Le Xuan Hung, Pham Thu Nga, Nguyen Thi Mai Huong

Main Article Content

Abstract

In this work, we present a method to fabricate nitrogen-doped Graphene (N-GQDs) and sulfur - nitrogen co-doped graphene quantum dots (S,N-GQDs) and investigate their optical properties. The GQDs are prepared using a microwave-assisted hydrothermal method, which is a simple, environmentally friendly approach that allows for easy dispersion in water and quick application. Structural and morphological analyses reveal that the material has a nanostructure with a size ranging from approximately 4.5 to 9.5 nm and their characteristic bonds are present. The effects of different dopants in GQDs crystal lattice on the optical properties are also systematically analyzed. Additionally, we provide an in-depth discussion of the luminescence mechanism.

Keywords: Graphene quantum dots, N-GQDs, S,N-GQDs, hydrothermal, photoluminescence spectra, EEM.

References

[1] P. Tian, L. Tang, K. S. Teng, S. P. Lau, Graphene Quantum dots from Chemistry to Applications, Materials Today Chemistry, Vol. 10, 2018, pp. 221-258.
[2] Z. Geng, B. H¨ahnlein, R. Granzner, M. Auge, A. A. Lebedev, V. Y. Davydov, M. Kittler, J.o. Pezoldt, F. Schwierz, Graphene Nanoribbons for Electronic Devices, Ann. Phys. (Berlin) Vol. 529, 2017, pp. 1700033.
[3] S. Zhu, Y. Song, X. Zhao, J. Shao, J. Zhang, B. Yang, The Photoluminescence Mechanism in Carbon Dots (Graphene Quantum Dots, Carbon Nanodots, and Polymer Dots): Current State and Future Perspective, Nano Research, Vol. 8, No. 2, 2015, pp. 355–381.
[4] H. Y. Nguyen, X. H. Le, N. T. Dao, N. T. Pham, T. H. H. Vu, N. H. Nguyen, T. N. Pham, Microwave-Assisted Synthesis of Graphene Quantum Dots and Nitrogen-Doped Graphene Quantum Dots: Raman Characterization and Their Optical Properties, Advances in Natural Sciences: Nanoscience and Nanotechnology, Vol. 10, No. 2, 2019, pp. 025005.
[5] Z. Wang, D. Chen, B. Gu, B. Gao, Z. Liu, Y. Yang, Q. Guo, X. Zheng, G. Wang, Yellow Emissive Nitrogen-Doped Graphene Quantum Dots as a Label-Free Fluorescent Probe for Fe3+ Sensing and Bioimaging, Diamond and Related Materials, Vol. 104, 2020.
[6] Z. Fan, Y. Li, X. Li, L. Fan, S. Zhou, D. Fang, S. Yang, Surrounding Media Sensitive Photoluminescence of Boron-Doped Graphene Quantum Dots for Highly Fluorescent Dyed Crystals, Chemical Sensing and Bioimaging, Carbon, Vol. 70, 2014, pp. 149-156.
[7] J. Qian, C. Shen, J. Yan, F. Xi, X. Dong, J. Liu, Tailoring the Electronic Properties of Graphene Quantum Dots by P Doping and Their Enhanced Performance in Metal-Free Composite Photocatalyst, The Journal of Physical Chemistry C, Vol. 122, No. 1, 2017, pp. 349-358.
[8] X. Liu, B. Sun, One-Pot Synthesis of Nitrogen-Doped Graphene Quantum Dots and Their Applications in Bioimaging and Detecting Copper Ions in Living Cells, ACS Omega, Vol. 8, No. 30, 2023, pp. 27333-27343.
[9] S. Bian, C. Shen, H. Hua, L. Zhou, H. Zhu, F. Xi, J. Liu, X. Dong, One-Pot Synthesis of Sulfur-Doped Graphene Quantum Dots as a Novel Fluorescent Probe for Highly Selective and Sensitive Detection of Lead(Ii), RSC Advances, Vol. 6, No. 74, 2016, pp. 69977-69983.
[10] S. Bian, C. Shen, Y. Qian, J. Liu, F. Xi, X. Dong, Facile Synthesis of Sulfur-Doped Graphene Quantum Dots as Fluorescent Sensing Probes for Ag+ Ions Detection, Sensors and Actuators B: Chemical, Vol. 242, 2017, pp. 231-237.
[11] T. Selvakumar, M. Rajaram, A. Natarajan, L. Harikrishnan, K. Alwar, A. Rajaram, Highly Efficient Sulfur and Nitrogen Codoped Graphene Quantum Dots as a Metal-Free Green Photocatalyst for Photocatalysis and Fluorescent Ink Applications, ACS Omega, Vol. 7, No. 15, 2022, pp. 12825-12834.
[12] M. M. Farahani, F. Ghorbani, N. Mosleh, Boric Acid Modified S and N Co-Doped Graphene Quantum Dots as Simple and Inexpensive Turn-On Fluorescent Nanosensor for Quantification of Glucose, Spectrochim Acta a Mol Biomol Spectrosc, Vol. 245, 2021, pp. 118892.
[13] H. S. Hojaghan, O. Amiri, M. Hassanpour, M. P. Kalamuei, H. Moayedi, M. S. Niasari, S,N Co-Doped Graphene Quantum Dots-Induced Ascorbic Acid Fluorescent Sensor: Design, Characterization and Performance, Food Chem, Vol. 295, 2019, pp. 530-536.
[14] S. Sajjadi, A. Khataee, R. Darvishi Cheshmeh Soltani, A. Hasanzadeh, N, S Co-Doped Graphene Quantum Dot–Decorated Fe3O4 Nanostructures: Preparation, Characterization and Catalytic Activity, Journal of Physics and Chemistry of Solids, Vol. 127, 2019, pp. 140-150.
[15] Z. Ouyang, Y. Lei, L. Luo, Z. Jiang, J. Hu, Y. Lin, S, N Co-Doped Graphene Quantum Dots Decorated Cdse for Enhanced Photoelectric Properties, Nanotechnology, Vol. 31, No. 9, 2020, pp. 095710.
[16] L. X. Hung, N. H. Yen, T. T. Hue, D. N. Thuan, P. N. Thang, V. T. H. Hanh, V. C. Nhung,
J. Laverdant, N. T. M. Huong, P. T. Nga, Fabrication and Optical Properties of Sulfur- and Nitrogen-Doped Graphene Quantum Dots by The Microwave–Hydrothermal Approach, Journal of Nanoparticle Research, Vol. 24, No. 10, 2022, pp. 206.
[17] M. T. Hasan, R. G. Rodriguez, C. Ryan, K. Pota, K. Green, J. L. Coffer, A. V. Naumov, Nitrogen-Doped Graphene Quantum Dots: Optical Properties Modification and Photovoltaic Applications, Nano Research, Vol. 12, No. 5, 2019, pp. 1041-1047.
[18] Z. Yang, M. Xu, Y. Liu, F. He, F. Gao, Y. Su, H. Wei, Y. Zhang, Nitrogen-Doped, Carbon-Rich, Highly Photoluminescent Carbon Dots from Ammonium Citrate, Nanoscale, Vol. 6, No. 3, 2014, pp. 1890-1895.
[19] S. S. Dwitya, Y. H. Hsueh, S. S. S. Wang, K. S. Lin, Ultrafine Nitrogen-Doped Graphene Quantum dot Structure and Antibacterial Activities Against Bacillus Subtilis 3610, Materials Chemistry and Physics, Vol. 295, 2023, pp. 127135.
[20] M. He, J. Zhang, H. Wang, Y. Kong, Y. Xiao, W. Xu, Material and Optical Properties of Fluorescent Carbon Quantum Dots Fabricated from Lemon Juice via Hydrothermal Reaction, Nanoscale Res Lett, Vol. 13, No. 1, 2018, pp. 175.
[21] W. Zhu, X. Feng, M. Zhao, Z. Wei, Z. Liu, G. Wang, Q. Guo, D. Chen, Scalable and Atom Economic Preparation of Red-Near-Infrared Emitted N-Doped Graphene Quantum Dots with a High Quantum Yield, Diamond and Related Materials, Vol. 116, 2021, pp. 108395.
[22] Z. Ouyang, Y. Lei, Y. Chen, Z. Zhang, Z. Jiang, J. Hu, Y. Lin, Preparation and Specific Capacitance Properties of Sulfur, Nitrogen Co-Doped Graphene Quantum Dots, Nanoscale Res Lett, Vol. 14, No. 1, 2019, pp. 219.
[23] Y. Su, Y. Zhang, X. Zhuang, S. Li, D. Wu, F. Zhang, X. Feng, Low-Temperature Synthesis of Nitrogen/Sulfur Co-Doped Three-Dimensional Graphene Frameworks as Efficient Metal-Free Electrocatalyst for Oxygen Reduction Reaction, Carbon, Vol. 62, 2013, pp. 296-301.
[24] Z. Yang, Z. Yao, G. Li, G. Fang, H. Nie, Z. Liu, X. Zhou, X.a. Chen, S. Huang, Sulfur-Doped Graphene as an Efficient Metal-free Cathode Catalyst for Oxygen Reduction, ACS Nano, Vol. 6, No. 1, 2012, pp. 205-211.
[25] P. R. Kharangarh, S. Umapathy, G. Singh, Thermal Effect of Sulfur Doping for Luminescent Graphene Quantum Dots, ECS Journal of Solid State Science and Technology, Vol. 7, No. 3, 2018, pp. M29-M34.
[26] P. R. Kharangarh, S. Umapathy, G. Singh, Investigation of Sulfur-Related Defects in Graphene Quantum Dots for Tuning Photoluminescence and High Quantum Yield, Applied Surface Science, Vol. 449, 2018, pp. 363-370.
[27] R. Das, S. Parveen, A. Bora, P. K. Giri, Origin of High Photoluminescence Yield and High SERS Sensitivity of Nitrogen-Doped Graphene Quantum Dots, Carbon, Vol. 160, 2020, pp. 273-286.
[28] S. Kadian, G. Manik, K. Ashish, M. Singh, R. P. Chauhan, Effect of Sulfur Doping on Fluorescence and Quantum Yield of Graphene Quantum Dots: An Experimental and Theoretical Investigation, Nanotechnology, Vol. 30, No. 43, 2019, pp. 435704.
[29] S. Kadian, G. Manik, A Highly Sensitive and Selective Detection of Picric Acid Using Fluorescent Sulfur-Doped Graphene Quantum Dots, Luminescence, Vol. 35, No. 5, 2020, pp. 763-772.
[30] X. Li, S.P. Lau, L. Tang, R. Ji, P. Yang, Sulphur Doping: A Facile Approach to Tune The Electronic Structure and Optical Properties of Graphene Quantum Dots, Nanoscale, Vol. 6, No. 10, 2014, pp. 5323-5328.
[31] S. Kang, Y. K. Jeong, K. H. Jung, Y. Son, W. R. Kim, J. H. Ryu, K. M. Kim, One-Step Synthesis of Sulfur-Incorporated Graphene Quantum Dots Using Pulsed Laser Ablation for Enhancing Optical Properties, Opt Express, Vol. 28, No. 15, 2020, pp. 21659-21667.
[32] T. Vu Tuyet Nhung, H. Van Tuyen, N. Tran, L. Xuan Hung, S, N Co-Doped Graphene Quantum Dots Fabricated by Rapid Microwave-Assisted Pyrolysis and Their Optical Properties, Materials Today Communications, Vol. 37, 2023, pp. 107282.