Bidentate Lewis Base Ligand-Mediated Surface Stabilization and Modulation of the Electronic Structure of CsPbBr3 Perovskite Nanocrystals,Journal of the American Chemical Society

当前位置： X-MOL 学术 › J. Am. Chem. Soc. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Bidentate Lewis Base Ligand-Mediated Surface Stabilization and Modulation of the Electronic Structure of CsPbBr3 Perovskite Nanocrystals
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-12-20 , DOI: 10.1021/jacs.4c13724
Md. Samim Hassan, Pooja Basera, Bilawal Khan, Arsenii S. Portniagin, Kunnathodi Vighnesh, Ye Wu, Daniil A. Rusanov, Maria Babak, Jr-Hau He, Michal Bajdich, Andrey L. Rogach

The desorption of conventional ligands from the surface of halide perovskite nanocrystals (NCs) often causes their structural instability and deterioration of the optoelectronic properties. To address this challenge, we present an approach of using a bidentate Lewis base ligand, namely, 1,4-bis(diphenylphosphino)butane (DBPP), for the synthesis of CsPbBr₃ NCs. The phosphine group of DBPP has a strong interaction with the PbBr₂ precursor, forming a highly crystalline intermediate complex during the reaction. In the presence of oleic acid, the uncoordinated phosphine group of DBPP is converted into the phosphonium cation, which strongly binds to the surface bromide of the formed CsPbBr₃ NCs through hydrogen bonding. Density functional theory calculations suggest that DBPP can strongly bind to the undercoordinated lead and surface bromide ions of CsPbBr₃ NCs through its unprotonated and protonated phosphine groups, respectively. The robust binding of DBPP to the surface of perovskite NCs helps to preserve their structural integrity under various environmental stresses. Moreover, the electron density and energy levels are regulated in DBPP-capped CsPbBr₃ NCs by the donation of electrons from the ligands to the NCs, resulting in their improved photocatalytic CO₂ reduction performance. Our study highlights the potential of using bidentate ligands to stabilize the surface of perovskite NCs and modulate their optical and electronic properties.

更新日期：2024-12-20

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南