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通过控制氧/氮元素水热合成具有超窄发射的高产率红色荧光碳点

Hydrothermal Synthesis of High-Yield Red Fluorescent Carbon Dots with Ultra-Narrow Emission by Controlled O/N Elements.

作者信息

Xian Yingmei, Li Kang

机构信息

School of Pharmacy, Guangdong Pharmaceutical University, Guangzhou, 510006, China.

出版信息

Adv Mater. 2022 May;34(21):e2201031. doi: 10.1002/adma.202201031. Epub 2022 Apr 28.

Abstract

Red fluorescent carbon dots (r-CDs) with narrow dual emissions (600 nm and 658-683 nm, full width at half-maximums (FWHMs) of 20 nm and 30 nm), fluorescence quantum yield of 41.0%, and yield of 83.3% are prepared by hydrothermal method using o-phenylenediamine as precursor and inorganic oxidant as yield enhancer, and they have graphite nitrate-like structures. The long-wavelength side emission is aggregation-induced emission (AIE). A logarithmic relationship between the AIE wavelength (y) and the concentration (x) (y = 8.853ln(x) + 688.53, R = 0.998) is found. This regularity and the high monochromaticity of AIE are related to the existence of highly ordered structures proved by X-ray diffraction. Its intrinsic emission (FWHM: 20 nm) is the narrowest among the r-CDs prepared by hydrothermal method. The reason is that the decrease of oxygen content makes the FWHMs become narrow, and the decrease of the pyridine nitrogen content and the increase of pyrrole nitrogen content make them narrower further. The Fourier-transform infrared spectra and control experiment prove that oxidative polymerization is a necessary preparation step. The linear relationship between the amount of the oxidant and the CDs yield indicates that the yield can be increased only by increasing the conversion rate of the polymerization process.

摘要

以邻苯二胺为前驱体、无机氧化剂为产率增强剂,通过水热法制备了具有窄双发射(600nm和658 - 683nm,半高宽分别为20nm和30nm)、荧光量子产率为41.0%、产率为83.3%的红色荧光碳点(r-CDs),其具有类石墨硝酸盐结构。长波长侧发射为聚集诱导发射(AIE)。发现AIE波长(y)与浓度(x)之间存在对数关系(y = 8.853ln(x) + 688.53,R = 0.998)。这种规律性以及AIE的高单色性与X射线衍射证明的高度有序结构的存在有关。其本征发射(半高宽:20nm)是水热法制备的r-CDs中最窄的。原因是氧含量的降低使半高宽变窄,吡啶氮含量的降低和吡咯氮含量的增加使其进一步变窄。傅里叶变换红外光谱和对照实验证明氧化聚合是必要的制备步骤。氧化剂用量与碳点产率之间的线性关系表明,只有提高聚合过程的转化率才能提高产率。

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