Interface Nucleophilic Substitution Reaction-Driven Precise Growth of Ag2Te Quantum Dots

IF 7.2 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Chemistry of Materials Pub Date : 2024-09-27 DOI:10.1021/acs.chemmater.4c00026

Zheng Li, Jun Xu, Wei Xie, Dongbing Zhao, Zhen-Ya Liu, Xian Yang, Haohao Fu, Shijia Jiang, Wei Zhao, Ming-Yu Zhang, An-An Liu, Dai-Wen Pang

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Abstract

Surface ligands of quantum dots (QDs) play pivotal roles in determining their optical properties and stability during the growth process. The stability and continuous growth of nanocrystals are crucial to precisely tuning their properties. However, the dilemma surrounding the stability of nanocrystals and their continuous growth remains unsolved, posing a formidable challenge. Herein, we have proposed a strategy for precise tuning of Ag₂Te QD growth driven by nucleophilic substitution reaction (SN2) between surface-bound thiol ligands and halogenated hydrocarbons (RX, X = Cl, Br, I), prompted by the generation of silver halide precipitate. As a result, Ag₂Te QDs with emission wavelengths precisely and continuously tunable in the range of 1176–2023 nm have been successfully synthesized in one pot. As the reaction advances, the quantity of the more strongly coordinating RS^– gradually diminishes, while that of the weaker coordinating dioctyl sulfide gradually increases. This dynamic process enables the growth of the QDs. The rate of the SN2 reaction can be adjusted by varying the species and concentration of RX, as well as the amount of Ag species, significantly influencing the growth rate of the QDs, a crucial factor for resolving the dilemma between the stability and tunability of the QDs. Additionally, this proposed strategy holds the potential to modulate the properties of various nanoparticles through chemical reactions at the interfaces.

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界面亲核取代反应驱动的 Ag2Te 量子点精确生长

量子点（QDs）的表面配体在决定其光学特性和生长过程中的稳定性方面起着举足轻重的作用。纳米晶体的稳定性和持续生长对精确调整其特性至关重要。然而，围绕纳米晶体的稳定性及其持续生长的难题仍未得到解决，这构成了一项艰巨的挑战。在此，我们提出了一种通过表面结合的硫醇配体与卤代烃（RX，X = Cl、Br、I）之间的亲核置换反应（SN2），在生成卤化银沉淀的驱动下精确调节 Ag2Te QD 生长的策略。结果，在一锅内成功合成了发射波长可在 1176-2023 纳米范围内精确连续调谐的 Ag2Te QDs。随着反应的进行，配位较强的 RS- 的数量逐渐减少，而配位较弱的二辛基硫醚的数量逐渐增加。这一动态过程使得 QDs 得以生长。SN2 反应的速率可以通过改变 RX 的种类和浓度以及 Ag 种类的数量来调节，从而显著影响 QDs 的生长速率，这是解决 QDs 稳定性和可调性之间难题的关键因素。此外，这种拟议策略还具有通过界面化学反应调节各种纳米粒子特性的潜力。

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来源期刊

Chemistry of Materials 工程技术-材料科学：综合

CiteScore

14.10

自引率

5.80%

发文量

929

审稿时长

1.5 months

期刊介绍： The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.