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化学进展 2023, Vol. 35 Issue (2): 263-373 DOI: 10.7536/PC220720 前一篇   后一篇

• 综述 •

碳点基水相室温磷光复合材料研究进展

廖子萱1,2, 王宇辉1,*(), 郑建萍1,*()   

  1. 1 中国科学院宁波材料技术与工程研究所 宁波 315201
    2 温州医科大学 温州 325035
  • 收稿日期:2022-07-14 修回日期:2022-09-30 出版日期:2023-02-24 发布日期:2022-10-31
  • 基金资助:
    浙江省自然科学基金(LY20B050003); 宁波市3315创新团队项目(2019A-14-C)
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Research Advance of Carbon-Dots Based Hydrophilic Room Temperature Phosphorescent Composites

Zixuan Liao1,2, Yuhui Wang1(), Jianping Zheng1()   

  1. 1 Ningbo Institute of Material Technology and Engineering, Chinese Academy of Sciences,Ningbo 315201, China
    2 Wenzhou Medical University,Wenzhou 325035, China
  • Received:2022-07-14 Revised:2022-09-30 Online:2023-02-24 Published:2022-10-31
  • Contact: *e-mail: wangyuhui@nimte.ac.cn (Yuhui Wang); zhengjianping@nimte.ac.cn (Jianping Zheng)
  • Supported by:
    Zhejiang Provincial National Natural Science Foundation of China(LY20B050003); Ningbo 3315 Innovation Teams Program(2019A-14-C)

室温磷光(RTP)凭借较长的发光寿命和强烈的环境敏感特性,在化学/生物传感、生物成像、高级光学防伪与信息加密等诸多领域表现出广阔的应用前景。近些年,具有制备简单、化学惰性、低毒性、易功能化等优势的固态非金属室温磷光碳点获得了研究者的青睐。然而,其磷光发射易受水环境中溶解氧和水分子影响而淬灭,导致其应用局限于固态基质(如防伪油墨)。因而,如何稳定水相下碳点的激发三重态是实现其RTP发射与应用的关键。本文依据近年来碳点基水相RTP复合材料的最新研究进展,归纳总结了其构建策略及在传感、成像及防伪等方面的应用,并探讨了其面临的挑战及未来的发展方向。

关键词： 室温磷光, 碳点, 水相, 制备, 传感, 生物成像, 光学防伪

Due to the unique merits of long luminescence lifetime and environmental sensitivity, room temperature phosphorescence (RTP) has demonstrated great potential in many fields, e.g., chemo/biosensing, bioimaging, biomedicine, and advanced optical anti-counterfeiting and encryption. In recent years, non-metal doped solid state room temperature phosphorescent (RTP) carbon-dots (CDs) have attracted broad attention because of their facile preparation, chemical inertness, low toxicity, easy surface modification, and so on. However, in an aqueous environment, their RTP emissions suffer from serious triplet quenching that induced by dissolved oxygen and water molecule. How to stabilize the triplet state in aqueous phase is the key to establish their RTP emission, and thus it is necessary to look back the state-of-the-art knowledge of CDs-based water-soluble RTP materials. In this review, in light of the recent advance, we summarize and discuss their synthesis strategies (e.g., inorganic salt melting, SiO2 coating, polymer combination, and hydrogen bond network stabilization), and relevant applications in sensing, imaging and anti-counterfeiting, and finally propose the challenging and future prospects. To the best of our knowledge, this is the first review on the synthesis and applications of hydrophilic RTP materials based on CDs. We hope that this review will provide inspiration for the further fabrication and versatile biological uses of CDs-based RTP materials.

Contents

1 Introduction

2 Synthetic strategies

2.1 Inorganic salt melting method

2.2 SiO2 coating

2.3 Polymer-based hydrogen stabilization

2.4 Rigid hydrogen bond network stabilization

3 Applications

3.1 Anti-counterfeiting and information encryption

3.2 Detections of metal ions and small molecules

3.3 Biological detection and imaging

3.4 Other applications

4 Conclusion and outlook

Key words: room temperature phosphorescence, carbon-dots, aqueous phase, synthesis, sensing, bioimaging, optical anti-counterfeiting
()
图1 荧光、磷光及延迟荧光原理示意图
Fig.1 Schematic illustration of fluorescence (FL), phosphorescence (PL) and delayed fluorescence (DF)
图2 水相RTP碳点的发展时间线[31,45???~49]
Fig.2 Development timeline of CDs-based RTP materials in aqueous phase[31,45???~49]
图3 (a)熔盐法制备CDs@MP示意图;(b)CDs-MP粉末及其水溶液在紫外灯辐照关闭后的磷光图片[49]
Fig.3 (a) The schematic illustration of the molten salt method for the in situ synthesis of CDs@MP nanocomposites; (b) RTP digital photographs of CDs@MP (power and aqueous solution) under ultraviolet light[49]
图4 (a)TEOS直接水解包覆的CDs-RhB@SiO2形成示意图[31];(b)表面共价固定法制备的CDs@SiO2形成示意图和紫外激发下的水相RTP照片[54]
Fig.4 (a) Schematic diagram of the formation of CDs-RhB@SiO2 via a TEOS hydrolysis-based coating[31]; (b) schematic illustration of the preparation of CDs@SiO2 using surface covalent fixation and the RTP photographs in aqueous solution under the UV excitation[54]
图5 (a)CDs/PVA薄膜的构筑以及RTP产生的机理[65];(b)碳点-氰尿酸氢键网络复合体系的构筑与结构示意图[66];(c)碳点-三聚氰胺水相RTP纳米复合体系的制备与结构示意图[48]
Fig.5 (a) Schematic illustration of the fabrication and RTP emission mechanism of the CDs/PVA film[65]; (b) the construction and structure schematic illustration of the CDs-CA hydrogen bond network[66]; (c) the fabrication and hydrogen bond structure schematic illustration of the CDs-melamine nano-hybrids[48]
图6 碳点基水相RTP材料的应用。(a)m-CDs@nSiO2复合材料用于信息加密与解密[47];(b)CDs-PVA磷光薄膜用于Fe3+传感[65];(c)CDs@SiO2水相RTP纳米复合体系应用于小鼠乳腺癌细胞的荧光与时间分辨成像[54];(d)氮掺杂磷光碳点用于光动力抗菌[87]
Fig.6 The applications of CDs-based water-soluble RTP materials. (a) Information encryption and decryption via the m-CDs@nSiO2 composites[47]; (b) Schematic illustration of the CDs-PVA RTP thin film for Fe3+ sensing[65]; (c) Fluorescence and time resolution imaging via the CDs@SiO2 aqueous RTP nanocomposites[54]; (d) Photodynamic antibacterial application using the nitrogen-doped phosphorescent carbon-dots[87]
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