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Identifying the existence of highly-fluorescent carboxylic group-rich carbon nanodots during a one-pot synthesis of branched polyethylenimine-passivated amine group-rich carbon nanodots

机译:一锅合成支化聚乙烯亚胺钝化的富含胺基的碳纳米点时,确定存在高荧光的富含羧基的碳纳米点的存在

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Carbon nanodots (C-Dots) have recently been proposed as promising alternatives to traditional semiconductor quantum dots and organic fluorophores. However, C-Dots were often prepared and studied as a mixture, and the ignorance of the real composition significantly limits the accurate understanding and control of physical/chemical properties of C-Dots and further practical applications. Herein, we demonstrated and identified for the first time the co-existence of highly-fluorescent carboxylic group-rich C-Dots (CR-C-Dots) and amine group-rich C-Dots (AR-C-Dots) during the one-pot pyrolysis of citric acid and branched polyethylenimine precursors. Transmission electron microscopy demonstrated that the average size of CR-C-Dots was slightly smaller than that of amine group-rich C-Dots (AR-C-Dots), 1.5 nm vs. 1.9 nm. Photophysical characterization indicated that CR-C-Dots had a longer fluorescence lifetime and higher quantum yields (QYs) than the AR-C-Dots, despite the same excitation-independent emission at 445 nm, unlike most previous reports, which stated that amine group passivation enhanced the QYs of C-Dots. Both the C-Dots showed excellent biocompatibility and great potential for cellular imaging. A fluorescence-and electron spin resonance-responsive dual-model probe for ascorbic acid detection was also constructed, further proving the existence of CR-C-Dots. This study facilitates the understanding of the nucleation/surface passivation process during C-Dots formation and the development of a new synthetic and purification strategy for C-Dots.
机译:碳纳米点(C-Dots)最近被提出作为传统半导体量子点和有机荧光团的有希望的替代品。但是,C点通常是作为混合物制备和研究的,对真实成分的无知极大地限制了对C点物理/化学性质以及进一步实际应用的准确理解和控制。在本文中,我们首次证明并鉴定了高荧光含量的富含羧基的C点(CR-C-Dots)和富含胺基的C点(AR-C-Dots)的共存柠檬酸和支链聚乙烯亚胺前体的热罐热解。透射电子显微镜显示,CR-C-Dots的平均尺寸略小于富胺基C-Dots(AR-C-Dots)的平均尺寸,分别为1.5 nm和1.9 nm。光物理特征表明,尽管在445 nm处有相同的激发无关发射,CR-C-Dots的荧光寿命比AR-C-Dots长,但荧光寿命更长,量子产率(QYs)更高,这与以前的大多数报道不同。钝化提高了C点的质量。两种C点均显示出优异的生物相容性和细胞成像的巨大潜力。还构建了用于抗坏血酸检测的荧光和电子自旋共振响应双模式探针,进一步证明了CR-C-Dots的存在。这项研究有助于理解C点形成过程中的成核/表面钝化过程,并为C点开发一种新的合成和纯化策略。

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