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通过电化学异质氧化还原反应实现全色发光碳点的表面态调制

Surface State Modulation via Electrochemical Heterogeneous Redox Reactions for Full-Color Emission Carbon Dots.

作者信息

Li Jinli, Sun Chengxiang, Li Qiang, Xu Xiran, Li Baolin, Tian Yijia, Zheng Dianyuan, Yao Rongbin, Yuan Kang, Guo Ziyang

机构信息

Jiangsu Province Engineering Research Center of Electrode Materials for Lithium Batteries, Lianyungang Normal College, Lianyungang, 222006, P. R. China.

School of Science, Jiangsu Ocean University, Lianyungang, 222005, P. R. China.

出版信息

ChemSusChem. 2025 Jan 14;18(2):e202401313. doi: 10.1002/cssc.202401313. Epub 2024 Sep 23.

DOI:10.1002/cssc.202401313
PMID:39087447
Abstract

Carbon dots (CDs) still suffer from unclear surface state fluorescence mechanism for fine modulation. Here, redox reactions for cathode and anode within electrochemical method are firstly employed to construct differentiated strategy for surface-state modulation, so as to obtain CDs with controllable emission in separated electrodes simultaneously. The fluorescence peaks of CDs from blue to red centered at 425 nm (mCDs-), 530 nm (mCDs+), 580 nm (oCDs-) and 665 nm (oCDs+) are mainly originated from the different bombardment effects of the ions and reaction tendencies of modifier during the electrolysis process. The phenylenediamine (as modifier) tends to introduce the amino groups on the surface of CDs- while introduced nitrogen atoms into the carbon nucleus skeleton around the anode, thus leading to much larger size and the formation of the graphite N for CDs+. It is the different surface states formed by phenylenediamine and the absorption redshift triggered by graphite N that ensures the tunable emission. The improved electrochemical method is of great significance for finely spectra modulation and efficient synthesis.

摘要

碳点(CDs)在精细调制方面仍存在表面态荧光机制不明确的问题。在此,首次采用电化学方法中阴极和阳极的氧化还原反应构建表面态调制的差异化策略,从而在分离的电极中同时获得发射可控的碳点。碳点的荧光峰从蓝色到红色,分别位于425 nm(mCDs-)、530 nm(mCDs+)、580 nm(oCDs-)和665 nm(oCDs+),主要源于电解过程中离子的不同轰击效应和修饰剂的反应倾向。对苯二胺(作为修饰剂)倾向于在CDs-表面引入氨基,同时在阳极周围的碳核骨架中引入氮原子,从而导致CDs+的尺寸大得多并形成石墨氮。正是对苯二胺形成的不同表面态以及石墨氮引发的吸收红移确保了发射可调。改进的电化学方法对于精细光谱调制和高效合成具有重要意义。

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