Mechanism of in situ confining carbon dots in phthalamide crystal for room-temperature phosphorescence†

IF 6.4 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Xingmei Li, Haixin Kang, Yingying Zhao, Tong Chen, Jingxia Zheng, Lin Chen, Bin Liu, Yongzhen Yang and Xuguang Liu
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Abstract

Carbon dot (CD)-based room temperature phosphorescence (RTP) materials have widespread applications in anti-counterfeiting, light-emitting diode (LED) lighting, and bioimaging due to their spectral tunability, long lifetime, and other excellent optical properties. However, challenges remain regarding their complicated preparation processes and unclear mechanism. In this work, we developed a one-step, in situ liquid-phase synthesis method using phthalic acid, formamide, and ethylene glycol to directly form RTP CDs@phthalamide composites with CD/organic crystal structures. The product required only filtration and drying without further post-processing, significantly simplifying the preparation procedure and facilitating large-scale production. The as-prepared CDs@phthalamide exhibit excitation-dependent phosphorescence with a naked-eye-visible afterglow of 5 s and a phosphorescence lifetime of 441 ms. The formation process and reaction mechanism of CDs@phthalamide were investigated by optimizing the reaction temperature and reaction time, calculating activation energies through theoretical simulations, and comparing the effect of different crystal structures of phthalamide and phthalimide crystals on luminescence. Unlike phthalimide, the phthalamide matrix effectively restricts the vibration and rotation of CD luminous centers, realizing efficient RTP emission. Density functional theory (DFT) calculations further verified that the N elements enhanced RTP performance. In addition, CDs@phthalamide shows potential application value in time-delayed LEDs and anti-counterfeiting.

Abstract Image

邻苯二胺晶体中原位约束碳点室温磷光机理研究
基于碳点(CD)的室温磷光(RTP)材料由于具有光谱可调性、寿命长等优异的光学性能,在防伪、发光二极管(LED)照明和生物成像等领域有着广泛的应用。但其制备工艺复杂、机理不明确等问题仍存在挑战。在这项工作中,我们开发了一种一步原位液相合成方法,使用邻苯二甲酸,甲酰胺和乙二醇直接形成具有CD/有机晶体结构的RTP CDs@phthalamide复合材料。该产品只需要过滤和干燥,无需进一步的后处理,大大简化了制备程序,便于大规模生产。制备的CDs@phthalamide具有激发依赖性的磷光,其肉眼可见的余辉为5 s,磷光寿命为441 ms。通过优化反应温度和反应时间,通过理论模拟计算活化能,比较酞酰胺和酞亚胺晶体不同晶体结构对发光的影响,研究CDs@phthalamide的形成过程和反应机理。与邻苯二胺不同,邻苯二胺基质有效地限制了CD发光中心的振动和旋转,实现了高效的RTP发射。密度泛函理论(DFT)计算进一步验证了N元素提高了RTP性能。此外,CDs@phthalamide在延时led和防伪方面显示出潜在的应用价值。
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来源期刊
Materials Chemistry Frontiers
Materials Chemistry Frontiers Materials Science-Materials Chemistry
CiteScore
12.00
自引率
2.90%
发文量
313
期刊介绍: Materials Chemistry Frontiers focuses on the synthesis and chemistry of exciting new materials, and the development of improved fabrication techniques. Characterisation and fundamental studies that are of broad appeal are also welcome. This is the ideal home for studies of a significant nature that further the development of organic, inorganic, composite and nano-materials.
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