Development of Heterojunction C-TiO2/g-C3N4 as New Photocatalysts for Degradation of Antibiotics Pollutant in Aquesous Environment
Main Article Content
Abstract
C-TiO2 was effectively hybridized with g-C3N4 in the varies mass ratio of C-TiO2/g-C3N4 (10, 20, 30 và 40%) to highly improve its photocatalytic activity for degradation of tetracycline (TC). The prepared samples were characterized by X-ray diffraction (XRD), Ultraviolet–visible absorption spectroscopy (UV-Vis DRS), Photoluminescence (PL) and Energy dispersive X-ray spectroscopy (EDX). As compared with C-TiO2 and g-C3N4, the decoration of C-TiO2 on g-C3N4 led to formation of C-TiO2/g-C3N4 heterojunction to effectively prevent the charge recombination in each material and exhibit great increases in visible light adsorption. The obtained PL and UV-Vis DRS indecated C-TiO2/g-C3N4 material, which the C-TiO2:g-C3N4 mass ratio was 20% showed the strongest tetracycline degradation efficiency (84.24%). With the further increasing in C-TiO2 content in C-TiO2/g-C3N4, photocatalytic degradation efficiency decreased. This was because the excessed C-TiO2 hindered optical absorption for electron-hole separation of g-C3N4 and the excessed C-TiO2 decorating on the surface g-C3N4 could also act as centers for electron-hole recombination leading to decrease photocatalytic degradation efficiency of the C-TiO2/g-C3N4.
Keywords:
C-TiO2, g-C3N4, recombination, photocatalytic activity, visible light, tetracycline.
References
[1] E. S. Elmolla, M. Chaudhuri, The Feasibility of using Combined TiO2 Photocatalysis-SBR Process for Antibiotic Wastewater Treatment, Desalination, Vol. 272, 2011, pp. 218-224.
[2] D. Dimitrakopoulou, I. Rethemiotaki, Z. Frontistis, N. Xekoukoulotakis, D. Venieri, D. Mantzavino, Degradation, Mineralization and Antibiotic Inactivation of Amoxygencillin by UV-A/TiO2 Photocatalysis, J. Environ, Manag., Vol. 98, 2012, pp. 168-174.
[3] Shuaishuai Ma, Jiandong Gu, Yingxia Han, Yuan Gao, Yuqing Zong, Zhaolian Ye, and Jinjuan Xue, Facile Fabrication of C−TiO2 Nanocomposites with Enhanced Photocatalytic Activity for Degradation of Tetracycline, ACS Omega, Vol. 4, No. 25, 2019, pp. 21063-21071.
[4] Y. Y. Gurkan, N. Turkten, A. Hatipoglu, Z. Cinar, Photocatalytic degradation of cefazolin over N-doped TiO2 under UV and sunlight irradiation: Prediction of the reaction paths via conceptual DFT, Chem. Eng. J., Vol. 184, 2012, pp. 113–124.
[5] Q. Gao, F. Si, S. Zhang, Y. Fang, X. Chen, and S. Yang, Hydrogenated F–doped TiO2 for photocatalytic hydrogen evolution and pollutant degradation, Int. J. Hydrogen Energ., Vol. 44, No. 16, 2019, pp. 8011-8019.
[6] M. Wang, J. Han, Y. Hu, and R. Guo, Mesoporous C, N-codoped TiO2 hybrid shells with enhanced visible light photocatalytic performance, RSC. Adv., 2017, vol. 7, pp. 15513-15520.
[7] Zhao Lu, Lei Zeng, Wulin Song, Ziyu Qin, Dawen Zeng, Changsheng Xie, In situ synthesis of C-TiO2/g-C3N4 heterojunction nanocomposite as highly visible light active photocatalyst originated from effective interfacial charge transfer, Applied Catalysis B: Environmental, Vol. 202, 2017, pp. 489–499.
[8] Mai Hung Thanh Tung, Nguyen Thi Dieu Cam, Doan Van Thuan, Pham Van Quan, Cao Van Hoang, Tran Thi Thu Phuong, Nguyen Tan Lam, Truong Thanh Tam, Nguyen Thi Phuong Le Chi, Nguyen Thi Lan, Dang Nguyen Thoại, Thanh-Dong Pham, Novel direct Z-scheme AgI/N–TiO2 photocatalyst for removal of polluted tetracycline under visible irradiation, Ceramics International, Vol. 46, No. 5, 2020, pp. 6012-6021.
[9] Q. Wang, P. Li, Z. Zhang, C. Jiang, K. Zuojiao, J. Liu, Y. Wang, Kinetics and mechanism insights into the photodegradation of tetracycline hydrochloride and ofloxacin mixed antibiotics with the flower-like BiOCl/TiO2 heterojunction, Journal of Photochemistry and Photobiology A: Chemistry, Vol. 378, 2019, pp. 114-124.
[10] S. Yuan, Q. Zhang, B. Xu, S. Liu, J. Wang, J. Xie, M. Zhang, T. Ohno, A new precursor to synthesize g-C3N4 with superior visible light absorption for photocatalytic application, Catal. Sci. Technol., Vol. 7, No. 9, 2017, 1826–1830.
[11] S. Yan, Z. Li and Z. Zou, Photodegradation performance of g-C3N4 fabricated by directly heating melaminee, Langmuir, Vol. 25, 2009, pp. 10397-10401.
[12] Y. Wang, X. Wang, and M. Antonietti, Polymeric Graphitic Carbon Nitride as a Heterogeneous Organocatalyst: From Photochemistry to Multipurpose Catalysis to Sustainable Chemistry, Angewandte Chemie International Edition, Vol. 51, 2012, pp. 68 – 89.
[13] Cheng-Qun Xu, Wei-De Zhang, Facile synthesis of nitrogen deficient g-C3N4 by copolymerization of urea and formamide for efficient photocatalytic hydrogen evolution, Cheng-Qun Xu, Molecular Catalysis, Vol. 453, 2018, pp. 85- 92.
[14] Sun, S., Li, J., Cui, J., Gou, X., Yang, Q., Liang, S., Zhang, J, Constructing oxygen-doped g-C3N4 nanosheets with an enlarged conductive band edge for enhanced visible-light-driven hydrogen evolution. Inorganic Chemistry Frontiers, Vol.5, No. 7, 2018, pp. 1721–1727.
[15] L. Kong, X. Zhang, C. Wang, J. Xu, X. Du, L. Li, Ti3+ defect mediated g-C3N4/TiO2 Z-scheme system for enhanced photocatalytic redox performance, Applied Surface Science, Vol. 448, 2018, pp. 288-296.
[16] T. Xiao, Z. Tang, Y. Yang, L. Tang, Y. Zhou, Z. Zou, In situ construction of hierarchical WO3/g-C3N4 composite hollow microspheres as a Z-Scheme photocatalyst for the degradation of antibiotics, Applied Catalysis B: Environmental, Vol. 220, 2018, pp. 417-428.
[17] H. Katsumata, T. Sakai, T. Suzuki and S. Kaneco, Highly efficient photocatalytic activity of g-C3N4/Ag3PO4 hybrid photocatalysts through Z-scheme photocatalytic mechanism under visible light, Industrial & Engineering Chemistry Research, Vol. 53, No. 19, 2014, pp. 8018 – 8025.
[18] Kumar, S., Surendar, T., Kumar, B., Baruah, A., & Shanker, V., Synthesis of highly efficient and recyclable visible-light responsive mesoporous g-C3N4 photocatalyst via facile template-free sonochemical route, RSC Advances, Vol. 4, No. 16, 2014, pp. 8132 -8138.
[19] Lai, C. W., & Sreekantan, S., Single Step Formation of C-TiO2Nanotubes: Influence of Applied Voltage and Their Photocatalytic Activity under Solar Illumination, International Journal of Photoenergy, Vol. 2013, 2013, pp. 1–8.
[2] D. Dimitrakopoulou, I. Rethemiotaki, Z. Frontistis, N. Xekoukoulotakis, D. Venieri, D. Mantzavino, Degradation, Mineralization and Antibiotic Inactivation of Amoxygencillin by UV-A/TiO2 Photocatalysis, J. Environ, Manag., Vol. 98, 2012, pp. 168-174.
[3] Shuaishuai Ma, Jiandong Gu, Yingxia Han, Yuan Gao, Yuqing Zong, Zhaolian Ye, and Jinjuan Xue, Facile Fabrication of C−TiO2 Nanocomposites with Enhanced Photocatalytic Activity for Degradation of Tetracycline, ACS Omega, Vol. 4, No. 25, 2019, pp. 21063-21071.
[4] Y. Y. Gurkan, N. Turkten, A. Hatipoglu, Z. Cinar, Photocatalytic degradation of cefazolin over N-doped TiO2 under UV and sunlight irradiation: Prediction of the reaction paths via conceptual DFT, Chem. Eng. J., Vol. 184, 2012, pp. 113–124.
[5] Q. Gao, F. Si, S. Zhang, Y. Fang, X. Chen, and S. Yang, Hydrogenated F–doped TiO2 for photocatalytic hydrogen evolution and pollutant degradation, Int. J. Hydrogen Energ., Vol. 44, No. 16, 2019, pp. 8011-8019.
[6] M. Wang, J. Han, Y. Hu, and R. Guo, Mesoporous C, N-codoped TiO2 hybrid shells with enhanced visible light photocatalytic performance, RSC. Adv., 2017, vol. 7, pp. 15513-15520.
[7] Zhao Lu, Lei Zeng, Wulin Song, Ziyu Qin, Dawen Zeng, Changsheng Xie, In situ synthesis of C-TiO2/g-C3N4 heterojunction nanocomposite as highly visible light active photocatalyst originated from effective interfacial charge transfer, Applied Catalysis B: Environmental, Vol. 202, 2017, pp. 489–499.
[8] Mai Hung Thanh Tung, Nguyen Thi Dieu Cam, Doan Van Thuan, Pham Van Quan, Cao Van Hoang, Tran Thi Thu Phuong, Nguyen Tan Lam, Truong Thanh Tam, Nguyen Thi Phuong Le Chi, Nguyen Thi Lan, Dang Nguyen Thoại, Thanh-Dong Pham, Novel direct Z-scheme AgI/N–TiO2 photocatalyst for removal of polluted tetracycline under visible irradiation, Ceramics International, Vol. 46, No. 5, 2020, pp. 6012-6021.
[9] Q. Wang, P. Li, Z. Zhang, C. Jiang, K. Zuojiao, J. Liu, Y. Wang, Kinetics and mechanism insights into the photodegradation of tetracycline hydrochloride and ofloxacin mixed antibiotics with the flower-like BiOCl/TiO2 heterojunction, Journal of Photochemistry and Photobiology A: Chemistry, Vol. 378, 2019, pp. 114-124.
[10] S. Yuan, Q. Zhang, B. Xu, S. Liu, J. Wang, J. Xie, M. Zhang, T. Ohno, A new precursor to synthesize g-C3N4 with superior visible light absorption for photocatalytic application, Catal. Sci. Technol., Vol. 7, No. 9, 2017, 1826–1830.
[11] S. Yan, Z. Li and Z. Zou, Photodegradation performance of g-C3N4 fabricated by directly heating melaminee, Langmuir, Vol. 25, 2009, pp. 10397-10401.
[12] Y. Wang, X. Wang, and M. Antonietti, Polymeric Graphitic Carbon Nitride as a Heterogeneous Organocatalyst: From Photochemistry to Multipurpose Catalysis to Sustainable Chemistry, Angewandte Chemie International Edition, Vol. 51, 2012, pp. 68 – 89.
[13] Cheng-Qun Xu, Wei-De Zhang, Facile synthesis of nitrogen deficient g-C3N4 by copolymerization of urea and formamide for efficient photocatalytic hydrogen evolution, Cheng-Qun Xu, Molecular Catalysis, Vol. 453, 2018, pp. 85- 92.
[14] Sun, S., Li, J., Cui, J., Gou, X., Yang, Q., Liang, S., Zhang, J, Constructing oxygen-doped g-C3N4 nanosheets with an enlarged conductive band edge for enhanced visible-light-driven hydrogen evolution. Inorganic Chemistry Frontiers, Vol.5, No. 7, 2018, pp. 1721–1727.
[15] L. Kong, X. Zhang, C. Wang, J. Xu, X. Du, L. Li, Ti3+ defect mediated g-C3N4/TiO2 Z-scheme system for enhanced photocatalytic redox performance, Applied Surface Science, Vol. 448, 2018, pp. 288-296.
[16] T. Xiao, Z. Tang, Y. Yang, L. Tang, Y. Zhou, Z. Zou, In situ construction of hierarchical WO3/g-C3N4 composite hollow microspheres as a Z-Scheme photocatalyst for the degradation of antibiotics, Applied Catalysis B: Environmental, Vol. 220, 2018, pp. 417-428.
[17] H. Katsumata, T. Sakai, T. Suzuki and S. Kaneco, Highly efficient photocatalytic activity of g-C3N4/Ag3PO4 hybrid photocatalysts through Z-scheme photocatalytic mechanism under visible light, Industrial & Engineering Chemistry Research, Vol. 53, No. 19, 2014, pp. 8018 – 8025.
[18] Kumar, S., Surendar, T., Kumar, B., Baruah, A., & Shanker, V., Synthesis of highly efficient and recyclable visible-light responsive mesoporous g-C3N4 photocatalyst via facile template-free sonochemical route, RSC Advances, Vol. 4, No. 16, 2014, pp. 8132 -8138.
[19] Lai, C. W., & Sreekantan, S., Single Step Formation of C-TiO2Nanotubes: Influence of Applied Voltage and Their Photocatalytic Activity under Solar Illumination, International Journal of Photoenergy, Vol. 2013, 2013, pp. 1–8.