Korean Chemical Engineering Research

The Korean Institute of Chemical Engineers (한국화학공학회)
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Photocatalytic Degradation and Adsorptive Removal of Tetracycline on Amine-Functionalized Graphene Oxide/ZnO Nanocomposites

  • Received : 2023.08.30
  • Accepted : 2023.10.05
  • Published : 2023.11.01
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Abstract

Due to the rapid development of the livestock industry, particularly due to residual pharmaceutical antibiotics, environmental populations have been negatively affected. Herein, we report a ZnO/melamine-functionalized carboxylic-rich graphene oxide (ZFG) photocatalyst for visible light-driven photocatalytic degradation of tetracycline hydrochloride in aqueous solutions. The properties of the photocatalysts were evaluated by XRD, FTIR, XPS, Fe-SEM, HR-TEM, TGA, Raman spectroscopy, UV-Vis spectroscopy, zeta potential, and electrochemical measurements. The photocatalytic activity was measured using high-performance liquid chromatography. The photocatalytic properties of the ZFG photocatalyst evaluated against the tetracycline hydrochloride (TCH) antibiotic under visible light irradiation showed superior photodegradation of 96.27% within 60 min at an initial pH of 11. The enhancement of photocatalytic degradation was due to the introduction of functionalized graphene, which increases the light-harvesting capability and molecular adsorption capability in addition to minimizing the recombination rate of photogenerated charge carriers due to its role as an electron acceptor and mediator.

Keywords

Acknowledgement

This study was supported by the Regional Innovation Strategy (RIS) through the Ministry of Education (MOE) (2021RIS-003).

References

  1. Zhou, C., Lai, C., Xu, P., Zeng, G., Huang, D., Li, Z., Zhang, C., Cheng, M., Hu, L., Wan, J., Chen, F., Xiong, W. and Deng, R., "Rational Design of Carbon-Doped Carbon Nitride/Bi12O17Cl2 Composites: A Promising Candidate Photocatalyst for Boosting Visible-Light-Driven Photocatalytic Degradation of Tetracycline," ACS Sustainable Chemistry & Engineering, 6, 6941-6949 (2018). https://doi.org/10.1021/acssuschemeng.8b00782
  2. Chen, X., Xu, X., Cui, J., Chen, C., Zhu, X., Sun, D. and Sun, D., "Visible-light Driven Degradation of Tetracycline Hydrochloride and 2,4-dichlorophenol Byfilm-like N-carbon@N-ZnO Catalyst with Three-dimensional Interconnected Nanofibrous Structure," J. Hazardous Materials, 392, 122331(2020).
  3. Tung, M. H. T., Cam, N. T. D., Thuan, D. V., Quan, P. V., Hoang, C. V., Phuong, T. T. T., Lam, N. T., Tam, T. T., Chi, N. T. P. L., Lan, N. T., Thoai, D. N. and Pham, T.-D., "Novel Direct Z-scheme AgI/N-TiO2 Photocatalyst for Removal of Polluted Tetracycline Under Visible Irradiation," Ceramics International, 46, 6012-6021(2020). https://doi.org/10.1016/j.ceramint.2019.11.058
  4. Chen, G., Yu, Y., Liang, L., Duan, X., Li, R., Lu, X., Yan, B., Li, N. and Wang, S., "Remediation of Antibiotic Wastewater by Coupled Photocatalytic and Persulfate Oxidation System: A Critical Review," J. Hazardous Materials, 408,124461(2020).
  5. Saadati, F., Keramati, N. and Ghazi, M. M., "Influence of Parameters on the Photocatalytic Degradation of Tetracycline in Wastewater: A Review," Critical Reviews in Environmental Science and Technology, 46, 757-782(2016). https://doi.org/10.1080/10643389.2016.1159093
  6. Das, P., Pan, A., Chakraborty, K., Pal, T. and Ghosh, S., "RGO-ZnSe Photocatalyst towards Solar-Light-Assisted Degradation of Tetracycline Antibiotic Water Pollutant," ChemistrySelect, 3, 10214-10219(2018). https://doi.org/10.1002/slct.201801657
  7. Thi, V. H. T. and Lee, B.-K., "Great Improvement on Tetracycline Removal Using ZnO Rod-activated Carbon Fiber Composite Prepared with a Facile Microwave Method," J. Hazardous Materials, 324, 329-339(2017).
  8. Zhao, C., Hong, P., Li, Y., Song, X., Wang, Y. and Yang, Y., "Mechanism of Adsorption of Tetracycline-Cu Multi-pollutants by Graphene Oxide Mechanism of Adsorption of Tetracycline-Cu Multi-pollutants by Graphene Oxide," J. Chemical Technology and Biotechnology, 94, 1176-1186(2019). https://doi.org/10.1002/jctb.5864
  9. Du, Q., Wu, P., Sun, Y., Zhang, J. and He, H., "Selective Photodegradation of Tetracycline by Molecularly Imprinted ZnO@Selective Photodegradation of Tetracycline by Molecularly Imprinted ZnO@," Chemical Engineering J., 390, 129350(2020).
  10. Yan, X., Yan, X., Ning, G., Li, J., Ai, T., Su, X. and Wang, Z., "A Novel Poly(triazine imide) Hollow Tube/ZnO Heterojunction for Tetracycline Hydrochloride Degradation Under Visible Light Irradiation," Advanced Powder Technology, 30, 359-365(2019). https://doi.org/10.1016/j.apt.2018.11.013
  11. Xu, F., Yuan, Y., Wu, D., Zhao, M., Gao, Z. and Jiang, K., "Synthesis of ZnO/Ag/graphene Composite and its Enhanced Photocatalytic Efficiency," Materials Research Bulletin, 48, 2066-2070(2013). https://doi.org/10.1016/j.materresbull.2013.02.034
  12. Thinh, D. B., Tien, N. T., Dat, N. M., Phong, H. H. T., Giang, N. T. H., Tai, L. T., Oanh, D. T. Y., Nam, H. M., Phong, M. T. and Hieu, N. H., "Improved Photodegradation of p-nitrophenol From Water Media Using Ternary MgFe2O4-doped TiO2/reduced Graphene Oxide," Synthetic Metals, 270, 116583(2020).
  13. Zhu, P., Chen, Y., Duan, M., Liu, M., Zou, P. and Zhou, M., "Enhanced Visible Photocatalytic Activity of Fe-Cu-ZnO/Graphene Oxide Photocatalysts for the Degradation of Organic Dyes," Canadian J. Chemical Engineering, 96, 1479-1488(2018). https://doi.org/10.1002/cjce.23109
  14. Sharma, P., Kumar, N., Chauhan, R., Singh, V., Srivastava, V. C., Sharma, P., Kumar, N., Chauhan, R., Singh, V. and Srivastava, V. C., "Growth of Hierarchical ZnO Nano Flower on Large Functionalized rGO Sheet for Superior Photocatalytic Mineralization of Antibiotic," Chemical Engineering J., 392, 123746(2020).
  15. Anirudhan, T. S. and Deepa, J. R., "Nano-zinc Oxide Incorporated Graphene Oxide/nanocellulose Composite for the Adsorption and Photo Catalytic Degradation of Ciprofloxacin Hydrochloride From Aqueous Solutions," J. Colloid and Interface Science, 490, 343-356(2017). https://doi.org/10.1016/j.jcis.2016.11.042
  16. Munawar, T., Mukhtar, F., Nadeem, M. S., Mahmood, K., Hussain, A., Ali, A., Arshad, M. I., un Nabi, M. A. and un Nabi, M. A., "Structural, Optical, Electrical, and Morphological Studies of rGO Anchored Direct Dual-Z-Scheme ZnO-Sm2O3-Y2O3 Heterostructured Nanocomposite: Direct Dual-Z-scheme ZnO-Sm2O3-Y2O0 Heterostructured Nanocomposite," Solid State Sciences, 106, 106307(2020).
  17. Jesus, J. L.-P., Manuel, S.-P., Carla, V. G.-P., Jose, R.-U., "Photodegradation of Tetracyclines in Aqueous Solution by Using UV and UV/H2O2 Oxidation Processes," J. Chemical Technology and Biotechnology, 85, 1325-1333(2010). https://doi.org/10.1002/jctb.2435
  18. Alireza, N.-E. and Arezoo, S., "Enhancement of the Photocatalytic Activity of Ferrous Oxide by Doping Onto the Nanoclinoptilolite Particles Towards Photodegradation of Tetracycline," Chemosphere, 107, 136-144(2014). https://doi.org/10.1016/j.chemosphere.2014.02.015
  19. Zyoud, A. H., Zubi, A., Zyoud, S. H., Hilal, M. H., Zyoud, S., Qamhieh, N., Hajamohideen, A. and Hajamohideen, A., "Kaolinsupported ZnO Nanoparticle Catalysts in Self-sensitized Tetracycline Photodegradation: Zero-point Charge and pH Effects," Applied Clay Science, 182, 105294(2019).
  20. Demircivi, P. and Demircivi, P., "Visible-light-enhanced Photoactivity of Perovskite-type W-doped BaTiO3 Photocatalyst for Photodegradation of Tetracycline," J. Alloys and Compounds, 774, 795-802(2019). https://doi.org/10.1016/j.jallcom.2018.09.354
  21. Ashok Kumar, K. V., Lakshminarayana, B, Suryakala, D. and Subrahmanyam, Ch., "Reduced Graphene Oxide Supported ZnO Quantum Dots for Visible Light-induced Simultaneous Removal of Tetracycline and Hexavalent Chromium," RSC Advances, 10, 20494-20503(2020). https://doi.org/10.1039/D0RA02062A
  22. Wu, F., Zhou, F., Zhu, Z., Zhan, S. and He, Q., "Enhanced Photocatalytic Activities of Ag3PO4/GO in Tetracycline Degradation," Chemical Physics Letters, 724, 90-95(2020).
  23. Abdel-Mottaleb, M. M., Khalil, A., Karim, S. A., Osman, T. A., and Khattab, A., "High Performance of PAN/GO-ZnO Composite Nanofibers for Photocatalytic Degradation Under Visible Irradiation," J. of the Mechanical Behavior of Biomedical Materials, 96, 118-124(2020). https://doi.org/10.1016/j.jmbbm.2019.04.040
  24. Kumar, K. V. A., Lakshminarayana, B., Suryakala, D., Subrahmanyam, C., "Reduced Graphene Oxide Supported ZnO Quantum Dots for Visible Light-induced Simultaneous Removal of Tetracycline and Hexavalent Chromium," RSC Advances, 10, 20494-20503(2020). https://doi.org/10.1039/D0RA02062A
  25. Wu, F., Zhou, F., Zhu, Z., Zhan, S. and He, Q., "Enhanced Photocatalytic Activities of Ag3PO4/GO in Tetracycline Degradation," Chemical Physics Letters, 724, 90-95(2020).
  26. Abdel-Mottaleb, M. M., Khalil, A., Karim, S., Osman, T. A. and Khattab, A., "High Performance of PAN/GO-ZnO Composite Nanofibers for Photocatalytic Degradation Under Visible Irradiation," J. of the Mechanical Behavior of Biomedical Materials, 96, 118-124(2019). https://doi.org/10.1016/j.jmbbm.2019.04.040
  27. Qiao, D., Li, Z., Duan, J. and He, X., "Adsorption and Photocatalytic Degradation Mechanism of Magnetic Graphene Oxide/ZnO Nanocomposites for Tetracycline Contaminants," Chemical Engineering J., 400, 125952(2020).
  28. Jia, K., Liu, G., Lang, D.-N., Chen, S.-F., Yang, C., Wu, R.-L., Wang, W. and Wang, J.-D., "Degradation of Tetracycline by Visible Light Over ZnO Nanophotocatalyst," J. of the Taiwan Institute of Chemical Engineers, 136, 104422(2022).
  29. Gang, R., Xu, L., Xia, Y., Zhang, L., Wang, S., Li, R., "Facile One-step Production of 2D/2D ZnO/rGO Nanocomposites under Microwave Irradiation for Photocatalytic Removal of Tetracycline," ACS Omega, 6, 3831-3839(2021). https://doi.org/10.1021/acsomega.0c05559
  30. Kar, S., Chakraborty, K., Pal, T. and Ghosh, S., "Enhanced Photocatalytic Degradation of Tetracycline by RGO-ZnO Composite, AIP Conference Proceedings, 2265, 030134(2020).