Optimizing Operating Conditions for Oxidative Coupling Methane (OCM) in the Presence of NaCl-MnOx/SiO2
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Published:
Jul 13, 2021
Keywords:
Oxidative coupling of methane (OCM) Ethylene production Methane conversion Novel catalyst
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Abstract
A novel NaCl-MnOx/SiO2, synthesized using slurry mixed method, was used as a catalyst in oxidative coupling of methane process. Optimal conditions were determined using both computational and experimental methods. NaCl, MnOx and SiO2 which are the component of our catalyst are studied. In this research, the catalyst provided the best experimental result when the ratio of MnOx to SiO2 was 2 to 1. CH4 conversion, C2+ selectivity, C2+ yield and C2H4/C2H6 ratio were achieved at 38%, 71%, 27% and 7.2, respectively when operated the process at optimal temperature of 750°C under atmospheric pressure with ratio of CH4:O2 at 4 and 3000 mL g–1 h–1 of weight hourly space velocity (WHSV). The catalytic performance of NaCl-MnOx/SiO2, was found to be higher than other recently developed catalysts. Besides, NaCl-MnOx/SiO2 gave only less than 10% selectivity of the unwanted CO2, while the other SiO2-based catalysts reported as high as 17% of CO2 selectivity. It also achieved high ethylene production when benchmark with previous research. The experimental results were validated using Aspen Plus at temperature ranging from 700 to 850°C.
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Thanasiriruk, M., Saychoo, P., Khajonvittayakul, C., Tongnan, V., Hartley, U. W., & Laosiripojana, N. (2021). Optimizing Operating Conditions for Oxidative Coupling Methane (OCM) in the Presence of NaCl-MnOx/SiO2. Applied Science and Engineering Progress, 14(3), 477–488. https://doi.org/10.14416/j.asep.2020.10.001
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References
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[25] S. Li, “Reaction chemistry of W-Mn/SiO2 catalyst for the oxidative coupling of methane,” Journal of Natural Gas Chemistry, vol. 12, pp. 1–9, 2003.
[26] C. Karakaya, H. Zhua, C. Loebick, J. G. Weissman, and R. J. Kee, “A detailed reaction mechanism for oxidative coupling of methane over Mn/Na2WO4/ SiO2 catalyst for non-isothermal conditions,” Catalysis. Today, vol. 312, pp. 10–22, Aug. 2018.
[27] Z. Yang, P. Yang, L. Zhang, M. Guo, and Y. Yan, “Investigation of low concentration methane combustion in a fluidized bed with Pd/Al2O3 as catalytic particles,” RSC Advances, vol. 4, pp. 59418–59426, Oct. 2014.
[28] C. Khajonvittayakul, V. Tongnan, T. Kangsadan, N. Laosiripojana, S. Jindasuwan, and U. W. Hartley, “Thermodynamic and mechanism study of syngas production via integration of nitrous oxide decomposition and methane partial oxidation in the presence of 10%NiO– La0.3Sr0.7Co0.7Fe0.3O3−δ,” Reaction Kinetics, Mechanisms and Catalysis, vol. 127, pp. 839– 855, Jun. 2019.
[29] J. H. Burgoyne and H. Hirsch, “The combustion of methane at high temperatures,” in Proceedings of the Royal Society A: Mathematical, Physical, 1954, pp. 73–93.
[30] G. E. Keller and M. M. Bhasin, “Synthesis of ethylene via oxidative coupling of methane,” Journal of Catalysis, vol. 73, pp. 9–19, Aug. 1981.
[31] I. Matsuura, Y. Utsumi, M. Nakai, and T. Doi, “Oxidative coupling of methane over lithiumpromoted zinc oxide catalyst,” Chemistry Letters, vol. 11, pp. 1981–1984, 1986.
[32] I. Pasquon, “New processes and perspectives in the field of heterogeneous oxidation catalysis in relation to other methods of oxidation,” Catalysis Today, vol. 1, pp. 297–333, 1987.
[33] K. Otsuka, M. Hatano, and T. Komatsu, “Synthesis of C2H4 by partial oxidation of CH4 over transition metal oxides with alkali-chlorides,” Studies in Surface Science and Catalysis, vol. 36, pp. 383– 387, 1988.
[34] R. Burch, G. D. Squire, and S. C. Tsang, “Comparative study of catalysts for the oxidative coupling of methane,” Applied Catalysis, vol. 43, pp. 105–116, Apr. 1988.
[35] M. Huff, P. M. Torniainen, D. A. Hickman, and L. D. Schmidt, “Partial oxidation of CH4, C2H6 and C3H8 on monoliths at short contact times,” Studies in Surface Science and Catalysis, vol. 81, pp. 315–320, 1994.
[36] V. Fleischer, R. Steuer, S. Parishan, and R. Schomäcker, “Investigation of the surface reaction network of the oxidative coupling of methane over Na2WO4/Mn/SiO2 catalyst by temperature programmed and dynamic experiments,” Journal of Catalysis, vol. 341, pp. 91–103, Jul. 2016.
[37] S. M. K. Shahri and S. M. Alavi, “Kinetic studies of the oxidative coupling ofmethane over the Mn/ Na2WO4/SiO2 catalyst,” Journal of Natural Gas Chemistry, vol. 18, pp. 25-34, Nov. 2008.
[38] S. Sengodan, R. Lan, J. Humphreys, D. Du, W. Xu, H. Wang, and S. Tao, “Advances in reforming and partial oxidation of hydrocarbons for hydrogen production and fuel cell applications,” Renewable and Sustainable Energy Reviews, vol. 82, pp. 761– 780, Feb. 2018.
[39] N. Hiyoshi and T. Ikeda, “Oxidative coupling of methane over alkali chloride–Mn–Na2WO4/ SiO2 catalysts: Promoting effect of molten alkali chloride,” Fuel Processing Technology, vol. 133, pp. 29–34, May 2015.
[40] A. Machocki and R. Jezior, “Oxidative coupling of methane over a sodium-calcium oxide catalyst modified with chloride ions” Chemical Engineering Journal, vol. 137, pp. 643–652, Apr. 2008.
[41] R. Burch, G. D. Squire, and S. C. Tsang, “Role of chlorine in improving selectivity in the oxidative coupling of methane to ethylene,” Applied Catalysis, vol. 46, pp. 69–87, Jan. 1989.
[42] A. Malekzadeh, A. K. Dalai, A. Khodadadi, and Y. Mortazavi, “Structural features of Na2WO4– MOx/SiO2 catalysts in oxidative coupling of methane reaction,” Catalysis Communications, vol. 9, pp. 960–965, Mar. 2008.
[43] G. D. Souza, N. M. Balzaretti, N. R. Marcilio, and O. Perez-Lopez, “Decomposition of ethanol over Ni-Al catalysts: Effect of copper addition,” Procedia Engineering, vol. 42, pp. 370–382, 2012.
[44] A. Gupta and S. Kerdsuwan, “Efficient energy conversion of wastes and fuels in power systems,” KMUTNB: International Journal of Applied Science and Technology, vol. 7, no. 2, pp. 1–26, 2014.
[45] M. R. Lee, M. J. Park, W. Jeon, J. W. Choi, Y. W. Suh, and D. J. Suh, “A kinetic model for the oxidative coupling of methane over Na2WO4/ Mn/SiO2,” Fuel Processing Technology, vol. 96, pp. 175–182, Apr. 2012.
[46] X. Li, G. Zhang, K. Tang, O. Ostrovski, and R. Tronstad, “Carbothermal reduction of quartz in methane-hydrogen-argon gas mixture,” Metallurgical and Materials Transactions B, vol. 46, no. 5, pp. 2384–2393, 2015.
[47] V. H. Rane, S. T. Chaudhari, and V. R. Choudhary, “Influence of alkali metal doping on surface properties and catalytic activity/selectivity of CaO catalysts in oxidative coupling ofmethane,” Journal of Natural Gas Chemistry, vol. 17, pp. 313–320, Dec. 2008.
[48] W. Liang, S. Sarsani, D. West, A. Mamedov, I. Lengyel, H. Perez, and J. Lowrey, “Performance improvement for a fixed-bed reactor with layered loading catalysts of different catalytic properties for oxidative coupling of methane,” Catalysis Today, vol. 299, pp. 60–66, Jan. 2018.
[49] T. W. Elkins, S. J. Roberts, and H. E. Hagelin- Weaver, “Effects of alkali and alkaline-earth metal dopants on magnesium oxide supported rare-earth oxide catalysts in the oxidative coupling of methane,” Applied Catalysis A: General, vol. 528, pp. 175–190, Nov. 2016.
[50] S. Gua, H. S. Oh, J. W. Choi, D. J. Suh, J. Jae, J. Choi, and J. M. Ha, “Effects of metal or metal oxide additives on oxidative coupling of methane using Na2WO4/SiO2 catalysts: Reducibility of metal additives to manipulate the catalytic activity,” Applied Catalysis A: General, vol. 562, pp. 114–119, Jul. 2018.
[51] H. Godinia, A. Gili, O. Görke, S. Arndt, U. Simon, A. Thomas, R. Schomäcker, and G. Wozny, “Sol–gel method for synthesis of Mn–Na2WO4/ SiO2 catalystfor methane oxidative coupling,” Catalysis Today, vol. 236, pp. 12–22, Nov. 2014.
[52] M. Yildiza, U. Simon, T. Otremba, Y. Aksu, K. Kailasam, and A. Thomas, “Support material variation for the MnxOy-Na2WO4/SiO2 catalyst,” Catalysis Today, vol. 228, pp. 5–14, Jun. 2014.
[53] M. Yildiz, Y. Aksu, U. Simon, K. Kailasam, O. Goerke, F. Rosowski, R. Schomacker, A. Thomas, and S. Arndt, “Enhanced catalytic performance of MnxOy–Na2WO4/SiO2 for the oxidative coupling of methane using an ordered mesoporous silica support,” Chemical Communications, vol. 50, pp. 14440–14442, 2014.
[2] H. Zimmermann and R. Walzl, “Ethylene,” in Ullmann's encyclopedia of industrial chemistry, 2012, vol. 3, pp. 465–526.
[3] O. Adekomaya, T. Jamiru, E. Sadiku, and A. Adediran, “Sustainability of high temperature polymeric meterials for electronic packaging applications,” International Journal of Applied Science and Technology, vol. 11, no. 13, pp. 217– 224, 2018.
[4] Y. Samphawamontri, T. Srinophakun, P. Dittanet and K. Choroencham, “Heat integrated process design, simulation and control of polymerization and drying sections for HDPE production,” International Journal of Applied Science and Technology, vol. 9, no. 2, pp. 121–136, 2016.
[5] K. Wagialla, “Petrochemical aromatics from liquid hydrocaybons a technoeconomic assesment,” presented at the 7th Saudi Engineering Conference, Riyadh, Saudi Arabia Stuttgart, Dec. 2–5, 2007.
[6] T. Ren, M. Patel, and K. Blok, “Olefins from conventional and heavy feedstocks: Energy use in steam cracking and alternative processes,” Energy Journal, vol. 31, pp. 425–451, Jun. 2006.
[7] A. Galadima and O. Muraza, “Revisiting the oxidative coupling of methane to ethylene in the golden period of shale gas: A review,” Journal of Industrial and Engineering Chemistry, vol. 37, pp. 1–13, Mar. 2016.
[8] J. Kim, L. H. Park, J. M. Ha, and E. D. Park, “Oxidative coupling of methane over Mn2O3- Na2WO4/SiC catalyst,” Catalysts, vol. 9, Apr. 2019.
[9] C. T. Au, K. D. Chen, H. X. Dai, Y. W. Liu, J. Z. Luo, and C. F. Ng, “Oxidative dehydrogenation of ethane to ethene over BaO- and BaBr2-Modified HO2O3 catalysts,” Journal of Catalysis, vol. 179, pp. 300–308, Jul. 1998.
[10] K. Otsuka and T. Komatsu, “Active catalysts in oxidative coupling of methane,” Journal of the Chemical Society, Chemical Communications, vol. 5, pp. 388–389, Jan. 1987.
[11] K. Otsuka, Q. Liu, M. Hatano, and A. Morikawa “Synthesis of ethylene by partial oxidation of methane over the oxides of transition elements with LiCl,” Chemistry Letters, vol. 15, no. 6, pp. 903– 906, 1986.
[12] J. S. Ahari, M. T. Sadeghi, and S. Z. Pashne, “Optimization of OCM reaction conditions over Na–W–Mn/SiO2 catalyst at elevated pressure,” Journal of the Taiwan Institute of Chemical Engineers, vol. 42, pp. 751–759, Feb. 2011.
[13] T. P. Tiemersma, M. J. Tuinier, F. Gallucci, J. A. M. Kuipers, and M. van Sint Annaland, “A kinetics study for the oxidative coupling of methane on a Mn/Na2WO4/SiO2 catalyst,” Applied Catalysis A: General, vol. 433–434, pp. 96–108, May. 2012.
[14] A. Malekzadeh, A. Khodadadi, M. Abedini, M. Amini, A. Bahramian, and A. K. Dalai, “Correlation of electrical properties and performance of OCM MOx/Na2WO4/SiO2 catalysts,” Catalysis Communications, vol. 2, pp. 241–247, Jul. 2001.
[15] S. Arndt, T. Otremba, U. Simon, M. Yildiz, H. Schubert, and R. Schomäcker, “Mn–Na2WO4/SiO2 as catalyst for the oxidative coupling of methane. What is really known?,” Applied Catalysis A: General, vol. 425–426, pp. 53–61, Feb. 2012.
[16] A. Palermo, J. P. H. Vazquez, A. F. Lee, M. S. Tikhov, and R. M. Lambert, “Critical influence of the amorphous silica-to-cristobalite phase transition on the performance of Mn/Na2WO4/ SiO2 catalysts for the oxidative coupling of methane,” Journal of Catalysis, vol. 177, pp. 259– 266, Apr. 1998.
[17] N. S. Hayek, N. S. Lucas, C. W. Damouny, and O. M. Gazit, “Critical surface parameters for the oxidative coupling of methane over the Mn− Na−W/SiO2 Catalyst,” ACS Applied Materials and Interfaces, vol. 9, pp. 40404–40411, 2017.
[18] J. Wang, L. Chou, B. Zhang, H. Song, J. Zhao, J. Yang, and S. Li, “Comparative study on oxidation of methane to ethane and ethylene over Na2WO4–Mn/SiO2 catalysts prepared by different methods,” Journal of Molecular Catalysis A: Chemical, vol. 245, pp. 272–277, Sep. 2005.
[19] L. Chou, Y. Cai, B. Zhang, J. Niu, S. Ji, and S. Li, “Oxidative coupling of methane over Na-W-Mn/ SiO2 catalysts at elevated pressures,” Journal of Natural Gas Chemistry, vol. 11, pp. 131–136, Dec. 2002.
[20] A. Aseem and M. P. Harold, “C2 yield enhancement during oxidative coupling of methane in a nonpermselective porous membrane reactor,” Chemical Engineering Science, vol. 175, pp. 199– 207, Sep. 2017.
[21] B. L. Farrell, V. O. Igenegbai, and S. Linic, “A viewpoint on direct methane conversion to ethane and ethylene using oxidative coupling on solid catalysts,” ACS Catalysis, vol. 6, pp. 4340–4346, May. 2016.
[22] A. Farsi, A. Moradi, S. Ghader, V. Shadravan, and Z. A. Manan, “Kinetics investigation of direct natural gas conversion by oxidative coupling of methane,” Journal of Natural Gas Science and Engineering, vol. 2, pp. 270–274, Sep. 2010.
[23] I. M. Alibe, K. A. Matori, E. Saion, A. M. Alibe, M. H. M. Zaid, and E. A. A. G. Engku, “A facile synthesis of amorphous silica nanaparticles by simple thermal treatment route,” Digest Journal of Nanomaterials and Biostructures, vol. 11, no. 4, pp. 1155–1164, 2016.
[24] T. W. Elkins and H. E. Hagelin-Weaver, “Characterization of Mn-Na2WO4/SiO2 and Mn-Na2WO4/MgO catalysts for the oxidative coupling of methane,” Applied Catalysis A: General, vol. 497, pp. 96–106, Feb. 2015.
[25] S. Li, “Reaction chemistry of W-Mn/SiO2 catalyst for the oxidative coupling of methane,” Journal of Natural Gas Chemistry, vol. 12, pp. 1–9, 2003.
[26] C. Karakaya, H. Zhua, C. Loebick, J. G. Weissman, and R. J. Kee, “A detailed reaction mechanism for oxidative coupling of methane over Mn/Na2WO4/ SiO2 catalyst for non-isothermal conditions,” Catalysis. Today, vol. 312, pp. 10–22, Aug. 2018.
[27] Z. Yang, P. Yang, L. Zhang, M. Guo, and Y. Yan, “Investigation of low concentration methane combustion in a fluidized bed with Pd/Al2O3 as catalytic particles,” RSC Advances, vol. 4, pp. 59418–59426, Oct. 2014.
[28] C. Khajonvittayakul, V. Tongnan, T. Kangsadan, N. Laosiripojana, S. Jindasuwan, and U. W. Hartley, “Thermodynamic and mechanism study of syngas production via integration of nitrous oxide decomposition and methane partial oxidation in the presence of 10%NiO– La0.3Sr0.7Co0.7Fe0.3O3−δ,” Reaction Kinetics, Mechanisms and Catalysis, vol. 127, pp. 839– 855, Jun. 2019.
[29] J. H. Burgoyne and H. Hirsch, “The combustion of methane at high temperatures,” in Proceedings of the Royal Society A: Mathematical, Physical, 1954, pp. 73–93.
[30] G. E. Keller and M. M. Bhasin, “Synthesis of ethylene via oxidative coupling of methane,” Journal of Catalysis, vol. 73, pp. 9–19, Aug. 1981.
[31] I. Matsuura, Y. Utsumi, M. Nakai, and T. Doi, “Oxidative coupling of methane over lithiumpromoted zinc oxide catalyst,” Chemistry Letters, vol. 11, pp. 1981–1984, 1986.
[32] I. Pasquon, “New processes and perspectives in the field of heterogeneous oxidation catalysis in relation to other methods of oxidation,” Catalysis Today, vol. 1, pp. 297–333, 1987.
[33] K. Otsuka, M. Hatano, and T. Komatsu, “Synthesis of C2H4 by partial oxidation of CH4 over transition metal oxides with alkali-chlorides,” Studies in Surface Science and Catalysis, vol. 36, pp. 383– 387, 1988.
[34] R. Burch, G. D. Squire, and S. C. Tsang, “Comparative study of catalysts for the oxidative coupling of methane,” Applied Catalysis, vol. 43, pp. 105–116, Apr. 1988.
[35] M. Huff, P. M. Torniainen, D. A. Hickman, and L. D. Schmidt, “Partial oxidation of CH4, C2H6 and C3H8 on monoliths at short contact times,” Studies in Surface Science and Catalysis, vol. 81, pp. 315–320, 1994.
[36] V. Fleischer, R. Steuer, S. Parishan, and R. Schomäcker, “Investigation of the surface reaction network of the oxidative coupling of methane over Na2WO4/Mn/SiO2 catalyst by temperature programmed and dynamic experiments,” Journal of Catalysis, vol. 341, pp. 91–103, Jul. 2016.
[37] S. M. K. Shahri and S. M. Alavi, “Kinetic studies of the oxidative coupling ofmethane over the Mn/ Na2WO4/SiO2 catalyst,” Journal of Natural Gas Chemistry, vol. 18, pp. 25-34, Nov. 2008.
[38] S. Sengodan, R. Lan, J. Humphreys, D. Du, W. Xu, H. Wang, and S. Tao, “Advances in reforming and partial oxidation of hydrocarbons for hydrogen production and fuel cell applications,” Renewable and Sustainable Energy Reviews, vol. 82, pp. 761– 780, Feb. 2018.
[39] N. Hiyoshi and T. Ikeda, “Oxidative coupling of methane over alkali chloride–Mn–Na2WO4/ SiO2 catalysts: Promoting effect of molten alkali chloride,” Fuel Processing Technology, vol. 133, pp. 29–34, May 2015.
[40] A. Machocki and R. Jezior, “Oxidative coupling of methane over a sodium-calcium oxide catalyst modified with chloride ions” Chemical Engineering Journal, vol. 137, pp. 643–652, Apr. 2008.
[41] R. Burch, G. D. Squire, and S. C. Tsang, “Role of chlorine in improving selectivity in the oxidative coupling of methane to ethylene,” Applied Catalysis, vol. 46, pp. 69–87, Jan. 1989.
[42] A. Malekzadeh, A. K. Dalai, A. Khodadadi, and Y. Mortazavi, “Structural features of Na2WO4– MOx/SiO2 catalysts in oxidative coupling of methane reaction,” Catalysis Communications, vol. 9, pp. 960–965, Mar. 2008.
[43] G. D. Souza, N. M. Balzaretti, N. R. Marcilio, and O. Perez-Lopez, “Decomposition of ethanol over Ni-Al catalysts: Effect of copper addition,” Procedia Engineering, vol. 42, pp. 370–382, 2012.
[44] A. Gupta and S. Kerdsuwan, “Efficient energy conversion of wastes and fuels in power systems,” KMUTNB: International Journal of Applied Science and Technology, vol. 7, no. 2, pp. 1–26, 2014.
[45] M. R. Lee, M. J. Park, W. Jeon, J. W. Choi, Y. W. Suh, and D. J. Suh, “A kinetic model for the oxidative coupling of methane over Na2WO4/ Mn/SiO2,” Fuel Processing Technology, vol. 96, pp. 175–182, Apr. 2012.
[46] X. Li, G. Zhang, K. Tang, O. Ostrovski, and R. Tronstad, “Carbothermal reduction of quartz in methane-hydrogen-argon gas mixture,” Metallurgical and Materials Transactions B, vol. 46, no. 5, pp. 2384–2393, 2015.
[47] V. H. Rane, S. T. Chaudhari, and V. R. Choudhary, “Influence of alkali metal doping on surface properties and catalytic activity/selectivity of CaO catalysts in oxidative coupling ofmethane,” Journal of Natural Gas Chemistry, vol. 17, pp. 313–320, Dec. 2008.
[48] W. Liang, S. Sarsani, D. West, A. Mamedov, I. Lengyel, H. Perez, and J. Lowrey, “Performance improvement for a fixed-bed reactor with layered loading catalysts of different catalytic properties for oxidative coupling of methane,” Catalysis Today, vol. 299, pp. 60–66, Jan. 2018.
[49] T. W. Elkins, S. J. Roberts, and H. E. Hagelin- Weaver, “Effects of alkali and alkaline-earth metal dopants on magnesium oxide supported rare-earth oxide catalysts in the oxidative coupling of methane,” Applied Catalysis A: General, vol. 528, pp. 175–190, Nov. 2016.
[50] S. Gua, H. S. Oh, J. W. Choi, D. J. Suh, J. Jae, J. Choi, and J. M. Ha, “Effects of metal or metal oxide additives on oxidative coupling of methane using Na2WO4/SiO2 catalysts: Reducibility of metal additives to manipulate the catalytic activity,” Applied Catalysis A: General, vol. 562, pp. 114–119, Jul. 2018.
[51] H. Godinia, A. Gili, O. Görke, S. Arndt, U. Simon, A. Thomas, R. Schomäcker, and G. Wozny, “Sol–gel method for synthesis of Mn–Na2WO4/ SiO2 catalystfor methane oxidative coupling,” Catalysis Today, vol. 236, pp. 12–22, Nov. 2014.
[52] M. Yildiza, U. Simon, T. Otremba, Y. Aksu, K. Kailasam, and A. Thomas, “Support material variation for the MnxOy-Na2WO4/SiO2 catalyst,” Catalysis Today, vol. 228, pp. 5–14, Jun. 2014.
[53] M. Yildiz, Y. Aksu, U. Simon, K. Kailasam, O. Goerke, F. Rosowski, R. Schomacker, A. Thomas, and S. Arndt, “Enhanced catalytic performance of MnxOy–Na2WO4/SiO2 for the oxidative coupling of methane using an ordered mesoporous silica support,” Chemical Communications, vol. 50, pp. 14440–14442, 2014.