Solubility and mass transfer of H2, CH4, and their mixtures in vacuum gas oil: An experimental and modeling study

doi:10.1016/j.cjche.2019.05.010

Abstract

Abstract: In this work, the solubility data and liquid-phase mass transfer coefficients of hydrogen (H₂), methane (CH₄) and their mixtures in vacuum gas oil (VGO) at temperatures (353.15-453.15 K) and pressures (1-7 MPa) were measured, which are necessary for catalytic cracking process simulation and design. The solubility of H₂ and CH₄ in VGO increases with the increase of pressure, but decreases with the increase of temperature. Henry's constants of H₂ and CH₄ follow the relation of ln H=-413.05/T + 5.27 and ln H=-990.67/T + 5.87, respectively. The molar fractions of H₂ and system pressures at different equilibrium time were measured to estimate the liquid-phase mass transfer coefficients. The results showed that with the increase of pressure, the liquid-phase mass transfer coefficients increase. Furthermore, the solubility of H₂ and CH₄ in VGO was predicted by the predictive COSMO-RS model, and the predicted values agree well with experimental data. In addition, the gas-liquid equilibrium (GLE) for H₂ + CH₄ + VGO system at different feeding gas ratios in volume fraction (i.e., H₂ 85% + CH₄ 15% and H₂ 90% + CH₄ 10%) was measured. The selectivity of H₂ to CH₄ predicted by the COSMO-RS model agrees well with experimental data. This work provides the basic thermodynamic and dynamic data for fuel oil catalytic cracking processes.

Key words: H₂, CH₄, Vacuum gas oil (VGO), Solubility, Mass transfer, COSMO-RS model

摘要： In this work, the solubility data and liquid-phase mass transfer coefficients of hydrogen (H₂), methane (CH₄) and their mixtures in vacuum gas oil (VGO) at temperatures (353.15-453.15 K) and pressures (1-7 MPa) were measured, which are necessary for catalytic cracking process simulation and design. The solubility of H₂ and CH₄ in VGO increases with the increase of pressure, but decreases with the increase of temperature. Henry's constants of H₂ and CH₄ follow the relation of ln H=-413.05/T + 5.27 and ln H=-990.67/T + 5.87, respectively. The molar fractions of H₂ and system pressures at different equilibrium time were measured to estimate the liquid-phase mass transfer coefficients. The results showed that with the increase of pressure, the liquid-phase mass transfer coefficients increase. Furthermore, the solubility of H₂ and CH₄ in VGO was predicted by the predictive COSMO-RS model, and the predicted values agree well with experimental data. In addition, the gas-liquid equilibrium (GLE) for H₂ + CH₄ + VGO system at different feeding gas ratios in volume fraction (i.e., H₂ 85% + CH₄ 15% and H₂ 90% + CH₄ 10%) was measured. The selectivity of H₂ to CH₄ predicted by the COSMO-RS model agrees well with experimental data. This work provides the basic thermodynamic and dynamic data for fuel oil catalytic cracking processes.

关键词: H₂, CH₄, Vacuum gas oil (VGO), Solubility, Mass transfer, COSMO-RS model

Zhigang Lei, Yifan Jiang, Yao Liu, Yichun Dong, Gangqiang Yu, Yanyong Sun, Ruili Guo. Solubility and mass transfer of H₂, CH₄, and their mixtures in vacuum gas oil: An experimental and modeling study[J]. Chinese Journal of Chemical Engineering, 2019, 27(12): 3000-3009.

References

[1] J.G. Speight, The Desulfurization of Heavy Oils and Residua, CRC Press, 1999.
[2] M.R. Riazi, Y.A. Roomi, A method to predict solubility of hydrogen in hydrocarbons and their mixtures, Chem. Eng. Sci. 62(2007) 6649-6658.
[3] I.V. Babich, J.A. Moulijn, Science and technology of novel processes for deep desulfurization of oil refinery streams:A review, Fuel 82(2003) 607-631.
[4] A.N. Harji, P.E. Koppel, W.L. Mazurek, P. Meysami, Processing options for bitumen upgrading, Canadian International Petroleum Conference, Petroleum Society of Canada, 2003 https://doi.org/10.2118/2003-140.
[5] H. Cai, J.M. Shaw, K.H. Chung, Hydrogen solubility measurements in heavy oil and bitumen cuts, Fuel 80(2001) 1055-1063.
[6] M. Saajanlehto, P. Uusi-Kyyny, V. Alopaeus, Hydrogen solubility in heavy oil systems:Experiments and modeling, Fuel 137(2014) 393-404.
[7] C. Liu, G. Que, Determination of hydrogen solubilities in petroleum fractions, Pet. Refin. Eng. 29(1999) 33-36.
[8] S. Liaw, S. Chiang, G.E. Klinzing, Hydrogen solubility of hydrogen-methane-tetralin and hydrogen-ethane-tetralin systems at elevated temperatures and pressures, Fuel 70(1991) 771-777.
[9] Z. Zhou, Z. Cheng, D. Yang, X. Zhou, W. Yuan, Solubility of hydrogen in pyrolysis gasoline, J. Chem. Eng. Data 51(2006) 972-976.
[10] L.J. Florusse, C.J. Peters, J.C. Pamies, L.F. Vega, H. Meijer, Solubility of hydrogen in heavy n-alkanes:Experiments and SAFT modeling, AIChE J. 49(2003) 3260-3269.
[11] L.R. Field, E. Wilhelm, R. Battino, The solubility of gases in liquids 6. Solubility of N₂, O₂, CO, CO₂, CH₄, and CF₄ in methylcyclohexane and toluene at 283 to 313 K, J. Chem. Thermodyn. 6(1974) 237-243.
[12] P.J. Hesse, R. Battino, P. Scharlin, E. Wilhelm, Solubility of gases in liquids. 20. Solubility of He, Ne, Ar, Kr, N₂, O₂, CH₄, CF₄, and SF₆ in n-alkanes n-Cl H_2l+2(6≤ l ≤ 16) at 298.15 K, J. Chem. Eng. Data 41(1996) 195-201.
[13] M. Zirrahi, H. Hassanzadeh, J. Abedi, M. Moshfeghian, Prediction of solubility of CH₄, C₂H₆, CO₂, N₂ and CO in bitumen, Can. J. Chem. Eng. 92(2014) 563-572.
[14] A. Klamt, Conductor-like screening model for real solvents:A new approach to the quantitative calculation of solvation phenomena, J. Phys. Chem. 99(1995) 2224-2235.
[15] A. Klamt, F. Eckert, COSMO-RS:A novel and efficient method for the a priori prediction of thermophysical data of liquids, Fluid Phase Equilib. 172(2000) 43-72.
[16] F. Eckert, A. Klamt, Validation of the COSMO-RS method:Six binary systems, Ind. Eng. Chem. Res. 40(2001) 2371-2378.
[17] S. Lin, J. Chang, S. Wang, W.A. Goddard, S.I. Sandler, Prediction of vapor pressures and enthalpies of vaporization using a COSMO solvation model, J. Phys. Chem. A 108(2004) 7429-7439.
[18] A. Klamt, COSMO-RS:From Quantum Chemistry to Fluid Phase Thermodynamics and Drug Design, Elsevier, 2005.
[19] A. Klamt, F. Eckert, M. Diedenhofen, Prediction or partition coefficients and activity coefficients of two branched compounds using COSMOtherm, Fluid Phase Equilib. 285(2009) 15-18.
[20] V.R. Ferro, E. Ruiz, M. Tobajas, J.F. Palomar, Integration of COSMO-based methodologies into commercial process simulators:Separation and purification of reuterin, AIChE J. 58(2012) 3404-3415.
[21] A. Klamt, F. Eckert, M. Diedenhofen, M.E. Beck, First principles calculations of aqueous pKa values for organic and inorganic acids using COSMO-RS reveal an inconsistency in the slope of the pKa scale, J. Phys. Chem. A 107(2003) 9380-9386.
[22] Z. Lei, C. Dai, B. Chen, Gas solubility in ionic liquids, Chem. Rev. 114(2014) 1289-1326.
[23] C.C. Pye, T. Ziegler, E. Van Lenthe, J.N. Louwen, An implementation of the conductor-like screening model of solvation within the Amsterdam density functional package-part II. COSMO for real solvents, Can. J. Chem. 87(2009) 790-797.
[24] Z. Lei, J. Yuan, J. Zhu, Solubility of CO₂ in propanone, 1-ethyl-3-methylimidazolium tetrafluoroborate, and their mixtures, J. Chem. Eng. Data 55(2010) 4190-4194.
[25] Z. Lei, C. Dai, Q. Yang, J. Zhu, B. Chen, UNIFAC model for ionic liquid-CO (H₂) systems:An experimental and modeling study on gas solubility, AIChE J. 60(2014) 4222-4231.
[26] C. Dai, W. Wei, Z. Lei, Solubility of CO₂ in the mixture of methanol and ZIF-8 at low temperatures, J. Chem. Eng. Data 60(2015) 1311-1317.
[27] Y.J. Heintz, L. Sehabiague, B.I. Morsi, K.L. Jones, D.R. Luebke, H.W. Pennline, Hydrogen sulfide and carbon dioxide removal from dry fuel gas streams using an ionic liquid as a physical solvent, Energy Fuel 23(2009) 4822-4830.
[28] H.W. Pennline, D.R. Luebke, K.L. Jones, C.R. Myers, B.I. Morsi, Y.J. Heintz, J.B. Ilconich, Progress in carbon dioxide capture and separation research for gasification-based power generation point sources, Fuel Process. Technol. 89(2008) 897-907.
[29] Y.J. Heintz, L. Sehabiague, B.I. Morsi, K.L. Jones, H.W. Pennline, Novel physical solvents for selective CO₂ capture from fuel gas streams at elevated pressures and temperatures, Energy Fuel 22(2008) 3824-3837.
[30] R.V. Chaudhari, R.V. Gholap, G. Emig, H. Hofmann, Gas-liquid mass transfer in "dead-end" autoclave reactors, Can. J. Chem. Eng. 65(1987) 744-751.
[31] J. Kumełan, D. Tuma, G. Maurer, Partial molar volumes of selected gases in some ionic liquids, Fluid Phase Equilib. 275(2009) 132-144.
[32] E. Brunner, Solubility of hydrogen in 10 organic solvents at 298.15, 323.15, and 373.15 K, J. Chem. Eng. Data 30(1985) 269-273.
[33] M.M.P. Zieverink, M.T. Kreutzer, A. Freek Kapteijn, J.A. Moulijn, Gas-liquid mass transfer in benchscale stirred tanks-Fluid properties and critical impeller speed for gas induction, Ind. Eng. Chem. Res. 45(2006) 4574-4581.
[34] E. Dietrich, C. Mathieu, H. Delmas, J. Jenck, Raney-nickel catalyzed hydrogenations:Gas-liquid mass transfer in gas-induced stirred slurry reactors, Chem. Eng. Sci. 47(1992) 3597-3604.
[35] A. Sharma, C. Julcour, A.A. Kelkar, R.M. Deshpande, H. Delmas, Mass transfer and solubility of CO and H₂ in ionic liquid. Case of [BMIM][PF₆] with gasinducing stirrer reactor, Ind. Eng. Chem. Res. 48(2009) 4075-4082.
[36] M. Teramoto, S. Tai, K. Nishii, H. Teranishi, Effects of pressure on liquid-phase mass transfer coefficients, Chem. Eng. J. 8(1974) 223-226.
[37] M. Gonzalezmiquel, J. Palomar, S. Omar, F. Rodriguez, CO₂/N₂ selectivity prediction in supported ionic liquid membranes (SILMs) by COSMO-RS, Ind. Eng. Chem. Res. 50(2011) 5739-5748.
[38] Y. Shimoyama, A. Ito, Predictions of cation and anion effects on solubilities, selectivities and permeabilities for CO₂ in ionic liquid using COSMO based activity coefficient model, Fluid Phase Equilib. 297(2010) 178-182.
[39] Y.S. Kim, W.Y. Choi, J.H. Jang, K.P. Yoo, C.S. Lee, Solubility measurement and prediction of carbon dioxide in ionic liquids, Fluid Phase Equilib. 228-229(2005) 439-445.
[40] T. Banerje, A. Khanna, Infinite dilution activity coefficients for trihexyltetradecyl phosphonium ionic liquids:Measurements and COSMO-RS prediction, J. Chem. Eng. Data 51(2006) 2170-2177.
[41] J. Han, C. Dai, G. Yu, Z. Lei, Parameterization of COSMO-RS model for ionic liquids, Green Energy Environ. 3(2018) 247-265.
[42] T. Gerlach, T. Ingram, G. Sieder, I. Smirnova, Modeling the solubility of CO₂ in aqueous methyl diethanolamine solutions with an electrolyte model based on COSMORS, Fluid Phase Equilib. 461(2018) 39-50.
[43] H. Jiang, B. Diao, D. Xu, L. Zhang, Y. Ma, J. Gao, Y. Wang, Deep eutectic solvents effect on vapor-liquid phase equilibrium for separation of allyl alcohol from its aqueous solution, J. Mol. Liq. 279(2019) 524-529.
[44] J. Gao, D. Xu, X. Cha, Z. Cui, L. Zhang, Y. Wang, Multiscale modeling and liquid-liquid equilibria insights for the extraction of heterocyclic nitrogen compounds from coal tar via[emim] [TOS] as extractant, J. Mol. Liq. 277(2019) 825-832.
[45] X. Liu, D. Xu, B. Diao, L. Zhang, J. Gao, D. Liu, Y. Wang, Choline chloride based deep eutectic solvents selection and liquid-liquid equilibrium for separation of dimethyl carbonate and ethanol, J. Mol. Liq. 275(2019) 347-353.
[46] Y. Ma, J. Gao, Y. Wang, J. Hu, P. Cui, Ionic liquid-based CO₂ capture in power plants for low carbon emissions, Int. J. Greenhouse Gas Control 75(2018) 134-139.
[47] Y. Zhou, D. Xu, L. Zhang, Y. Ma, X. Ma, J. Gao, Y. Wang, Separation of thioglycolic acid from its aqueous solution by ionic liquids:Ionic liquids selection by the COSMO-SAC model and liquid-liquid phase equilibrium, J. Chem. Thermodyn. 118(2018) 263-273.
[48] G. Wen, W. Bai, F. Zheng, J.A. Reyes-Labarta, Y. Ma, Y. Wang, J. Gao, Ternary liquid-liquid equilibrium of an azeotropic mixture (hexane + methanol) with different imidazolium-based ionic liquids at T=298.15 K and 101.325 kPa, Fluid Phase Equilib. 461(2018) 51-56.
[49] K. Zhang, D. Xu, Y. Zhou, P. Shi, J. Gao, Y. Wang, Isobaric vapor-liquid phase equilibrium measurements, correlation, and prediction for separation of the mixtures of cyclohexanone and alcohols, J. Chem. Eng. Data 63(2018) 2038-2045.
[50] G. Wen, X. Geng, W. Bai, Y. Wang, J. Gao, Ternary liquid-liquid equilibria for systems containing (dimethyl carbonate or methyl acetate + methanol +1-methylmidazole hydrogen sulfate) at 298.15 K and 318.15 K, J. Chem. Thermodyn. 121(2018) 49-54.
[51] P. Wang, D. Xu, P. Yan, J. Gao, L. Zhang, Y. Wang, Separation of azeotrope (ethanol and ethyl methyl carbonate) by different imidazolium-based ionic liquids:Ionic liquids interaction analysis and phase equilibrium measurements, J. Mol. Liq. 261(2018) 89-95.
[52] P.G.T. Fogg, W. Gerrard, Solubility of Gases in Liquids:A Critical Evaluation of Gas/Liquid Systems in Theory and Practice, Wiley, New York, 1991.

Solubility and mass transfer of H₂, CH₄, and their mixtures in vacuum gas oil: An experimental and modeling study

Solubility and mass transfer of H₂, CH₄, and their mixtures in vacuum gas oil: An experimental and modeling study

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	Jingzhou Guo, Yuanzuo Zou, Bo Shi, Yuan Pu, Jiexin Wang, Dan Wang, Jianfeng Chen. Experimental verification of nanonization enhanced solubility for poorly soluble optoelectronic molecules [J]. Chinese Journal of Chemical Engineering, 2023, 60(8): 8-15.
[2]	Bo Yu, Guang Fu, Xinpei Li, Libo Zhang, Jing Li, Hongtao Qu, Dongbin Wang, Qingfeng Dong, Mengmeng Zhang. Arsenic removal from acidic industrial wastewater by ultrasonic activated phosphorus pentasulfide [J]. Chinese Journal of Chemical Engineering, 2023, 60(8): 46-52.
[3]	Jiahao Lu, Zhimeng Wang, Qi Zhang, Cheng Sun, Yanyan Zhou, Sijia Wang, Xiangyun Qiu, Shoudong Xu, Rentian Chen, Tao Wei. The effects of amino groups and open metal sites of MOFs on polymer-based electrolytes for all-solid-state lithium metal batteries [J]. Chinese Journal of Chemical Engineering, 2023, 60(8): 80-89.
[4]	Xingjuan Liang, Dehua Xu, Zhengjuan Yan, Jingxu Yang, Xinlong Wang, Zhiye Zhang, Jingli Wu, Honggang Zhen. Solid-liquid phase equilibrium for the system ammonium polyphosphate-urea ammonium nitrate-potassium chloride-water at 273.2 K [J]. Chinese Journal of Chemical Engineering, 2023, 60(8): 131-142.
[5]	Huiqi Wang, Jianpo Ren, Shihao Zhang, Jiayu Dai, Yue Niu, Ketao Shi, Qiuxiang Yin, Ling Zhou. Measurement and correlation of solubility of 9-fluorenone in 11 pure organic solvents from T = 283.15 to 323.15 K [J]. Chinese Journal of Chemical Engineering, 2023, 60(8): 235-241.
[6]	Anjun Liu, Jie Chen, Meng Guo, Chengmin Chen, Meihong Yang, Chao Yang. The internal circulations on internal mass transfer rate of a single drop in nonlinear uniaxial extensional flow [J]. Chinese Journal of Chemical Engineering, 2023, 59(7): 51-60.
[7]	Xun Tao, Fan Zhou, Xinlei Yu, Songling Guo, Yunfei Gao, Lu Ding, Guangsuo Yu, Zhenghua Dai, Fuchen Wang. Effect of carbon dioxide on oxy-fuel combustion of hydrogen sulfide: An experimental and kinetic modeling [J]. Chinese Journal of Chemical Engineering, 2023, 59(7): 105-117.
[8]	Wen Yu, Yiyang Bo, Yiling Luo, Xiyan Huang, Rixiang Zhang, Jiaheng Zhang. Enhancing effect of choline chloride-based deep eutectic solvents with polyols on the aqueous solubility of curcumin-insight from experiment and theoretical calculation [J]. Chinese Journal of Chemical Engineering, 2023, 59(7): 160-168.
[9]	Zhonghao Li, Yuanyuan Yang, Huanong Cheng, Yun Teng, Chao Li, Kangkang Li, Zhou Feng, Hongwei Jin, Xinshun Tan, Shiqing Zheng. Measurement and model of density, viscosity, and hydrogen sulfide solubility in ferric chloride/trioctylmethylammonium chloride ionic liquid [J]. Chinese Journal of Chemical Engineering, 2023, 59(7): 210-221.
[10]	Yun-Zhang Liu, Lu-Yao Zhang, Dan He, Li-Zhen Chen, Zi-Shuai Xu, Jian-Long Wang. Solubility measurement, correlation and thermodynamic properties of 2, 3, 4-trichloro-1, 5-dinitrobenzene in fifteen mono-solvents at temperatures from 278.15 to 323.15 K [J]. Chinese Journal of Chemical Engineering, 2023, 58(6): 224-233.
[11]	Pengbao Lian, Lizhen Chen, Dan He, Guangyuan Zhang, Zishuai Xu, Jianlong Wang. Crystallization thermodynamics of 2,4(5)-dinitroimidazole in binary solvents [J]. Chinese Journal of Chemical Engineering, 2023, 57(5): 173-182.
[12]	Yueting Shi, Junhai Zhao, Lingli Chen, Hongru Li, Shengtao Zhang, Fang Gao. Double open mouse-like terpyridine parts based amphiphilic ionic molecules displaying strengthened chemical adsorption for anticorrosion of copper in sulfuric acid solution [J]. Chinese Journal of Chemical Engineering, 2023, 57(5): 233-246.
[13]	Chao Yang, Zhelin Su, Yeshuang Wang, Huiling Fan, Meisheng Liang, Zhaohui Chen. Insight into the effect of gel drying temperature on the structure and desulfurization performance of ZnO/SiO₂ adsorbents [J]. Chinese Journal of Chemical Engineering, 2023, 56(4): 233-241.
[14]	Ming Chen, Huiyan Jiao, Jun Li, Zhibin Wang, Feng He, Yang Jin. Liquid–liquid two-phase flow in a wire-embedded concentric microchannel: Flow pattern and mass transfer performance [J]. Chinese Journal of Chemical Engineering, 2023, 56(4): 281-289.
[15]	Wen Tian, Junyi Ji, Hongjiao Li, Changjun Liu, Lei Song, Kui Ma, Siyang Tang, Shan Zhong, Hairong Yue, Bin Liang. Measurements of the effective mass transfer areas for the gas–liquid rotating packed bed [J]. Chinese Journal of Chemical Engineering, 2023, 55(3): 13-19.