李虎， 原长洲

济南大学 材料科学与工程学院， 山东 济南 250022

引用格式：

李虎， 原长洲. 葛花衍生的氮掺杂碳点的制备及其应用［J］. 中国粉体技术， 2025， 31（2）： 1-14.

Citation:LI Hu， YUAN Changzhou. Preparation and applications of nitrogen-doped carbon dots derived from flos puerariae［J］. China Powder Science and Technology， 2025， 31（2）： 1-14.

DOI：10.13732/j.issn.1008-5548.2025.02.008

收稿日期： 2024-12-17， 修回日期： 2025-12-25，上线日期： 2025-02-09。

基金项目： 国家自然科学基金项目： 编号： 52171211。

第一作者简介： 李虎（1998—），男，硕士生，研究方向为碳量子点。E-mail：alihu_me@163.com。

通信作者简介： 原长洲（1978—），男，教授，博士，博士生导师， 山东省泰山学者特聘教授， 研究方向为储能材料与器件。E-mail： mse_yuancz@ujn.edu.cn。

摘要： 【目的】 研究制备葛花衍生的碳点在Fe³⁺检测、 隐形荧光墨水和逻辑门运算等方面的应用。 【方法】 采用水热合成法，利用葛花富含蛋白质和酚类物质的性质，以葛花为前驱体，制备氮掺杂的葛花碳点；通过多种表征手段，研究葛花碳点的结构性能、光学性能和稳定性，探讨葛花碳点的离子检测等应用。【结果】 葛花碳点具有良好的分散性和光致发光能力，最佳激发波长为365 nm，发射蓝色荧光，可以作隐形荧光墨水应用；葛花碳点表面拥有大量的官能团，可以利用静态猝灭的方式有效检测Fe³⁺，同时具备良好的抗干扰能力；利用抗坏血酸可以还原Fe³⁺使得荧光恢复的原理，设计的葛花碳点-Fe³⁺-抗坏血酸体系，可用于蕴涵式逻辑门运算。【结论】 成功制备的生物质氮掺杂碳点，可用于Fe³⁺检测、隐形荧光墨水和逻辑门运算等。

关键词：碳量子点；荧光材料；金属离子检测；荧光墨水；逻辑门

Abstract

Objective Excessive Fe³⁺ causes environmental degradation and a decline in human health. Therefore， developing a simple and sensitive method for Fe³⁺ detection is crucial. As a new material for fluorescence-based methods， carbon dots have attracted significant attention due to their high sensitivity， selectivity， and low cost. Flos puerariae， a legume， contains abundant hydroxyl and amino molecules， making it an ideal precursor for carbon dot preparation.

Methods Flos puerariae carbon dots were synthesized via a hydrothermal method. The physicochemical properties and optical performance of these carbon dots were characterized in detail using transmission electron microscopy， X-ray diffraction， Fourier-transform infrared spectroscopy， X-ray photoelectron spectroscopy， ultraviolet-visible （UV-vis） spectrophotometry， and fluorescence spectrophotometry. The morphology， particle size， crystal structure， elemental composition， surface functional groups， photoluminescence properties， and optical stability of these carbon dots were studied. Their application potential in metal ion detection， invisible fluorescent ink， and implication logic gates was systematically investigated. In addition， their fluorescence quenching and reversible recovery mechanisms were studied.

Results and Discussion The flos puerariae carbon dots exhibited an uneven quasi-spherical shape， with a particle size ranging from 1 to 3 nm and an average diameter of 2.52 nm. X-ray diffraction analysis revealed high disorder in these carbon dots. Fourier-transform infrared spectroscopy and X-ray photoelectron spectroscopy revealed that these carbon dots contained abundant carboxyl， hydroxyl， carbonyl， and amino groups， with elemental composition of 67.78% C， 8.41% N， and 23.81% O. Flos puerariae carbon dots exhibited excellent photoluminescence properties and optical stability. The optimal excitation wavelength was 365 nm， and the optimal emission wavelength was 444 nm. The carbon dots maintained good fluorescence stability under long-term 365 nm UV irradiation， varying temperatures， high-ion concentrations， or long-term room temperature storage. Invisible fluorescent ink was prepared using the carbon dot aqueous solution. This ink was used to write words and sailboat patterns， and to spray bird patterns. The handwritten and spray-painted patterns were invisible under normal sunlight but emitted bright blue light and showed clear patterns under 365 nm ultraviolet light. The carbon dots showed obvious concentration dependence and good resistance to pH changes. The fluorescence intensity of the solution was most stable at pH 7 with a 20-fold dilution， which was suitable for metal ion detection. When 13 metal ions and 12 interference components were added to the solution， only Fe³⁺ caused significant fluorescence quenching. The carbon dots exhibited a sensitive concentration response to Fe³⁺ with a limit of detection （LOD） of 1.897 9 μmol/L， which was lower than the national minimum standard in China. Using the Stern-Volmer equation， the interaction between carbon dots and iron ions was found to follow the pattern of static quenching. Moreover， the carbon dots showed strong resistance to interference， with PO₄^3- and ascorbic acid （AA） causing fluorescence recovery. AA completely reduced Fe³⁺ to Fe²⁺， leading to full fluorescence recovery. An implication logic gate was designed based on the reversible fluorescence switching characteristics of flos puerariae carbon dots， demonstrating good reversibility.Conclusion Nitrogen-doped blue fluorescent flos puerariae carbon dots are successfully synthesized using flos puerariae as the precursor. Flos puerariae carbon dots exhibit a quasi-spherical shape and good dispersion， with abundant functional groups on the surface. These carbon dots possess good optical properties and stability， making them suitable for preparing invisible fluorescent ink. Flos puerariae carbon dots demonstrated good selectivity， sensitivity， and anti-interference ability in Fe³⁺ detection. The static quenching caused by Fe³⁺ can be fully restored by AA. Flos puerariae carbon dots have been successfully used to design implication logic gates due to their reversible fluorescence switching characteristics.

Keywords： carbon quantum dot； fluorescent material； metal ion detection； fluorescent ink； logical gate

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