Hostname: page-component-76fb5796d-vvkck Total loading time: 0 Render date: 2024-04-26T13:48:07.696Z Has data issue: false hasContentIssue false

Preparation of multicolored carbon quantum dots using HNO3/HClO4 oxidation of graphitized carbon

Published online by Cambridge University Press:  16 September 2019

Chao Tan
Affiliation:
College of Chemical Engineering, Jiangsu Provincial Key Lab for the Chemistry and Utilization of Agro-forest Biomass, Nanjing Forestry University, Nanjing 210037, China
Songlin Zuo*
Affiliation:
College of Chemical Engineering, Jiangsu Provincial Key Lab for the Chemistry and Utilization of Agro-forest Biomass, Nanjing Forestry University, Nanjing 210037, China
Yunyang Zhao
Affiliation:
Institute of Applied Physics and Materials Engineering, Joint Key Laboratory of the Ministry of Education, University of Macau, Macau 999078, China
Baoshou Shen
Affiliation:
Department of Environmental Engineering, College of Urban and Environmental Sciences Northwest University, Xi’an 710127, China
*
a)Address all correspondence to this author. e-mail: zslnl@njfu.com.cn
Get access

Abstract

The microstructure of carbon quantum dots (CQDs) has a great influence on their fluorescence properties. Here, different microstructures of CQDs were synthesized by the selective oxidation of graphitized activated carbon using HNO3/HClO4 as the oxidant. We characterized the microstructure and surface chemistry of the CQDs, and the results show that the degree of graphitization of activated carbon has a significant effect on the structure and fluorescence properties of the obtained CQDs. The fluorescence of the CQD solution can be tuned from yellow to green by regulating the degree of graphitization of the activated carbon by heat treatment at high temperature (up to 2500 °C). Moreover, the increased degree of graphitization of the raw carbon precursor is beneficial for significantly reducing the fluorescence self-absorption quenching of the concentrated CQD solution. Importantly, the as-prepared CQDs have no cytotoxicity and can be used as bioimaging agents.

Type
Article
Copyright
Copyright © Materials Research Society 2019 

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

Xu, X., Ray, R., Gu, Y., Ploehn, H.J., Gearheart, L., Raker, K., and Scrivens, W.A.: Electrophoretic analysis and purification of fluorescent single-walled carbon nanotube fragments. J. Am. Chem. Soc. 126, 12736 (2004).CrossRefGoogle ScholarPubMed
Hua, J., Yang, J., Zhu, Y., Zhao, C., and Yang, Y.: Highly fluorescent carbon quantum dots as nanoprobes for sensitive and selective determination of mercury(II) in surface waters. Spectrochim. Acta. Part A. 187, 149 (2017).CrossRefGoogle Scholar
Zhuang, Q., Guo, P., Zheng, S., Lin, Q., Lin, Y., Wang, Y., and Ni, Y.: Green synthesis of luminescent graphitic carbon nitride quantum dots from human urine and its bioimaging application. Talanta 188, 35 (2018).CrossRefGoogle ScholarPubMed
Ding, H., Du, F., Liu, P., Chen, Z., and Shen, J.: DNA–carbon dots function as fluorescent vehicles for drug delivery. ACS Appl. Mater. Interfaces. 7, 6889 (2015).CrossRefGoogle ScholarPubMed
Dong, Y., Shao, J., Chen, C., Li, H., Wang, R., Chi, Y., and Chen, G.: Blue luminescent graphene quantum dots and graphene oxide prepared by tuning the carbonization degree of citric acid. Carbon 50, 4738 (2012).CrossRefGoogle Scholar
Pei, S., Zhang, J., Gao, M., Wu, D., Yang, Y., and Liu, R.: A facile hydrothermal approach towards photoluminescent carbon dots from amino acids. J. Colloid Interface Sci. 439, 129 (2015).CrossRefGoogle ScholarPubMed
Yang, Z.C., Wang, M., Yong, A.M., Wong, S.Y., Zhang, X.H., Tan, H., and Wang, J.: Intrinsically fluorescent carbon dots with tunable emission derived from hydrothermal treatment of glucose in the presence of monopotassium phosphate. Chem. Commun. 47, 11615 (2011).CrossRefGoogle ScholarPubMed
Zhou, J., Lin, P., Ma, J., Shan, X., Feng, H., Chen, C., and Qian, C.: Facile synthesis of halogenated carbon quantum dots as an important intermediate for surface modification. RSC Adv. 3, 9625 (2013).CrossRefGoogle Scholar
Liu, Q., Zhang, N., Shi, H., Ji, W., Guo, X., Yuan, W., and Hu, Q.: One-step microwave synthesis of carbon dots for highly sensitive and selective detection of copper ions in aqueous solution. New J. Chem. 42, 3097 (2018).CrossRefGoogle Scholar
Qiao, Z.A., Wang, Y., Gao, Y., Li, H., Dai, T., Liu, Y., and Huo, Q.: Ommercially activated carbon as the source for producing multicolor photoluminescent carbon dots by chemical oxidation. Chem. Commun. 46, 8812 (2010).CrossRefGoogle ScholarPubMed
Liu, M., Xu, Y., Niu, F., Gooding, J.J., and Liu, J.: Carbon quantum dots directly generated from electrochemical oxidation of graphite electrodes in alkaline alcohols and the applications for specific ferric ion detection and cell imaging. Analyst 141, 2657 (2016).CrossRefGoogle ScholarPubMed
Hu, S., Liu, J., Yang, J., Wang, Y., and Cao, S.: Laser synthesis and size tailor of carbon quantum dots. J. Nanopart. Res. 13, 7247 (2011).CrossRefGoogle Scholar
Xu, J., Sahu, S., Cao, L., Anilkumar, P., Tackett, K.N., Qian, H., and Sun, Y.P.: Carbon nanoparticles as chromophores for photon harvesting and photoconversion. ChemPhysChem 12, 3604 (2011).CrossRefGoogle ScholarPubMed
Loh, K.P., Bao, Q., Eda, G., and Chhowalla, M.: Graphene oxide as a chemically tunable platform for optical applications. Nat. Chem. 2, 1015 (2010).CrossRefGoogle ScholarPubMed
Zhu, S., Song, Y., Wang, J., Wan, H., Zhang, Y., Ning, Y., and Yang, B.: Photoluminescence mechanism in graphene quantum dots: Quantum confinement effect and surface/edge state. Nano Today 13, 10 (2017).CrossRefGoogle Scholar
Liang, Z., Zeng, L., Cao, X., Wang, Q., Wang, X., and Sun, R.: Sustainable carbon quantum dots from forestry and agricultural biomass with amplified photoluminescence by simple NH4OH passivation. J. Mater. Chem. C. 2, 9760 (2014).CrossRefGoogle Scholar
Zheng, H., Wang, Q., Long, Y., Zhang, H., Huang, X., and Zhu, R.: Enhancing the luminescence of carbon dots with a reduction pathway. Chem. Commun. 47, 10650 (2011).CrossRefGoogle ScholarPubMed
Yeh, T.F., Teng, C.Y., Chen, S.J., and Teng, H.: Nitrogen-doped graphene oxide quantum dots as photocatalysts for overall water-splitting under visible light illumination. Adv. Mater. 26, 3297 (2014).CrossRefGoogle ScholarPubMed
Dong, Y., Pang, H., Yang, H.B., Guo, C., Shao, J., Chi, Y., and Yu, T.: Carbon-based dots co-doped with nitrogen and sulfur for high quantum yield and excitation-independent emission. Angew. Chem. 125, 7954 (2013).CrossRefGoogle Scholar
Chandra, S., Mitra, S., Laha, D., Bag, S., Das, P., Goswami, A., and Pramanik, P.: Fabrication of multi-structure nanocarbons from carbon xerogel: A unique scaffold towards bio-imaging. Chem. Commun. 30, 8587 (2011).CrossRefGoogle Scholar
Wu, M., Wang, Y., Wu, W., Hu, C., Wang, X., Zheng, J., and Qiu, J.: Preparation of functionalized water-soluble photoluminescent carbon quantum dots from petroleum coke. Carbon 78, 480 (2014).CrossRefGoogle Scholar
Liu, H., Ye, T., and Mao, C.: Fluorescent carbon nanoparticles derived from candle soot. Angew. Chem. 119, 6593 (2007).CrossRefGoogle Scholar
Dong, Y., Lin, J., Chen, Y., Fu, F., Chi, Y., and Chen, G.: Graphene quantum dots, graphene oxide, carbon quantum dots and graphite nanocrystals in coals. Nanoscale 6, 7410 (2014).CrossRefGoogle ScholarPubMed
Hu, C., Yu, C., Li, M., Wang, X., Yang, J., Zhao, Z., and Qiu, J.: Chemically tailoring coal to fluorescent carbon dots with tuned size and their capacity for Cu(II) detection. Small 10, 4926 (2014).CrossRefGoogle ScholarPubMed
Kang, M., Bae, Y.S., and Lee, C.H.: Effect of heat treatment of activated carbon supports on the loading and activity of Pt catalyst. Carbon 43, 1512 (2005).CrossRefGoogle Scholar
Feng, B., Bhatia, S.K., and Barry, J.C.: Structural ordering of coal char during heat treatment and its impact on reactivity. Carbon 40, 481 (2002).CrossRefGoogle Scholar
Miao, M., Zuo, S., Zhao, Y., Wang, Y., Xia, H., Tan, C., and Gao, H.: Selective oxidation rapidly decomposes biomass-based activated carbons into graphite-like crystallites. Carbon 140, 504 (2018).CrossRefGoogle Scholar
Zhao, J., Yang, L., Li, F., Yu, R., and Jin, C.: Structural evolution in the graphitization process of activated carbon by high-pressure sintering. Carbon 47, 744 (2009).CrossRefGoogle Scholar
Kumar, U., Gaikwad, V., Mayyas, M., Sahajwalla, V., and Joshi, R.K.: Extraordinary supercapacitance in activated carbon produced via a sustainable approach. J. Power Sources 394, 140 (2018).CrossRefGoogle Scholar
Li, Y., Hu, Y., Zhao, Y., Shi, G., Deng, L., Hou, Y., and Qu, L.: An electrochemical avenue to green-luminescent graphene quantum dots as potential electron-acceptors for photovoltaics. Adv. Mater. 23, 776 (2011).CrossRefGoogle ScholarPubMed
Xu, Y.J., Weinberg, G., Liu, X., Timpe, O., Schlögl, R., and Su, D.S.: Nanoarchitecturing of activated carbon: Facile strategy for chemical functionalization of the surface of activated carbon. Adv. Funct. Mater. 18, 3613 (2008).CrossRefGoogle Scholar
Zhu, S., Zhang, J., Tang, S., Qiao, C., Wang, L., Wang, H., and Wang, X.: Surface chemistry routes to modulate the photoluminescence of graphene quantum dots: From fluorescence mechanism to up-conversion bioimaging applications. Adv. Funct. Mater. 22, 4732 (2012).CrossRefGoogle Scholar
Cheng, H.N., Wartelle, L.H., Klasson, K.T., and Edwards, J.C.: Solid-state NMR and ESR studies of activated carbons produced from pecan shells. Carbon 48, 2455 (2010).CrossRefGoogle Scholar
Chen, L.S., Wang, L.L., Pan, T.Y., Yang, Z.H.O.U., Zhang, Y.Y., and Zhang, D.X.: Calibration of solid state NMR carbon structural parameters and application in coal structure analysis. J. Fuel Chem. Technol. 45, 1153 (2017).CrossRefGoogle Scholar
Zhu, S., Zhang, J., Qiao, C., Tang, S., Li, Y., Yuan, W., and Gao, H.: Strongly green-photoluminescent graphene quantum dots for bioimaging applications. Chem. Commun. 47, 6858 (2011).CrossRefGoogle ScholarPubMed
Wang, C., Hu, T., Wen, Z., Zhou, J., Wang, X., Wu, Q., and Wang, C.: Concentration-dependent color tunability of nitrogen-doped carbon dots and their application for iron(III) detection and multicolor bioimaging. J. Colloid Interface Sci. 521, 33 (2018).CrossRefGoogle ScholarPubMed
Eda, G., Lin, Y.Y., Mattevi, C., Yamaguchi, H., Chen, H.A., Chen, I.S., and Chhowalla, M.: Blue photoluminescence from chemically derived graphene oxide. Adv. Mater. 22, 505 (2010).CrossRefGoogle ScholarPubMed
Wu, C., Wang, C., Han, T., Zhou, X., Guo, S., and Zhang, J.: Insight into the cellular internalization and cytotoxicity of graphene quantum dots. Adv. Healthcare Mater. 2, 1613 (2013).CrossRefGoogle ScholarPubMed
Zhang, C., Cui, Y., Song, L., Liu, X., and Hu, Z.: Microwave assisted one-pot synthesis of graphene quantum dots as highly sensitive fluorescent probes for detection of iron ions and pH value. Talanta 150, 54 (2016).CrossRefGoogle ScholarPubMed
Supplementary material: File

Tan et al. supplementary material

Figures S1-S5 and Tables S1-S4

Download Tan et al. supplementary material(File)
File 31 MB