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锡碲纳米晶形成的合成机制。

Synthetic Mechanisms in the Formation of SnTe Nanocrystals.

机构信息

Materials Science Program, University of Rochester, 4011 Wegmans Hall, Rochester, New York 14627, United States.

Department of Chemistry, University of Rochester, 404 Hutchison Hall, Rochester, New York 14627, United States.

出版信息

J Am Chem Soc. 2022 Apr 13;144(14):6251-6260. doi: 10.1021/jacs.1c11697. Epub 2022 Mar 29.

Abstract

Infrared active colloidal semiconducting nanocrystals (NCs) are important for applications including photodetectors and photovoltaics. While much research has been conducted on nanocrystalline materials such as the Pb and Hg chalcogenides, less toxic alternatives such as SnTe have been far less explored. Previous synthetic work on SnTe NCs have characterized photophysical properties of the nanoparticles. This study focuses on understanding the fundamental chemical mechanisms involved in SnTe NC formation, with the aim to improve synthetic outcomes. The solvent oleylamine, common to all SnTe syntheses, is found to form a highly reactive, heteroleptic Sn-oleylamine precursor that is the primary molecular Sn species initiating NC formation and growth. Further, the capping ligand oleic acid (OA) reacts with this amine to produce tin oxide (SnO), facilitating the formation of an NC SnO shell. Therefore, the use of OA during synthesis is counterproductive to the formation of stoichiometric SnTe nanoparticles. The knowledge of chemical reaction mechanisms creates a foundation for the production of high-quality, unoxidized, and stoichiometric SnTe NCs.

摘要

红外活性胶体半导体纳米晶体(NCs)在包括光电探测器和光伏在内的应用中非常重要。虽然已经对 Pb 和 Hg 族化合物等纳米晶材料进行了大量研究,但毒性较小的替代品如 SnTe 的研究则要少得多。以前关于 SnTe NCs 的合成工作已经对纳米颗粒的光物理性质进行了表征。本研究重点是了解 SnTe NC 形成过程中的基本化学机制,旨在改善合成结果。溶剂油胺是所有 SnTe 合成中常见的物质,它形成了一种高反应性的杂配位 Sn-油胺前体,这是引发 NC 形成和生长的主要分子 Sn 物种。此外,封端配体油酸(OA)与该胺反应生成氧化锡(SnO),有利于 SnO 壳的形成。因此,在合成过程中使用 OA 不利于形成化学计量的 SnTe 纳米颗粒。化学反应机制的知识为生产高质量、未氧化和化学计量的 SnTe NCs 奠定了基础。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/286f/9011400/3311eec97a7a/ja1c11697_0001.jpg

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