高发光 AgInS2 和 AgInS2/ZnS 量子点的连续流动水合成,The Journal of Physical Chemistry C

当前位置： X-MOL 学术 › J. Phys. Chem. C › 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.)

高发光 AgInS2 和 AgInS2/ZnS 量子点的连续流动水合成
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2022-11-23 , DOI: 10.1021/acs.jpcc.2c06849
Céline Rivaux ₁ , Tugce Akdas ₁ , Ranjana Yadav ₁ , Omar El-Dahshan ₁ , Davina Moodelly ₁ , Wai Li Ling ₂ , Dmitry Aldakov ₁ , Peter Reiss ₁

Affiliation

半导体量子点 (QD) 的连续流动合成有望实现高度可重复性、可扩展性以及对所有反应参数的精确控制。在这里，我们将该技术应用于 Ag-In-S (AIS) 核和 AIS/ZnS 核/壳 QD 的水相合成，并优化了包括反应温度、压力、时间、性质和前体比例在内的几个参数。在较短的反应时间（8-15 分钟）内，核的光致发光量子产率 (PLQY) 值为 32%/44%（平均/最佳），核/壳系统的光致发光量子产率为 77%/83%。我们通过结合结构和光学研究证明，高 PLQY 源自供体-受体对重组过程，主要涉及 [In _Ag²⁺ + 2V _Ag^–] 缺陷复合物的形成有利于大量过量使用的铟（In:Ag 比率为 4:1）和低反应温度（100–120 °C）。在 ZnS 壳生长过程中结构无序进一步增强，除了表面钝化和非辐射衰变通道的去除外，还导致添加的锌离子部分扩散到 AIS 核中并形成 Zn In - 反_位^缺陷。所提出的方法提供了出色的重现性和高可扩展性，促进了高发光 AIS/ZnS QD 的大规模生产。

"点击查看英文标题和摘要"

Continuous Flow Aqueous Synthesis of Highly Luminescent AgInS2 and AgInS2/ZnS Quantum Dots

Continuous flow synthesis of semiconductor quantum dots (QDs) holds the promise of being highly reproducible, being scalable, and providing precise control of all reaction parameters. Here, we applied this technique to the aqueous synthesis of the Ag–In–S (AIS) core and AIS/ZnS core/shell QDs and optimized several parameters comprising reaction temperature, pressure, time, nature, and the ratio of precursors. Photoluminescence quantum yield (PLQY) values of 32%/44% (average/best) for the core and 77%/83% for the core/shell system have been obtained in short reaction times (8–15 min). We demonstrate by means of combined structural and optical studies that the high PLQY originates from donor–acceptor pair recombination processes, involving essentially [In_Ag²⁺ + 2V_Ag^–] defect complexes whose formation is favored by the large excess of indium used (In:Ag ratio of 4:1), and the low reaction temperature (100–120 °C). The structural disorder is further enhanced during ZnS shell growth, which in addition to surface passivation and removal of nonradiative decay channels leads to the partial diffusion of the added zinc ions into the AIS core and the formation of Zn_In⁻ antisite defects. The presented method provides excellent reproducibility and high scalability, facilitating the large-scale production of highly luminescent AIS/ZnS QDs.

更新日期：2022-11-23

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