Role of Acids in Producing Ultrabright, Dual‐Emissive Carbon Dots and their Urea/Biuret Composites with Ultralong Afterglow

IF 2.7 4区 材料科学 Q3 CHEMISTRY, PHYSICAL
Dong-mei Yan, Zhi‐ying Zhang, Yun Liu, Yan Guan, Dongming Sun
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Abstract

Since 2015, m‐phenylenediamines (mPD) have become a popular carbon source for the synthesis of carbonized polymer dots (CPDs). However, their exact fluorescence mechanism is still obscure. To elucidate this, inorganic acids that are carbon‐free are chosen as additives for a comparative study. It is found that the green fluorescence quantum yield (nearly 80%), photostability, and reaction yield (over 90%) can be enhanced by introduction of most of inorganic acids with moderate amount. Besides, green‐blue dual emission is observed in acid‐assisted groups. UV‐vis absorption, Fourier‐transform infrared spectroscopy, and surface‐enhanced Raman scattering results indicate that the green fluorescence center is composed of quinoid rings, whereas the blue fluorophore contains benzenoid rings. Moreover, room‐temperature afterglow with lifetime up to 1.25 s is observed exclusively in acid‐assisted CPDs composites with urea/biuret. The blue chromophore is proposed to be the origin of the triplet level that induces the long afterglow. This work provides an in‐depth understanding on the macromolecular structures of CPDs derived from phenylenediamines, and contributes a new line of thought to the origin of phosphorescence in N‐doped carbon dots.

Abstract Image

酸在制备超亮双发射碳点及其超长余辉尿素/双缩脲复合材料中的作用
自2015年以来,间苯二胺(mPD)已成为合成碳化聚合物点(CPD)的流行碳源。然而,它们的确切荧光机制仍然不清楚。为了阐明这一点,选择无碳的无机酸作为添加剂进行比较研究。研究发现,通过引入适量的大多数无机酸,可以提高绿色荧光量子产率(近80%)、光稳定性和反应产率(超过90%)。此外,在酸辅助基团中观察到绿蓝双发射。紫外-可见吸收、傅立叶变换红外光谱和表面增强拉曼散射结果表明,绿色荧光中心由醌环组成,而蓝色荧光团包含苯环。此外,仅在含有尿素/缩二脲的酸辅助CPDs复合材料中观察到寿命高达1.25 s的室温余辉。蓝色发色团被认为是引发长余辉的三重态能级的起源。这项工作深入了解了苯二胺衍生的CPDs的大分子结构,并为N掺杂碳点磷光的起源提供了新的思路。
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来源期刊
Particle & Particle Systems Characterization
Particle & Particle Systems Characterization 工程技术-材料科学:表征与测试
CiteScore
5.50
自引率
0.00%
发文量
114
审稿时长
3.0 months
期刊介绍: Particle & Particle Systems Characterization is an international, peer-reviewed, interdisciplinary journal focusing on all aspects of particle research. The journal joined the Advanced Materials family of journals in 2013. Particle has an impact factor of 4.194 (2018 Journal Impact Factor, Journal Citation Reports (Clarivate Analytics, 2019)). Topics covered include the synthesis, characterization, and application of particles in a variety of systems and devices. Particle covers nanotubes, fullerenes, micelles and alloy clusters, organic and inorganic materials, polymers, quantum dots, 2D materials, proteins, and other molecular biological systems. Particle Systems include those in biomedicine, catalysis, energy-storage materials, environmental science, micro/nano-electromechanical systems, micro/nano-fluidics, molecular electronics, photonics, sensing, and others. Characterization methods include microscopy, spectroscopy, electrochemical, diffraction, magnetic, and scattering techniques.
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