Synthesis of Zn/Al-ZnO Composite Using Zn/Al-Layered Double Hydroxide for Oxidative Desulfurization of 4-Methyldibenzothiophene
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Keywords:
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Desulfurization, 4-Methyldibenzothiophene, Zn/Al-Layered Double Hydroxide, ZnAl-ZnO
Abstract
Zn/Al-ZnO composites made from Zn/Al-Layered Double Hydroxide base material and ZnO as a precursor were successfully made in this study. Characterization analysis using SEM-EDS, XRD, and FTIR. The SEM analysis results show the Zn/Al-LDH has a smooth surface, overlapping, and is prone to aggregation, resulting in non-uniform particle size. However, it forms a uniform grain shape. Zn/Al-ZnO have rough surfaces with uniform particle shape and size, and the presence of pores on the particle surface. EDS analysis shows the Zn element which is more abundant in Zn/Al-ZnO. XRD analysis of Zn/Al-LDH showed the hydrotalcite. XRD analysis on ZnO showed the hexagonal wurtzite crystal structure. Zn/Al-ZnO composites at an angle of 2θ show the same peak of the base material and the precursor. FTIR analysis of the composite revealed the presence of O-H groups at wave numbers 3445 cm−1, 1633 cm−1, and 1504 cm−1, indicating the presence of nitrate. Additionally, vibrations at wave numbers 1382 cm−1 corresponded to antisymmetric (v3) stretching of nitrate, while wave numbers 418 cm−1 and 606 cm−1 indicated metal-oxygen stretching vibrations. Of all the factors used in the desulfurization of 4-methyldibenzothiophene, Zn/Al-ZnO composites had the highest %conversion rate of both the base material and the precursor. The %conversion values of Zn/Al-ZnO at the time of contact were 99.40%, catalyst dosage 99.38%, solvent 99.10%, and temperature 99.56%, respectively. The catalyst is heterogeneous and reusable for the desulfurization of 4-methyldibenzothiophene.
References
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Lesbani, A., N. R. Palapa, R. J. Sayeri, T. Taher, and N. Hidayati (2021). High Reusability of NiAl LDH/Biochar Composite in the Removal Methylene Blue from Aqueous Solution. Indonesian Journal of Chemistry, 21(2); 421–434
Li, A., Y. Zhang, W. Ge, Y. Zhang, L. Liu, and G. Qiu (2022). Removal of Heavy Metals from Wastewaters with Biochar Pyrolyzed from MgAl-Layered Double Hydroxide-Coated Rice Husk: Mechanism and Application. Bioresource Technology, 347; 126425
Lin, Y., L. Feng, X. Li, Y. Chen, G. Yin, and W. Zhou (2020). Study on Ultrasound-Assisted Oxidative Desulfurization for Crude Oil. Ultrasonics Sonochemistry, 63; 104946
Liu, S., Z. Liu, H. Zhu, Z. Wang, J. Guo, X. Zhang, H. Yu, X. Yue, P. Ning, and B. Li (2023). The Roles of Red Mud as Desulfurization and Denitrification in Flue Gas: A Review. Journal of Environmental Chemical Engineering; 109770
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Mahboob, I., I. Shafiq, S. Shafique, P. Akhter, M. Hussain, and Y.-K. Park (2022). Effect of Active Species Scavengers in Photocatalytic Desulfurization of Hydrocracker Diesel Using Mesoporous Ag3VO4. Chemical Engineering Journal, 441; 136063
Mahjoubi, F. Z., A. Khalidi, M. Abdennouri, and N. Barka (2017). Zn–Al Layered Double Hydroxides Intercalated with Carbonate, Nitrate, Chloride and Sulphate Ions: Synthesis,
Characterisation and Dye Removal Properties. Journal of Taibah University for Science, 11(1); 90-100
Malani, R. S., A. H. Batghare, J. B. Bhasarkar, and V. S. Moholkar (2021). Kinetic Modelling and Process Engineering Aspects of Biodesulfurization of Liquid Fuels: Review and Analysis. Bioresource Technology Reports, 14; 100668
Mallakpour, S., E. Azadi, and M. Dinari (2023). Removal of Cationic and Anionic Dyes Using Ca Alginate and Zn-Al Layered Double Hydroxide/Metal-Organic Framework. Carbohydrate Polymers, 301; 120362
Miceli, M., P. Frontera, A. Macario, and A. Malara (2021). Recovery/Reuse of Heterogeneous Supported Spent Catalysts. Catalysts, 11(5); 591
Palapa, N. R., T. Taher, A. Wijaya, and A. Lesbani (2021). Modification of Cu/Cr Layered Double Hydroxide by Keggin Type Polyoxometalate as Adsorbent of Malachite Green from Aqueous Solution. Science and Technology Indonesia, 6(3); 209–217
Parhi, P. and P. Misra (2023). Hydrometallurgical Investigation Routed through Microwave (MW) Assisted Leaching and Solvent Extraction Using Ionic Liquids for Extraction and Recovery of Molybdenum from Spent Desulphurization Catalyst. Inorganic Chemistry Communications, 149; 110394
Pei, T., Y. Chen, H. Wang, and L. Xia (2023). Heteropolyacid Ionic Liquid-Based MCF: An Efficient Heterogeneous Catalyst for Oxidative Desulfurization of Fuel. Materials, 16(8); 3195
Polikarpova, P., A. Akopyan, A. Shlenova, and A. Anisimov (2020). New Mesoporous Catalysts with Brønsted Acid Sites for Deep Oxidative Desulfurization of Model Fuels. Catalysis Communications, 146; 106123
Priatna, S., Y. Hakim, S. Wibyan, S. Sailah, and R. Mohadi (2023). Interlayer Modification of West Java Natural Ben tonite as Hazardous Dye Rhodamine B Adsorption. Science and Technology Indonesia, 8(2); 160–169
Privat, R., J.-N. Jaubert, F. Garcia, and M. Molière (2010). Ethanol-Hydrocarbon Blend Vapor Prediction. J. Eng. Gas Turbines Power, 132(9); 091504
Rohman, A. (2014). Rice Bran Oil’s Role in Health and Cooking. In Wheat and Rice in Disease Prevention and Health. Elsevier, pages 481–490
Smith, G. L., J. E. Eyley, X. Han, X. Zhang, J. Li, N. M. Jacques, H. G. Godfrey, S. P. Argent, L. J. Mc-Cormick McPherson, and S. J. Teat (2019). Reversible Coordinative Binding and Separation of Sulfur Dioxide in a Robust Metal–Organic Framework with Open Copper Sites. Nature Materials, 18(12); 1358–1365
Tchalala, M., P. Bhatt, K. Chappanda, S. Tavares, K. Adil, Y. Belmabkhout, A. Shkurenko, A. Cadiau, N. Heymans, and G. De Weireld (2019). Fluorinated MOF Platform for Selective Removal and Sensing of SO2 from Flue Gas and Air. Nature Communications, 10(1); 1328
Tripathi, N., R. S. Singh, and C. D. Hills (2019). Microbial Removal of Sulphur from Petroleum Coke (Petcoke). Fuel, 235; 1501–1505
Wibiyan, S., A. Wijaya, and P. M. S. B. N. Siregar (2023). Adsorption of Phenol using Cellulose and Hydrochar: Kinetic, Isotherm, and Regeneration Studies. Indonesian Journal of Material Research, 1(2); 61–67
Wu, Y., P. Duan, and C. Yan (2018). Role of Layered Double Hydroxides in Setting, Hydration Degree, Microstructure and Compressive Strength of Cement Paste. Applied Clay Science, 158; 123–131
Yuliasari, N., A. Wijaya, R. Mohadi, E. Elfita, and A. Lesbani (2022). Photocatalytic Degradation of Malachite Green by Layered Double Hydroxide Based Composites. Bulletin of Chemical Reaction Engineering & Catalysis, 17(2); 240–249
Zhang, H., Z. Jin, M. Xu, Y. Zhang, J. Huang, H. Cheng, X. Wang, Z. Zheng, and Y. Ding (2021). Enhanced Iso-propanol Sensing Performance of the CdS Nanoparticle Decorated ZnO Porous Nanosheets-Based Gas Sensors. IEEE Sensors Journal, 21(12); 13041–13047
Zhang, Y., Z. Chen, X. Liu, Z. Dong, P. Zhang, J. Wang, Q. Deng, Z. Zeng, S. Zhang, and S. Deng (2019). Efficient SO2 Removal Using a Microporous Metal–Organic Framework with Molecular Sieving Effect. Industrial & Engineering Chemistry Research, 59(2); 874–882
Zhu, H., W. Lin, Q. Li, Y. Hu, S. Guo, C. Wang, and F. Yan (2020). Bipyridinium-Based Ionic Covalent Triazine Frameworks for CO2, SO2, and NO Capture. ACS Applied Materials & Interfaces, 12(7); 8614–8621
Zhuang, X., Z. Zhang, Y. Wang, and Y. Li (2018). The Effect of Alternative Solvents to n-Hexane on the Green Extraction of Litsea cubeba Kernel Oils as New Oil Sources. Industrial Crops and Products, 126; 340–346
Ahmad, M., M. Yousaf, W. Cai, and Z. Zhao (2023a). Formulation of Heterometallic ZIF-8@ Cu/Ni/ZnO@CNTs Heterostructure Photocatalyst for Ultra-Deep Desulphurization of Coal and Fuels. Chemical Engineering Journal, 453;139846
Ahmad, N., M. Badaruddin, N. Yuliasari, F. S. Arsyad, and A. Lesbani (2022a). Highly Efficient Catalytic Oxidative Desulfurization of Dibenzothiophene using Layered Double Hydroxide Modified Polyoxometalate Catalyst. Bulletin of Chemical Reaction Engineering & Catalysis, 17(4); 821–830
Ahmad, N., E. S. Fitri, A. Wijaya, A. Amri, M. Mardiyanto, I. Royani, and A. Lesbani (2022b). Catalytic Oxidative Desulfurization of Dibenzothiophene Utilizing Composite Based Zn/Al Layered Double Hydroxide. Bulletin of Chemical Reaction Engineering & Catalysis, 17(4); 733–742
Ahmad, N., A. Wijaya, E. S. Fitri, F. S. Arsyad, R. Mohadi, and A. Lesbani (2022c). Catalytic Oxidative Desulfurization of Dibenzothiophene by Composites Based Ni/al-Oxide. Science and Technology Indonesia, 7(3); 385–391
Ahmad, N., N. Yuliasari, F. S. Arsyad, I. Royani, R. Mohadi, and A. Lesbani (2023b). Catalytic Oxidative Desulfurization of Dibenzothiophene by Heterogeneous M2+/Al-Layered Double Hydroxide (M2+= Zn, Mg, Ni) Modified Zinc Oxide. Iranian Journal of Catalysis, 13(1); 35–45
Akopyan, A., E. Eseva, P. Polikarpova, A. Kedalo, A. Vutolkina, and A. Glotov (2020). Deep Oxidative Desulfurization of Fuels in the Presence of Brönsted Acidic Polyoxometalate-Based Ionic Liquids. Molecules, 25(3); 536
Anqi, A. E. (2023). Machine Learning Modeling for Optimization of Sulfur Compounds Separation from Fuels: Process Optimization for Reduction of Environmental Pollution. Case Studies in Thermal Engineering, 45; 102989
Azni, M. A., R. Md Khalid, U. A. Hasran, and S. K. Kamarudin (2023). Review of the Effects of Fossil Fuels and the Need for a Hydrogen Fuel Cell Policy in Malaysia. Sustainability, 15(5); 4033
Bartoli, M., C. Zhu, J. Asomaning, M. Chae, and D. C. Bressler (2022). Biosolids-Based Catalyst for Oxidative Desulphurization of Drop-In Fuels Derived from Waste Fats. Fuel, 324; 124546
Chandran, D., M. Khalid, R. Walvekar, N. M. Mubarak, S. Dharaskar, W. Y. Wong, and T. C. S. M. Gupta (2019). Deep Eutectic Solvents for Extraction-Desulphurization: A Review. Journal of Molecular Liquids, 275; 312–322
Chang, H., H. Yi, and J. Zhang (2021). Preparation of a NiOBi2WO6 Catalyst and Its Photocatalytic Oxidative Desulfurization Performance. Colloid and Interface Science Communications, 41; 100381
Chen, C., B. Lu, X. Zhao, W. Qian, J. Liu, T. Trabelsi, J. S. Francisco, J. Qin, J. Li, and L. Wang (2020). Capture of the Sulfur Monoxide–Hydroxyl Radical Complex. Journal of the American Chemical Society, 142(5); 2175–2179
Han, H., L. Zhou, K. Liu, Z. Lu, and N. Luo (2020). A Process Optimization on High Temperature Electrolytic Desulfurization in Hot Metal Pretreatment Using Magnesit-Based Desulfurizer. Metalurgija, 59(3); 295–298
Han, Y., M. Wu, L. Hao, and H. Yi (2018). Sulfur Dioxide Derivatives Alleviate Cadmium Toxicity by Enhancing Antioxidant Defence and Reducing Cd2+ Uptake and Translocation in Foxtail Millet Seedlings. Ecotoxicology and Environmental Safety, 157; 207–215
Houda, S., C. Lancelot, P. Blanchard, L. Poinel, and C. Lamonier (2018). Oxidative Desulfurization of Heavy Oils with High Sulfur Content: A Review. Catalysts, 8(9); 344
Intachai, S., T. Nakato, and N. Khaorapapong (2021). Zno Decorated on Low Carbonate NiAl Layered Double Hydroxide as Efficient Photocatalyst for Methyl Orange Degradation. Applied Clay Science, 201; 105927
Lesbani, A., A. Anggraini, R. Mohadi, D. Rohendi, and M. Said (2017). Desulfurization of 4-Methyl Dibenzothiophene Using Titanium Supported Keggin Type Polyoxometalate. In AIP Conference Proceedings, volume 1823. AIP Publishing, pages 1–9
Lesbani, A., N. R. Palapa, R. J. Sayeri, T. Taher, and N. Hidayati (2021). High Reusability of NiAl LDH/Biochar Composite in the Removal Methylene Blue from Aqueous Solution. Indonesian Journal of Chemistry, 21(2); 421–434
Li, A., Y. Zhang, W. Ge, Y. Zhang, L. Liu, and G. Qiu (2022). Removal of Heavy Metals from Wastewaters with Biochar Pyrolyzed from MgAl-Layered Double Hydroxide-Coated Rice Husk: Mechanism and Application. Bioresource Technology, 347; 126425
Lin, Y., L. Feng, X. Li, Y. Chen, G. Yin, and W. Zhou (2020). Study on Ultrasound-Assisted Oxidative Desulfurization for Crude Oil. Ultrasonics Sonochemistry, 63; 104946
Liu, S., Z. Liu, H. Zhu, Z. Wang, J. Guo, X. Zhang, H. Yu, X. Yue, P. Ning, and B. Li (2023). The Roles of Red Mud as Desulfurization and Denitrification in Flue Gas: A Review. Journal of Environmental Chemical Engineering; 109770
Lozano-Lunar, A., R. Otero, J. I. Álvarez, J. R. Jiménez, and J. M. Fernández-Rodríguez (2023). Application of Layer Double Hydroxide in Cementitious Matrices for the Improvement of the Double Barrier Technique in the Immobilisation of Lead Waste. Applied Clay Science, 238; 106938
Mahboob, I., I. Shafiq, S. Shafique, P. Akhter, M. Hussain, and Y.-K. Park (2022). Effect of Active Species Scavengers in Photocatalytic Desulfurization of Hydrocracker Diesel Using Mesoporous Ag3VO4. Chemical Engineering Journal, 441; 136063
Mahjoubi, F. Z., A. Khalidi, M. Abdennouri, and N. Barka (2017). Zn–Al Layered Double Hydroxides Intercalated with Carbonate, Nitrate, Chloride and Sulphate Ions: Synthesis,
Characterisation and Dye Removal Properties. Journal of Taibah University for Science, 11(1); 90-100
Malani, R. S., A. H. Batghare, J. B. Bhasarkar, and V. S. Moholkar (2021). Kinetic Modelling and Process Engineering Aspects of Biodesulfurization of Liquid Fuels: Review and Analysis. Bioresource Technology Reports, 14; 100668
Mallakpour, S., E. Azadi, and M. Dinari (2023). Removal of Cationic and Anionic Dyes Using Ca Alginate and Zn-Al Layered Double Hydroxide/Metal-Organic Framework. Carbohydrate Polymers, 301; 120362
Miceli, M., P. Frontera, A. Macario, and A. Malara (2021). Recovery/Reuse of Heterogeneous Supported Spent Catalysts. Catalysts, 11(5); 591
Palapa, N. R., T. Taher, A. Wijaya, and A. Lesbani (2021). Modification of Cu/Cr Layered Double Hydroxide by Keggin Type Polyoxometalate as Adsorbent of Malachite Green from Aqueous Solution. Science and Technology Indonesia, 6(3); 209–217
Parhi, P. and P. Misra (2023). Hydrometallurgical Investigation Routed through Microwave (MW) Assisted Leaching and Solvent Extraction Using Ionic Liquids for Extraction and Recovery of Molybdenum from Spent Desulphurization Catalyst. Inorganic Chemistry Communications, 149; 110394
Pei, T., Y. Chen, H. Wang, and L. Xia (2023). Heteropolyacid Ionic Liquid-Based MCF: An Efficient Heterogeneous Catalyst for Oxidative Desulfurization of Fuel. Materials, 16(8); 3195
Polikarpova, P., A. Akopyan, A. Shlenova, and A. Anisimov (2020). New Mesoporous Catalysts with Brønsted Acid Sites for Deep Oxidative Desulfurization of Model Fuels. Catalysis Communications, 146; 106123
Priatna, S., Y. Hakim, S. Wibyan, S. Sailah, and R. Mohadi (2023). Interlayer Modification of West Java Natural Ben tonite as Hazardous Dye Rhodamine B Adsorption. Science and Technology Indonesia, 8(2); 160–169
Privat, R., J.-N. Jaubert, F. Garcia, and M. Molière (2010). Ethanol-Hydrocarbon Blend Vapor Prediction. J. Eng. Gas Turbines Power, 132(9); 091504
Rohman, A. (2014). Rice Bran Oil’s Role in Health and Cooking. In Wheat and Rice in Disease Prevention and Health. Elsevier, pages 481–490
Smith, G. L., J. E. Eyley, X. Han, X. Zhang, J. Li, N. M. Jacques, H. G. Godfrey, S. P. Argent, L. J. Mc-Cormick McPherson, and S. J. Teat (2019). Reversible Coordinative Binding and Separation of Sulfur Dioxide in a Robust Metal–Organic Framework with Open Copper Sites. Nature Materials, 18(12); 1358–1365
Tchalala, M., P. Bhatt, K. Chappanda, S. Tavares, K. Adil, Y. Belmabkhout, A. Shkurenko, A. Cadiau, N. Heymans, and G. De Weireld (2019). Fluorinated MOF Platform for Selective Removal and Sensing of SO2 from Flue Gas and Air. Nature Communications, 10(1); 1328
Tripathi, N., R. S. Singh, and C. D. Hills (2019). Microbial Removal of Sulphur from Petroleum Coke (Petcoke). Fuel, 235; 1501–1505
Wibiyan, S., A. Wijaya, and P. M. S. B. N. Siregar (2023). Adsorption of Phenol using Cellulose and Hydrochar: Kinetic, Isotherm, and Regeneration Studies. Indonesian Journal of Material Research, 1(2); 61–67
Wu, Y., P. Duan, and C. Yan (2018). Role of Layered Double Hydroxides in Setting, Hydration Degree, Microstructure and Compressive Strength of Cement Paste. Applied Clay Science, 158; 123–131
Yuliasari, N., A. Wijaya, R. Mohadi, E. Elfita, and A. Lesbani (2022). Photocatalytic Degradation of Malachite Green by Layered Double Hydroxide Based Composites. Bulletin of Chemical Reaction Engineering & Catalysis, 17(2); 240–249
Zhang, H., Z. Jin, M. Xu, Y. Zhang, J. Huang, H. Cheng, X. Wang, Z. Zheng, and Y. Ding (2021). Enhanced Iso-propanol Sensing Performance of the CdS Nanoparticle Decorated ZnO Porous Nanosheets-Based Gas Sensors. IEEE Sensors Journal, 21(12); 13041–13047
Zhang, Y., Z. Chen, X. Liu, Z. Dong, P. Zhang, J. Wang, Q. Deng, Z. Zeng, S. Zhang, and S. Deng (2019). Efficient SO2 Removal Using a Microporous Metal–Organic Framework with Molecular Sieving Effect. Industrial & Engineering Chemistry Research, 59(2); 874–882
Zhu, H., W. Lin, Q. Li, Y. Hu, S. Guo, C. Wang, and F. Yan (2020). Bipyridinium-Based Ionic Covalent Triazine Frameworks for CO2, SO2, and NO Capture. ACS Applied Materials & Interfaces, 12(7); 8614–8621
Zhuang, X., Z. Zhang, Y. Wang, and Y. Li (2018). The Effect of Alternative Solvents to n-Hexane on the Green Extraction of Litsea cubeba Kernel Oils as New Oil Sources. Industrial Crops and Products, 126; 340–346
Authors
Mohadi, R., Ahmad, N., Wibiyan, S., Zahara, Z. A. ., Fitri, E. S., Mardiyanto, Royani, I., & Lesbani, A. (2023). Synthesis of Zn/Al-ZnO Composite Using Zn/Al-Layered Double Hydroxide for Oxidative Desulfurization of 4-Methyldibenzothiophene. Science and Technology Indonesia, 8(4), 701–709. https://doi.org/10.26554/sti.2023.8.4.701-709
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