Room-Temperature, Multigram-Scale Synthesis and Conversion Mechanism of Highly Luminescent Lead Sulfide Quantum Dots

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry Letters Pub Date : 2023-09-05 DOI:10.1021/acs.jpclett.3c02005
Zhen Jia, Yu Dai, Haoyun Shao, Jingyi Xu, Qingyu Meng and Juan Qiao*, 
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Abstract

PbS quantum dots (QDs) are attractive near-infrared (NIR) materials, but traditional synthetic methods require inert atmosphere and/or high temperature. Herein we develop a facile, room-temperature synthetic route for in situ halide passivated PbS QDs through controllable reactions between lead halide, N,N′-diphenyl thiourea, and oleyamine (OLA) in toluene. Contrast experiments and theoretical calculations reveal that the OLA plays a bifunctional role as a mild base to initiate the formation of PbS monomers and as a dynamic ligand to control the crystallization of PbS QDs and further ligand exchange. The oleic acid-capped PbS QDs exhibit high photoluminescence quantum yields up to 45%. The scaled-up synthesis on multigram scales shows great batch-to-batch consistency. We further demonstrate high-power NIR light-emitting diodes using the PbS QDs as color converters, delivering NIR optical power of 9.2 mW at 160 mA. This work provides a simple and versatile synthetic route for high-quality PbS QDs and boosts the applications of NIR materials.

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室温、多克尺度高发光硫化铅量子点合成及转化机理研究
PbS量子点(QDs)是极具吸引力的近红外(NIR)材料,但传统的合成方法需要惰性气氛和/或高温。本文通过卤化铅、N,N ' -二苯基硫脲和聚胺(OLA)在甲苯中的可控反应,开发了一种简便的室温原位卤化物钝化PbS量子点合成路线。对比实验和理论计算表明,OLA具有两种功能,一是作为温和的碱来引发PbS单体的形成,二是作为动态配体来控制PbS量子点的结晶和进一步的配体交换。油酸盖顶的PbS量子点具有较高的光致发光量子产率,可达45%。多图尺度上的放大合成显示出批次间的一致性。我们进一步展示了使用PbS量子点作为颜色转换器的高功率近红外发光二极管,在160 mA时提供9.2 mW的近红外光功率。本研究为制备高质量PbS量子点提供了一条简单、通用的合成途径,促进了近红外材料的应用。
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来源期刊
The Journal of Physical Chemistry Letters
The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
9.60
自引率
7.00%
发文量
1519
审稿时长
1.6 months
期刊介绍: The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.
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