi Moungi G
Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA.
National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY, 11973, USA.
Adv Mater. 2023 Sep;35(39):e2304069. doi: 10.1002/adma.202304069. Epub 2023 Jul 30.
Mechanistic studies of the morphology of lead halide perovskite nanocrystals (LHP-NCs) are hampered by a lack of generalizable suitable synthetic strategies and ligand systems. Here, the synthesis of zwitterionic CsPbBr NCs is presented with controlled anisotropy using a proposed "surface-selective ligand pairs" strategy. Such a strategy provides a platform to systematically study the binding affinity of capping ligand pairs and the resulting LHP morphologies. By using zwitterionic ligands (ZwL) with varying structures, majority ZwL-capped LHP NCs with controlled morphology are obtained, including anisotropic nanoplatelets and nanorods, for the first time. Combining experiments with density functional theory calculations, factors that govern the ligand binding on the different surface facets of LHP-NCs are revealed, including the steric bulkiness of the ligand, the number of binding sites, and the charge distance between binding moieties. This study provides guidance for the further exploration of anisotropic LHP-NCs.
卤化铅钙钛矿纳米晶体（LHP-NCs）形态的机理研究因缺乏可推广的合适合成策略和配体体系而受阻。在此，使用提出的“表面选择性配体对”策略，实现了具有可控各向异性的两性离子CsPbBr纳米晶体的合成。这种策略提供了一个平台，用于系统地研究封端配体对的结合亲和力以及由此产生的LHP形态。通过使用具有不同结构的两性离子配体（ZwL），首次获得了大多数具有可控形态的ZwL封端LHP纳米晶体，包括各向异性的纳米片和纳米棒。将实验与密度泛函理论计算相结合，揭示了控制配体在LHP-NCs不同表面晶面上结合的因素，包括配体的空间位阻、结合位点的数量以及结合部分之间的电荷距离。本研究为进一步探索各向异性LHP-NCs提供了指导。
