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用于颜色转换和X射线成像的高性能钙钛矿纳米晶薄膜的有机硅基配体设计

Organosilicon-Based Ligand Design for High-Performance Perovskite Nanocrystal Films for Color Conversion and X-ray Imaging.

作者信息

Chen Junchi, Jiang Guocan, Hamann Elias, Mescher Henning, Jin Qihao, Allegro Isabel, Brenner Philipp, Li Zhengquan, Gaponik Nikolai, Eychmüller Alexander, Lemmer Uli

机构信息

Light Technology Institute, Karlsruhe Institute of Technology (KIT), Engesserstrasse 13, 76131 Karlsruhe, Germany.

Zhejiang Institute of Photoelectronics, Department of Physics, Zhejiang Normal University, Jinhua, 321004 Zhejiang, P. R. China.

出版信息

ACS Nano. 2024 Apr 9;18(14):10054-10062. doi: 10.1021/acsnano.3c11991. Epub 2024 Mar 25.

Abstract

Perovskite nanocrystals (PNCs) bear a huge potential for widespread applications, such as color conversion, X-ray scintillators, and active laser media. However, the poor intrinsic stability and high susceptibility to environmental stimuli including moisture and oxygen have become bottlenecks of PNC materials for commercialization. Appropriate barrier material design can efficiently improve the stability of the PNCs. Particularly, the strategy for packaging PNCs in organosilicon matrixes can integrate the advantages of inorganic-oxide-based and polymer-based encapsulation routes. However, the inert long-carbon-chain ligands (e.g., oleic acid, oleylamine) used in the current ligand systems for silicon-based encapsulation are detrimental to the cross-linking of the organosilicon matrix, resulting in performance deficiencies in the nanocrystal films, such as low transparency and large surface roughness. Herein, we propose a dual-organosilicon ligand system consisting of (3-aminopropyl)triethoxysilane (APTES) and (3-aminopropyl)triethoxysilane with pentanedioic anhydride (APTES-PA), to replace the inert long-carbon-chain ligands for improving the performance of organosilicon-coated PNC films. As a result, strongly fluorescent PNC films prepared by a facile solution-casting method demonstrate high transparency and reduced surface roughness while maintaining high stability in various harsh environments. The optimized PNC films were eventually applied in an X-ray imaging system as scintillators, showing a high spatial resolution above 20 lp/mm. By designing this promising dual organosilicon ligand system for PNC films, our work highlights the crucial influence of the molecular structure of the capping ligands on the optical performance of the PNC film.

摘要

钙钛矿纳米晶体(PNCs)在广泛的应用领域具有巨大潜力,如颜色转换、X射线闪烁体和有源激光介质。然而,其固有的稳定性较差以及对包括水分和氧气在内的环境刺激高度敏感,已成为PNC材料商业化的瓶颈。合适的阻隔材料设计可以有效提高PNCs的稳定性。特别是,将PNCs封装在有机硅基质中的策略可以整合基于无机氧化物和基于聚合物的封装路线的优点。然而,目前用于硅基封装的配体系统中使用的惰性长碳链配体(如油酸、油胺)不利于有机硅基质的交联,导致纳米晶体薄膜存在性能缺陷,如透明度低和表面粗糙度大。在此,我们提出一种由(3-氨丙基)三乙氧基硅烷(APTES)和带有戊二酸酐的(3-氨丙基)三乙氧基硅烷(APTES-PA)组成的双有机硅配体系统,以取代惰性长碳链配体,从而改善有机硅包覆的PNC薄膜的性能。结果,通过简便的溶液浇铸法制备的强荧光PNC薄膜具有高透明度和降低的表面粗糙度,同时在各种恶劣环境中保持高稳定性。优化后的PNC薄膜最终作为闪烁体应用于X射线成像系统,显示出高于20 lp/mm的高空间分辨率。通过为PNC薄膜设计这种有前景的双有机硅配体系统,我们的工作突出了封端配体的分子结构对PNC薄膜光学性能的关键影响。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccda/11008364/0df3a9c19040/nn3c11991_0001.jpg

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