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通过调控硫掺杂合成在分散态和聚集态均具有强发光的碳点。

Synthesis of carbon dots with strong luminescence in both dispersed and aggregated states by tailoring sulfur doping.

机构信息

Hospital of Stomatology, Jilin University, Changchun 130021, PR China; Jilin Provincial Key Laboratory of Tooth Development and Bone Remodeling, Jilin University, Changchun 130021, PR China.

Department of Chemistry, Durham University, Durham DH1 3LE, UK.

出版信息

J Colloid Interface Sci. 2022 Mar;609:54-64. doi: 10.1016/j.jcis.2021.11.179. Epub 2021 Dec 1.

DOI:10.1016/j.jcis.2021.11.179
PMID:34894555
Abstract

Carbon dots (CDots), a class of environmentally friendly carbon-based luminescent nanomaterial, have been applied in a wide variety of fields, including bioimaging and light-emitting diodes (LEDs). Prior to these applications, however, CDots usually require modifications because some of its limitations (e.g., the aggregation-induced luminescence quenching) make it difficult to apply in solid state. In order to realize CDots-based multiple applications simultaneously, this paper examines how CDots with a strong greenish-yellow fluorescence in both dispersed and aggregated states are prepared by microwave-assisted heating salicylic acid and thiourea. Based on control testing and the analysis of density functional theory calculations, S element from thiourea is doped into CDots and proves to be critical in governing the photoluminescence (PL) emission color. Featured with excellent biocompatibility and photostability, the dispersed CDots with photoluminescence quantum yields (32%) are able to function as a biological imaging reagent in vitro and in vivo without any side effect. Furthermore, the aggregated CDots also exhibit high photoluminescence quantum yields (26%) and remarkable resistance to organic solvent. These advantages will ensure that S-doped CDots can be applied as a color conversion layer so that white LEDs with different Commission International de L'Eclariage coordinates and tunable color temperature can be fabricated.

摘要

碳点(CDots)是一类环保型碳基发光纳米材料,已广泛应用于生物成像和发光二极管(LED)等多个领域。然而,在这些应用之前,CDots 通常需要进行修饰,因为其一些局限性(例如聚集诱导荧光猝灭)使其难以在固态下应用。为了实现 CDots 的多种应用,本文研究了如何通过微波辅助加热水杨酸和硫脲来制备在分散态和聚集态下均具有强烈黄绿色荧光的 CDots。通过控制实验和密度泛函理论计算分析,证明来自硫脲的 S 元素掺杂到 CDots 中对于控制光致发光(PL)发射颜色起着关键作用。所制备的分散态 CDots 具有良好的生物相容性和光稳定性,其光致发光量子产率(32%)可以作为体外和体内的生物成像试剂,而没有任何副作用。此外,聚集态 CDots 也表现出高的光致发光量子产率(26%)和对有机溶剂的显著耐受性。这些优点确保了 S 掺杂 CDots 可以用作颜色转换层,从而可以制造出具有不同国际照明委员会(Commission International de L'Eclariage)坐标和可调色温的白色 LED。

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