Construction of Ternary Heterojunction g-C3N4 /BiVO4 /GQDs Nanocomposite and Its Methylene Blue Photodegradation Performance

Heroldinho Arieveali, Tien Setyaningtyas, Kapti Riyani, Anung Riapanitra

Abstract

Ternary heterojunction g-C3N4/BiVO4/GQDs (CBG) composite photocatalysts were successfully made by high-temperature solidstate method. The prepared CBG photocatalyst was used to degrade the methylene blue (MB) solution under the simulation of visible light irradiation. The analysis of photocatalytic activity was carried out in the parameters of mass variation of composite components, pH of MB solution, and kinetic rate measurement. The results showed that the adsorption-photocatalysis synergy effect occurred at its best in CBG-20 samples with pH 9 in MB solution with a degradation kinetic rate following the pseudo-first order within 150 min of removal time as the optimum condition that could degrade MB by 94.81%. The result showed that the photocatalytic activity of the
ternary composite was higher than that of pristine g-C3N4, BiVO4, or the binary composite of g-C3N4/BiVO4. Trapping experiments results support the direct dual Z-scheme which shows that ·O2- is the most significant radical for the photocatalytic degradation of MB. The prepared ternary composites show outstanding application prospects in wastewater treatment.

References

Akbari, A., Z. Sabouri, H. A. Hosseini, A. Hashemzadeh, M. Khatami, and M. Darroudi (2020). Effect of Nickel Oxide Nanoparticles as a Photocatalyst in Dyes Degradation and Evaluation of Effective Parameters in Their Removal from Aqueous Environments. Inorganic Chemistry Communications, 115; 107867.

Bahrudin, N. N. (2022). Evaluation of Degradation Kinetic and Photostability of Immobilized TiO₂/Activated Carbon Bilayer Photocatalyst for Phenol Removal. Applied Surface Science Advances, 7; 100208.

Bankole, O. M., T. D. Olorunsola, and A. S. Ogunlaja (2021). Photocatalytic Decontamination of Toxic Hexavalent Chromium in Water Over Graphitic Carbon Nitride Supported Sulfur Nanoparticles. Journal of Photochemistry and Photobiology A: Chemistry, 405; 112934.

Chaudhuri, A., L. Mandal, X. Chi, M. Yang, M. C. Scott, M. Motapothula, X. J. Yu, P. Yang, Y. Shao-Horn, T. Venkatesan, A. T. S. Wee, and A. Rusydi (2018). Direct Observation of Anisotropic Small-hole Polarons in an Orthorhombic Structure of BiVO₄ Films. Physical Review B, 97(19); 195150.

Cheng, C., Q. Liang, M. Yan, Z. Liu, Q. He, T. Wu, S. Luo, Y. Pan, C. Zhao, and Y. Liu (2022). Advances in Preparation, Mechanism and Applications of Graphene Quantum Dots/Semiconductor Composite Photocatalysts: A Review. Journal of Hazardous Materials, 424; 127721.

Dihom, H. R., M. M. Al-Shaibani, R. M. S. Radin Mohamed, A. A. Al-Gheethi, A. Sharma, and M. H. B. Khamidun (2022). Photocatalytic Degradation of Disperse Azo Dyes in Textile Wastewater Using Green Zinc Oxide Nanoparticles Synthesized in Plant Extract: A Critical Review. Journal of Water Process Engineering, 47; 102705.

El-Yazeed, W. S. A., S. A. El-Hakam, A. A. Salah, and A. A. Ibrahim (2021). Fabrication and Characterization of Reduced Graphene-BiVO₄ Nanocomposites for Enhancing Visible Light Photocatalytic and Antibacterial Activity. Journal of Photochemistry and Photobiology A: Chemistry, 417; 113362.

Elmorsy, E. S., W. A. Amer, A. Mahrous, and M. M. Ayad (2023). Insight into the Novel ZIF-8@N-CQDs/ZIF-67 Nanocomposite for Photocatalytic Degradation of Methylene Blue under Visible Light Irradiation. Materials Science and Engineering: B, 298; 116900.

Fakhrul, M., R. Samsudin, A. Dumas, R. Bashiri, N. M. Mohamed, and S. Sufian (2020). Development of the g-C₃N₄/BiVO₄ Microflower Photocatalyst for Photocatalytic Degradation of Amoxicillin and Hydrogen Production. Malaysian Journal of Microscopy, 16(1); 180–187.

Feng, S., T. Chen, Z. Liu, J. Shi, X. Yue, and Y. Li (2020). Z-Scheme CdS/CQDs/g-C₃N₄ Composites with Visible-Near-Infrared Light Response for Efficient Photocatalytic Organic Pollutant Degradation. Science of The Total Environment, 704; 135404.

Hatefi, R., A. Mashinchian-Moradi, H. Younesi, and S. Nojavan (2020). Graphene Quantum Dots Based on Maltose as a High Yield Photocatalyst for Efficient Photodegradation of Imipramine in Wastewater Samples. Journal of Environmental Health Science and Engineering, 18; 1531–1540.

Ibarbia, A., H. J. Grande, and V. Ruiz (2020). On the Factors Behind the Photocatalytic Activity of Graphene Quantum Dots for Organic Dye Degradation. Particle and Particle Systems Characterization, 37(5); 2000061.

Jabbar, Z. H., A. A. Okab, B. H. Graimed, M. A. Issa, and S. H. Ammar (2023). Photocatalytic Destruction of Congo Red Dye in Wastewater Using a Novel Ag₂WO₄/Bi₂S₃ Nanocomposite Decorated g-C₃N₄ Nanosheet as Ternary S-Scheme Heterojunction: Improving the Charge Transfer Efficiency. Diamond and Related Materials, 133; 109711.

Jin, C., W. Li, Y. Chen, R. Li, J. Huo, Q. He, and Y. Wang (2020). Efficient Photocatalytic Degradation and Adsorption of Tetracycline Over Type-II Heterojunctions Consisting of ZnO Nanorods and K-Doped Exfoliated g-C₃N₄ Nanosheets. Industrial and Engineering Chemistry Research, 59(7); 2860–2873.

Kalaycıoğlu, Z., B. Özuğur Uysal, O. Pekcan, and F. B. Erim (2023). Efficient Photocatalytic Degradation of Methylene Blue Dye from Aqueous Solution with Cerium Oxide Nanoparticles and Graphene Oxide-Doped Polyacrylamide. ACS Omega, 8(14); 13004–13015.

Kamble, G. S., T. S. Natarajan, S. S. Patil, M. Thomas, R. K. Chougale, P. D. Sanadi, U. S. Siddharth, and Y. C. Ling (2023). BiVO4 as a Sustainable and Emerging Photocatalyst: Synthesis Methodologies, Engineering Properties, and Its Volatile Organic Compounds Degradation Efficiency. Nanomaterials, 13(9); 1528.

Kumar, R., A. Sudhaik, A. A. P. Khan, P. Raizada, A. M. Asiri, S. Mohapatra, S. Thakur, V. K. Thakur, and P. Singh (2022). Current Status on Designing of Dual Z-Scheme Photocatalysts for Energy and Environmental Applications. Journal of Industrial and Engineering Chemistry, 106; 340–355.

Kumar, S., A. Dhiman, P. Sudhagar, and V. Krishnan (2018). ZnO-Graphene Quantum Dots Heterojunctions for Natural Sunlight-Driven Photocatalytic Environmental Remediation. Applied Surface Science, 447; 802–815.

Li, P., Y. Hu, D. Lu, J. Wu, and Y. Lv (2023). Study on g C3N4/BiVO4 Binary Composite Photocatalytic Materials. Micromachines, 14(3); 639.

Li, Y., B. Yang, and B. Liu (2021). Synthesis of BiVO4 Nanoparticles with Tunable Oxygen Vacancy Level: The Phenomena and Mechanism for Their Enhanced Photocatalytic Performance. Ceramics International, 47(7); 9849–9855.

Liaqat, M., R. M. Munir, I. Maryam, T. Iqbal, S. Afsheen, A. G. Nabi, R. R. M. Khan, A. El-marghany, I. Warad, and A. Basit (2024). Synthesis and Characterization of WO3/BiVO4/Graphene Ternary Nanocomposites for the Photodegradation of Methylene Blue and Tetracycline. Materials Chemistry and Physics, 320; 129465.

Liu, Y., X. Zhang, X. Li, and Z. Zhou (2024). Visible Light Driven S-Scheme GQDs/BiOBr Heterojunction with Enhanced Photocatalytic Degradation of Rhodamine B and Mechanism Insight. Journal of Water Process Engineering, 57; 104588.

Liu, Z., F. Li, Y. Luo, M. Li, G. Hu, X. Pu, T. Tang, J. Wen, X. Li, and W. Li (2021). Size Effect of Graphene Quantum Dots on Photoluminescence. Molecules, 26(13); 3922.

Ma, C., J. Lee, Y. Kim, W. C. Seo, H. Jung, and W. Yang (2021). Rational Design of α Fe2O3 Nanocubes Supported BiVO4 Z-Scheme Photocatalyst for Photocatalytic Degradation of Antibiotic Under Visible Light. Journal of Colloid and Interface Science, 581; 514–522.

Mansha, M. S., T. Iqbal, M. Farooq, K. N. Riaz, S. Afsheen, M. S. Sultan, N. Al-Zaqri, I. Warad, and A. Masood (2023). Facile Hydrothermal Synthesis of BiVO4 Nanomaterials for Degradation of Industrial Waste. Heliyon, 9(5); e15978.

Nadimi, M., A. Ziarati Saravani, M. A. Aroon, and A. Ebrahimian Pirbazari (2019). Photodegradation of Methylene Blue by a Ternary Magnetic TiO2/Fe3O4/Graphene Oxide Nanocomposite Under Visible Light. Materials Chemistry and Physics, 225; 464–474.

Nagar, A. and S. Basu (2021). Ternary g C3N4/Ag/BiVO4 Nanocomposite: Fabrication and Implementation to Remove Organic Pollutants. Environmental Technology and Innovation, 23; 101646.

Ramírez, A. E., M. Montero-Muñoz, L. L. López, J. E. Ramos-Ibarra, J. A. H. Coaquira, B. Heinrichs, and C. A. Páez (2021). Significantly Enhancement of Sunlight Photocatalytic Performance of ZnO by Doping with Transition Metal Oxides. Scientific Reports, 11(1); 2804.

Ranjith, R., N. Karmegam, M. Alsawalha, X. Hu, and K. Jothimani (2023). Construction of g C3N4/CdS/BiVO4 Ternary Nanocomposite with Enhanced Visible-Light-Driven Photocatalytic Activity Toward Methylene Blue Dye Degradation in the Aqueous Phase. Journal of Environmental Management, 330; 117132.

Remlalfaka, W., C. Murugesan, P. N. Anantharamaiah, and N. M. Prabu (2021). Fabrication of Magnetically Recoverable BiVO4/NiFe2O4 Composites for the Photocatalytic Degradation of Methylene Blue. Ceramics International, 47(8); 11526–11535.

Riapanitra, A., T. Setyaningtyas, and G. H. Haryadinaru (2024). Photodegradation of Methylene Blue Dye Using BiVO4/g C3N4 Composites Under Visible Light Irradiation. Jurnal Kimia Sains Dan Aplikasi, 27(8); 363–370.

Riapanitra, A., T. Setyaningtyas, K. Riyani, R. Andreas, A. L. Ariyanti, and U. Sulaeman (2022). Synthesis of Vanadium Oxide Material and Its Photocatalytic Activity in the Degradation of Methylene Blue. In AIP Conference Proceedings, volume 2553.

Rini, N. P., N. I. Istiqomah, Sunarta, and E. Suharyadi (2023). Enhancing Photodegradation of Methylene Blue and Reusability Using CoO/ZnO Composite Nanoparticles. Case Studies in Chemical and Environmental Engineering, 7; 100301.

Sarwar, A., A. Razzaq, M. Zafar, I. Idrees, F. Rehman, and W. Y. Kim (2023). Copper Tungstate (CuWO4)/Graphene Quantum Dots (GQDs) Composite Photocatalyst for Enhanced Degradation of Phenol Under Visible Light Irradiation. Results in Physics, 45; 106253.

Sen, T. K. (2023). Adsorptive Removal of Dye (Methylene Blue) Organic Pollutant from Water by Pine Tree Leaf Biomass Adsorbent. Processes, 11(7); 1877.

Sharifi, T., D. Crmaric, M. Kovacic, M. Popovic, M. K. Rokovic, H. Kusic, D. Jozić, G. Ambrožić, D. Kralj, J. Kontrec, B. Zener, U. L. Stangar, D. D. Dionysiou, and A. L. Bozic (2021). Tailored BiVO4 for Enhanced Visible-Light Photocatalytic Performance. Journal of Environmental Chemical Engineering, 9(5); 106025.

Shubha, J. P., H. S. Savitha, S. F. Adil, M. Khan, M. R. Hatshan, K. Kavalli, and B. Shaik (2021). Straightforward Synthesis of Mn3O4/ZnO/Eu2O3-Based Ternary Heterostructure Nano-Photocatalyst and Its Application for the Photodegradation of Methyl Orange and Methylene Blue Dyes. Molecules, 26(15); 4661.

Su, F., P. Li, J. Huang, M. Gu, Z. Liu, and Y. Xu (2021). Photocatalytic Degradation of Organic Dye and Tetracycline by Ternary Ag2O/AgBr-CeO2 Photocatalyst Under Visible-Light Irradiation. Scientific Reports, 11(1); 85.

Tahir, M., S. Tasleem, and B. Tahir (2020). Recent Development in Band Engineering of Binary Semiconductor Materials for Solar Driven Photocatalytic Hydrogen Production. International Journal of Hydrogen Energy, 45(32); 15985–16038.

Thi, V. H. T., T. H. Cao, T. N. Pham, T. T. Pham, and M. C. Le (2019). Synergistic Adsorption and Photocatalytic Activity Under Visible Irradiation Using Ag-ZnO/GO Nanoparticles Derived at Low Temperature. Journal of Chemistry, 2019; 2979517.

Waheed, Z., S. Ghazanfar, M. Usman, H. M. Asif, M. Tariq, K. Mahmood, A. Haider, and M. Sirajuddin (2023). Synthesis and Characterization of Ternary Composite g C3N4-WO3/rGO for Photocatalytic Activity in Degradation of Methylene Blue. Bulletin of the Chemical Society of Ethiopia, 37(5); 1123–1131.

Wang, S., L. Zhao, L. Gao, D. Yang, S. Wen, W. Huang, Z. Sun, J. Guo, X. Jiang, and C. Lu (2022). Fabrication of Ternary Dual Z-Scheme AgI/ZnIn2S4/BiVO4 Heterojunction Photocatalyst with Enhanced Photocatalytic Degradation of Tetracycline Under Visible Light. Arabian Journal of Chemistry, 15(10); 104159.

Wu, Y., X. Zhao, S. Huang, Y. Li, X. Zhang, G. Zeng, L. Niu, Y. Ling, and Y. Zhang (2021). Facile Construction of 2D g C3N4 Supported Nanoflower-like NaBiO3 with Direct Z-Scheme Heterojunctions and Insight into Its Photocatalytic Degradation of Tetracycline. Journal of Hazardous Materials, 414; 125547.

Yu, F., F. Gong, Q. Yang, and Y. Wang (2022). Fabrication of a Magnetic Retrievable Dual Z-Scheme g C3N4/BiVO4/CoFe2O4 Composite Photocatalyst with Significantly Enhanced Activity for the Degradation of Rhodamine B and Hydrogen Evolution Under Visible Light. Diamond and Related Materials, 125; 109004.

Zhao, G., J. Ding, F. Zhou, X. Chen, L. Wei, Q. Gao, K. Wang, and Q. Zhao (2021). Construction of a Visible-Light-Driven Magnetic Dual Z-Scheme BiVO4/g C3N4/NiFe2O4 Photocatalyst for Effective Removal of Ofloxacin: Mechanisms and Degradation Pathway. Chemical Engineering Journal, 405; 126704.

Zhao, Z., J. Wang, C. Xu, Z. Du, R. Yu, Y. Zhao, J. Han, J. Zuo, Z. Guo, C. Tang, and Y. Fang (2024). Construction of a Novel Ternary GQDs/g C3N4/ZIF-67 Photocatalyst for Enhanced Photocatalytic Carbon Dioxide Reduction. Catalysts, 14(6); 334.

Zhong, X., Y. Li, H. Wu, and R. Xie (2023). Recent Progress in BiVO4-Based Heterojunction Nanomaterials for Photocatalytic Applications. Materials Science and Engineering: B, 289.

Zulkarnain, Y. M. Hakim, E. Melwita, and R. Mohadi (2024). The Effects of Hydrothermal Temperatures on ZnO-Bentonite Composite Synthesis on Adsorption and Photodegradation of Methylene Blue Dye. Science and Technology Indonesia, 9(4); 1033–1041.

Authors

Heroldinho Arieveali
Tien Setyaningtyas
Kapti Riyani
Anung Riapanitra
anung.riapanitra@unsoed.ac.id (Primary Contact)
Arieveali, H. ., Setyaningtyas, T., Riyani, K., & Riapanitra, A. (2025). Construction of Ternary Heterojunction g-C3N4 /BiVO4 /GQDs Nanocomposite and Its Methylene Blue Photodegradation Performance. Science and Technology Indonesia, 10(3), 777–788. https://doi.org/10.26554/sti.2025.10.3.777-788

Article Details