CDs/SiO2复合荧光粉的制备与优化
Design of CDs/SiO2 Composite Phosphors
DOI: 10.12677/ms.2026.162037, PDF,    科研立项经费支持
作者: 刘 杨, 王 睿, 张 蕾, 孙明烨*:牡丹江师范学院物理与电子工程学院,黑龙江 牡丹江
关键词: 碳点固态发光二氧化硅溶胶凝胶法聚乙烯吡咯烷酮CDs Solid-State Luminescence SiO2 Sol-Gel Method PVP
摘要: 本文研究思路如下,采用溶剂热法制成多色碳点(CDs),采用溶胶–凝胶法制备出碳点–二氧化硅(CDs/SiO2)复合荧光粉。另外,为了优化CDs/SiO2复合荧光粉的发光强度,引入了聚乙烯吡咯烷酮(PVP)作为表面活性剂,通过正硅酸乙酯(TEOS)的水解缩合反应,将CDs嵌入SiO2基质中。PVP的引入有效调控了复合荧光粉的微观结构和界面特性,其分子链上的C=O、C-N等官能团不仅能通过空间位阻效应防止碳点团聚,更能与硅羟基前驱体形成强氢键,引导SiO2在CDs表面进行异相成核与生长,显著抑制了TEOS的均相成核现象。
Abstract: The research methodology is as follows: Multicolor carbon dots (CDs) were synthesized via a solvothermal method. CDs/SiO2 composite phosphors were subsequently prepared using a sol-gel process. Furthermore, to enhance the luminescence intensity of the CDs/SiO2 composite phosphors, polyvinylpyrrolidone (PVP) was introduced as a surfactant. Through the hydrolysis and condensation of tetraethyl orthosilicate (TEOS), the CDs were embedded within the SiO2 matrix. The incorporation of PVP effectively regulates the microstructure and interfacial properties of the composite. The functional groups such as C=O and C-N on the PVP molecular chains not only prevent the aggregation of CDs via steric hindrance but also form strong hydrogen bonds with the silanol precursors. This interaction guides the heterogeneous nucleation and growth of SiO2 on the CD surfaces, significantly suppressing the homogeneous nucleation of TEOS.
文章引用:刘杨, 王睿, 张蕾, 孙明烨. CDs/SiO2复合荧光粉的制备与优化[J]. 材料科学, 2026, 16(2): 183-192. https://doi.org/10.12677/ms.2026.162037

参考文献

[1] Mandal, S., Pal, J., Subramanian, R. and Das, P. (2020) Amplified Fluorescence of Mg2+ Selective Red-Light Emitting Carbon Dot in Water and Direct Evaluation of Creatine Kinase Activity. Nano Research, 13, 2770-2776. [Google Scholar] [CrossRef
[2] Ji, C., Zhou, Y., Leblanc, R.M. and Peng, Z. (2020) Recent Developments of Carbon Dots in Biosensing: A Review. ACS Sensors, 5, 2724-2741. [Google Scholar] [CrossRef] [PubMed]
[3] Ghosh, S., Ali, H. and Jana, N.R. (2019) Water Dispersible Red Fluorescent Carbon Nanoparticles via Carbonization of Resorcinol. ACS Sustainable Chemistry & Engineering, 7, 12629-12637. [Google Scholar] [CrossRef
[4] Miao, S., Liang, K., Zhu, J., Yang, B., Zhao, D. and Kong, B. (2020) Hetero-Atom-Doped Carbon Dots: Doping Strategies, Properties and Applications. Nano Today, 33, Article ID: 100879. [Google Scholar] [CrossRef
[5] Gao, M., Zeng, J., Liang, K., Zhao, D. and Kong, B. (2020) Interfacial Assembly of Mesoporous Silica‐Based Optical Heterostructures for Sensing Applications. Advanced Functional Materials, 30, Article ID: 1906950. [Google Scholar] [CrossRef
[6] Kong, B., Tang, J., Zhang, Y., Jiang, T., Gong, X., Peng, C., et al. (2015) Incorporation of Well-Dispersed Sub-5-nm Graphitic Pencil Nanodots into Ordered Mesoporous Frameworks. Nature Chemistry, 8, 171-178. [Google Scholar] [CrossRef] [PubMed]
[7] Holá, K., Sudolská, M., Kalytchuk, S., Nachtigallová, D., Rogach, A.L., Otyepka, M., et al. (2017) Graphitic Nitrogen Triggers Red Fluorescence in Carbon Dots. ACS Nano, 11, 12402-12410. [Google Scholar] [CrossRef] [PubMed]
[8] Ghosh, S., Ghosh, A., Ghosh, G., Marjit, K. and Patra, A. (2021) Deciphering the Relaxation Mechanism of Red-Emitting Carbon Dots Using Ultrafast Spectroscopy and Global Target Analysis. The Journal of Physical Chemistry Letters, 12, 8080-8087. [Google Scholar] [CrossRef] [PubMed]
[9] Xu, Q., Kuang, T., Liu, Y., Cai, L., Peng, X., Sreenivasan Sreeprasad, T., et al. (2016) Heteroatom-Doped Carbon Dots: Synthesis, Characterization, Properties, Photoluminescence Mechanism and Biological Applications. Journal of Materials Chemistry B, 4, 7204-7219. [Google Scholar] [CrossRef] [PubMed]
[10] Kong, J., Wei, Y., Zhou, F., Shi, L., Zhao, S., Wan, M., et al. (2024) Carbon Quantum Dots: Properties, Preparation, and Applications. Molecules, 29, Article No. 2002. [Google Scholar] [CrossRef] [PubMed]
[11] Qu, S., Zhou, D., Li, D., Ji, W., Jing, P., Han, D., et al. (2016) Toward Efficient Orange Emissive Carbon Nanodots through Conjugated Sp2‐Domain Controlling and Surface Charges Engineering. Advanced Materials, 28, 3516-3521. [Google Scholar] [CrossRef] [PubMed]
[12] Rajakumar, G., Zhang, X., Gomathi, T., Wang, S., Azam Ansari, M., Mydhili, G., et al. (2020) Current Use of Carbon-Based Materials for Biomedical Applications—A Prospective and Review. Processes, 8, Article No. 355. [Google Scholar] [CrossRef
[13] Yadav, P.K., Chandra, S., Kumar, V., Kumar, D. and Hasan, S.H. (2023) Carbon Quantum Dots: Synthesis, Structure, Properties, and Catalytic Applications for Organic Synthesis. Catalysts, 13, Article No. 422. [Google Scholar] [CrossRef
[14] Zhan, Y., Shang, B., Chen, M. and Wu, L. (2019) One‐Step Synthesis of Silica‐Coated Carbon Dots with Controllable Solid‐State Fluorescence for White Light‐Emitting Diodes. Small, 15, Article ID: 1901161. [Google Scholar] [CrossRef] [PubMed]
[15] Li, X., Zhang, S., Kulinich, S.A., Liu, Y. and Zeng, H. (2014) Engineering Surface States of Carbon Dots to Achieve Controllable Luminescence for Solid-Luminescent Composites and Sensitive Be2+ Detection. Scientific Reports, 4, 2584-2860. [Google Scholar] [CrossRef
[16] Raabe, G. and Michl, J. (1985) Multiple Bonding to Silicon. Chemical Reviews, 85, 419-509. [Google Scholar] [CrossRef
[17] Pham, X., Park, S., Ham, K., Kyeong, S., Son, B.S., Kim, J., et al. (2021) Synthesis and Application of Silica-Coated Quantum Dots in Biomedicine. International Journal of Molecular Sciences, 22, Article No. 10116. [Google Scholar] [CrossRef] [PubMed]
[18] Dixit, C.K., Bhakta, S., Kumar, A., Suib, S.L. and Rusling, J.F. (2016) Fast Nucleation for Silica Nanoparticle Synthesis Using a Sol-Gel Method. Nanoscale, 8, 19662-19667. [Google Scholar] [CrossRef] [PubMed]
[19] Chen, C., Wang, H., Xue, Y., Xue, Z., Liu, H., Xie, X., et al. (2016) Structure, Rheological, Thermal Conductive and Electrical Insulating Properties of High-Performance Hybrid Epoxy/Nanosilica/AgNWs Nanocomposites. Composites Science and Technology, 128, 207-214. [Google Scholar] [CrossRef
[20] Ye, L., Zhang, Y., Song, C., Li, Y. and Jiang, B. (2017) A Simple Sol-Gel Method to Prepare Superhydrophilic Silica Coatings. Materials Letters, 188, 316-318. [Google Scholar] [CrossRef
[21] Cannavale, A., Fiorito, F., Manca, M., Tortorici, G., Cingolani, R. and Gigli, G. (2010) Multifunctional Bioinspired Sol-Gel Coatings for Architectural Glasses. Building and Environment, 45, 1233-1243. [Google Scholar] [CrossRef
[22] Harris, M.T., Brunson, R.R. and Byers, C.H. (1990) The Base-Catalyzed Hydrolysis and Condensation Reactions of Dilute and Concentrated TEOS Solutions. Journal of Non-Crystalline Solids, 121, 397-403. [Google Scholar] [CrossRef
[23] Ziaei-Azad, H. and Semagina, N. (2014) Bimetallic Catalysts: Requirements for Stabilizing PVP Removal Depend on the Surface Composition. Applied Catalysis A: General, 482, 327-335. [Google Scholar] [CrossRef
[24] Jadhav, S.V., Nikam, D.S., Khot, V.M., Thorat, N.D., Phadatare, M.R., Ningthoujam, R.S., et al. (2013) Studies on Colloidal Stability of PVP-Coated LSMO Nanoparticles for Magnetic Fluid Hyperthermia. New Journal of Chemistry, 37, 3121-3130. [Google Scholar] [CrossRef
[25] Lu, G., Li, S., Guo, Z., Farha, O.K., Hauser, B.G., Qi, X., et al. (2012) Imparting Functionality to a Metal-Organic Framework Material by Controlled Nanoparticle Encapsulation. Nature Chemistry, 4, 310-316. [Google Scholar] [CrossRef] [PubMed]
[26] Koczkur, K.M., Mourdikoudis, S., Polavarapu, L. and Skrabalak, S.E. (2015) Polyvinylpyrrolidone (PVP) in Nanoparticle Synthesis. Dalton Transactions, 44, 17883-17905. [Google Scholar] [CrossRef] [PubMed]
[27] Sun, M.Y., Han, Y., Yuan, X., Jing, P.T., Zhang, L., Zhao, J.L. and Zheng, Y.J. (2020) Efficient Full-Color Emitting Carbon-Dot-Based Composite Phosphors by Chemical Dispersion. Nanoscale, 10, 1622-1630.
[28] Wang, S.J., Colec, I.S., Zhao, D.Y. and Li, Q. (2012) The Duo Roles of Functional Groups in the Photoluminescence of Graphene Quantum Dots, RSC Publishing.
[29] Zhu, J., Zhao, H., Yang, Y., Wu, W., Hu, L., Wei, Y., et al. (2024) Photo-Stimulus-Responsive Dual-Emitting Fluorescence of Spiropyran-Encapsulated Carbon Dots-Functionalized Silicon Dioxide for Dynamic Information Encryption. Science China Materials, 67, 680-689. [Google Scholar] [CrossRef
[30] Cohen Stuart, M.A., Fleer, G.J. and Bijsterbosch, B.H. (1982) The Adsorption of Poly(Vinyl Pyrrolidone) Onto Silica. I. Adsorbed Amount. Journal of Colloid and Interface Science, 90, 310-320. [Google Scholar] [CrossRef
[31] Van de Steeg, H.G.M., Cohen Stuart, M.A., De Keizer, A. and Bijsterbosch, B.H. (1992) Polyelectrolyte Adsorption: A Subtle Balance of Forces. Langmuir, 8, 2538-2546. [Google Scholar] [CrossRef
[32] Gun’ko, V.M., Zarko, V.I., Voronin, E.F., Goncharuk, E.V., Andriyko, L.S., Guzenko, N.V., et al. (2006) Successive Interaction of Pairs of Soluble Organics with Nanosilica in Aqueous Media. Journal of Colloid and Interface Science, 300, 20-32. [Google Scholar] [CrossRef] [PubMed]
[33] Ai, L., Yang, Y., Wang, B., Chang, J., Tang, Z., Yang, B., et al. (2021) Insights into Photoluminescence Mechanisms of Carbon Dots: Advances and Perspectives. Science Bulletin, 66, 839-856. [Google Scholar] [CrossRef] [PubMed]