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由水分散性碳点基复合材料获得的聚集诱导室温磷光

Aggregation-Induced Room-Temperature Phosphorescence Obtained from Water-Dispersible Carbon Dot-Based Composite Materials.

作者信息

Wang Chan, Chen Yueyue, Xu Yalan, Ran Guoxia, He Yimin, Song Qijun

机构信息

Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, International Research Center for Photoresponsive Molecules and Materials, School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, P. R. China.

出版信息

ACS Appl Mater Interfaces. 2020 Mar 4;12(9):10791-10800. doi: 10.1021/acsami.9b20500. Epub 2020 Feb 20.

Abstract

Room-temperature phosphorescence (RTP) materials are desirable in chemical sensing because of their long emission lifetime and they are free from background autofluorescence. Nevertheless, the achievement of RTP in aqueous solution is still a highly challenging task. Herein, a molten salt method to prepare carbon dot (CD)-based RTP materials is presented by direct calcination of carbon sources in the presence of inorganic salts. The resultant CD composites (CDs@MP) exhibit bright RTP with a quantum yield of 26.4% and a lifetime of 1.28 s, which lasts for about 6 s to the naked eye. Importantly, their aqueous dispersion also has good RTP characteristics. This is the first time that the long-lived CDs@MP with RTP are achieved in aqueous solution owing to the synergistic effect of crystalline confinement and aggregation-induced phosphorescence. Further investigations reveal that three key processes may be responsible for the observed RTP of the composite materials: (1) The rigid crystalline salt shell can preserve the triplet states of CDs@MP in water and suppress the nonradiative deactivation; (2) The addition of high-charge-density metal ions Mg(II) and phosphorus element in the composite facilitates the singlet-to-triplet intersystem crossing process and enhances the RTP emission; (3) The aggregation of CDs@MP nanocomposites enables the matrix shell to self-assemble into a network, which further improves the rigidity of the shell and prevents the intermolecular motions, hence prolonging the RTP lifetime. The unique RTP feature and good water dispersibility allow the CD-based composite materials to be applicable in detection of temperature and pH in the aqueous phase. Our approach for producing long-lived RTP CDs@MP is effective, simple, and low-cost, which opens a new route to develop RTP materials that are applicable in aqueous solution.

摘要

室温磷光(RTP)材料因其长发射寿命且无背景自发荧光而在化学传感领域备受青睐。然而,在水溶液中实现室温磷光仍是一项极具挑战性的任务。在此,我们提出一种熔盐法,通过在无机盐存在下直接煅烧碳源来制备基于碳点(CD)的室温磷光材料。所得的CD复合材料(CDs@MP)表现出明亮的室温磷光,量子产率为26.4%,寿命为1.28秒,肉眼可观察到其持续约6秒。重要的是,它们在水中的分散液也具有良好的室温磷光特性。由于晶体限域和聚集诱导磷光的协同作用,这是首次在水溶液中实现具有长寿命室温磷光的CDs@MP。进一步研究表明,复合材料观察到的室温磷光可能由三个关键过程导致:(1)刚性晶体盐壳可在水中保留CDs@MP的三重态并抑制非辐射失活;(2)复合材料中高电荷密度金属离子Mg(II)和磷元素的加入促进了单重态到三重态的系间窜越过程并增强了室温磷光发射;(3)CDs@MP纳米复合材料的聚集使基质壳自组装成网络,进一步提高了壳的刚性并阻止了分子间运动,从而延长了室温磷光寿命。独特的室温磷光特性和良好的水分散性使得基于CD的复合材料可应用于水相中温度和pH的检测。我们制备长寿命室温磷光CDs@MP的方法有效、简单且低成本,为开发适用于水溶液的室温磷光材料开辟了一条新途径。

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