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卤化锗作为理想前驱体:设计一条更有效且毒性更低的路线来制备高光电质量的金属卤化物钙钛矿纳米晶体。

Germanium Halides Serving as Ideal Precursors: Designing a More Effective and Less Toxic Route to High-Optoelectronic-Quality Metal Halide Perovskite Nanocrystals.

作者信息

Wang Xiaochen, Bai Tianxin, Yang Bin, Zhang Ruiling, Zheng Daoyuan, Jiang Junke, Tao Shuxia, Liu Feng, Han Ke-Li

机构信息

Institute of Molecular Sciences and Engineering, Institute of Frontier and Interdisciplinary Science, Shandong University, Qingdao 266237, People's Republic of China.

State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, People's Republic of China.

出版信息

Nano Lett. 2022 Jan 26;22(2):636-643. doi: 10.1021/acs.nanolett.1c03527. Epub 2022 Jan 12.

Abstract

The three-precursors approach has proven to be advantageous for obtaining high-quality metal halide perovskite nanocrystals (PNCs). However, the current halide precursors of choice are mainly limited to those highly toxic organohalides, being unfavorable for large-scale and sustainable use. Moreover, most of the resulting PNCs still suffer from low quality in terms of photoluminescence quantum yield (PLQY). Herein we present all-inorganic germanium salts, GeX (X = Cl, Br, I), serving as robust and less hazardous alternatives that are capable of ensuring improved material properties for both Pb-based and Pb-free PNCs. Importantly, unlike most of the other inorganic halide sources, the GeX compound does not deliver the Ge element into the final compositions, whereas the PLQY and phase stability of the resulting nanocrystals are significantly improved. Theoretical calculations suggest that Ge halide precursors provide favorable conditions in both dielectric environment and thermodynamics, which jointly contribute to the formation of size-confined defect-suppressed nanoparticles.

摘要

三前驱体方法已被证明有利于获得高质量的金属卤化物钙钛矿纳米晶体(PNCs)。然而,目前所选用的卤化物前驱体主要局限于那些剧毒的有机卤化物,不利于大规模和可持续使用。此外,就光致发光量子产率(PLQY)而言,大多数所得的PNCs质量仍然较低。在此,我们提出全无机锗盐GeX(X = Cl、Br、I),作为强大且危害较小的替代品,能够确保提高基于Pb的和无Pb的PNCs的材料性能。重要的是,与大多数其他无机卤化物源不同,GeX化合物不会将Ge元素引入最终成分中,而所得纳米晶体的PLQY和相稳定性却得到显著提高。理论计算表明,锗卤化物前驱体在介电环境和热力学方面都提供了有利条件,这共同有助于形成尺寸受限、缺陷抑制的纳米颗粒。

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