Process design for gas condensate desulfurization and synthesis of nano-13X zeolite adsorbent: equilibrium and dynamic studies
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摘要
This paper summarizes the results of a study of adsorption of sulfur compounds from a high-sulfur feed on improved spherical-shaped nano-AgX zeolite. For this purpose, the nano-AgX zeolite was initially synthesized and improved with silver compounds such as silver nitrate, and then it was utilized in the adsorption process. In order to investigate the equilibrium and dynamics of the adsorption process, adsorptive desulfurization of real feed(i.e., sour gas condensate from the South Pars gas field) was carried out in batch and continuous processes under several operating conditions; a temperature-dependent Langmuir isotherm model was used to fit the equilibrium data. The value of monolayer adsorption capacity(q_m) and adsorption enthalpy(ΔH) were calculated to be 1.044 mmol/g and 16.8 kJ/mol, respectively. Furthermore, a detailed theoretical model was employed in order to model the breakthrough experiments. The results revealed that an increase in the feed flow rate and 1/T values will cause linear and exponential increase in the total mass transfer coefficient(ks). Isotherm and dynamic breakthrough models were found to be in agreement with the experimental data.
This paper summarizes the results of a study of adsorption of sulfur compounds from a high-sulfur feed on improved spherical-shaped nano-AgX zeolite. For this purpose, the nano-AgX zeolite was initially synthesized and improved with silver compounds such as silver nitrate, and then it was utilized in the adsorption process. In order to investigate the equilibrium and dynamics of the adsorption process, adsorptive desulfurization of real feed(i.e., sour gas condensate from the South Pars gas field) was carried out in batch and continuous processes under several operating conditions; a temperature-dependent Langmuir isotherm model was used to fit the equilibrium data. The value of monolayer adsorption capacity(q_m) and adsorption enthalpy(ΔH) were calculated to be 1.044 mmol/g and 16.8 kJ/mol, respectively. Furthermore, a detailed theoretical model was employed in order to model the breakthrough experiments. The results revealed that an increase in the feed flow rate and 1/T values will cause linear and exponential increase in the total mass transfer coefficient(ks). Isotherm and dynamic breakthrough models were found to be in agreement with the experimental data.
This paper summarizes the results of a study of adsorption of sulfur compounds from a high-sulfur feed on improved spherical-shaped nano-AgX zeolite. For this purpose, the nano-AgX zeolite was initially synthesized and improved with silver compounds such as silver nitrate, and then it was utilized in the adsorption process. In order to investigate the equilibrium and dynamics of the adsorption process, adsorptive desulfurization of real feed(i.e., sour gas condensate from the South Pars gas field) was carried out in batch and continuous processes under several operating conditions; a temperature-dependent Langmuir isotherm model was used to fit the equilibrium data. The value of monolayer adsorption capacity(q_m) and adsorption enthalpy(ΔH) were calculated to be 1.044 mmol/g and 16.8 kJ/mol, respectively. Furthermore, a detailed theoretical model was employed in order to model the breakthrough experiments. The results revealed that an increase in the feed flow rate and 1/T values will cause linear and exponential increase in the total mass transfer coefficient(ks). Isotherm and dynamic breakthrough models were found to be in agreement with the experimental data.
引文
Bakhtiari G,Abdouss M,Bazmi M, Royaee SJ. Optimization of sulfur adsorption over Ag-zeolite nanoadsorbent by experimental design method. Int J Environ Sci Technol. 2016a; 13:803-12.https://doi.org/10.1007/s13762-015-0910-2.
Bakhtiari Gh, Abdouss M, Bazmi M, Royaee SJ. High efficiency desulfurization of gas condensate by adsorption method on improved zeolite. AFINIDAD. 2016b;574:148-55.
Chen H, Wang Y, Yang FH, Yang RT. Desulfurization of high-sulfur jet fuel by mesoporousπ-complexation adsorbents. Chem Eng Sci. 2009;64:5240-6. https://doi.org/10.1016/j.ces.2009.08.031.
Cychosz KA, Wong-Foy AG, Matzger AJ. Liquid phase adsorption by microporous coordination polymers:removal of organosulfur compounds. J Am Chem Soc. 2008;130:6938-9. https://doi.org/10.1021/ja802121u.
Duan L,Gao X,Meng X,et al. Adsorption, co-adsorption, and reactions of sulfur compounds, aromatics,olefins over Ceexchanged Y zeolite. J Phys Chem C. 2012;116:25748-56.https://doi.org/10.1021/jp303040m.
Ghassabzadeh H, Torab-Mostaedi M, Mohaddespour A, et al. Characterizations of Co(Ⅱ)and Pb(Ⅱ)removal process from aqueous solutions using expanded perlite. Desalination. 2010;261:73-9.https://doi.org/10.1016/j.desal.2010.05.028.
Hasan Z, Jeon J, Jhung SH. Oxidative desulfurization of benzothiophene and thiophene with WOx/ZrO2 catalysts:effect of calcination temperature of catalysts. J Hazard Mater.2012;205-206:216-21. https://doi.org/10.1016/j.jhazmat.2011.12.059.
Hemandez-Maldonado AJ, Yang FH, Qi G, Yang RT. Desulfurization of transportation fuels byπ-complexation sorbents:Cu(Ⅰ)-,Ni(Ⅱ)-, and Zn(Ⅱ)-zeolites. Appl Catal B Environ.2005;56:111-26. https://doi.org/10.1016/j.apcatb.2004.06.023.
Jiang J, Ng FTT. Production of low sulfur diesel fuel via adsorption:an equilibrium and kinetic study on the adsorption ofdibenzothiophene onto NaY zeolite. Adsorption.2010;16:549-58. https://doi.org/10.1007/s10450-010-9259-5.
Khaled M. Adsorption performance of multiwall carbon nanotubes and graphene oxide for removal of thiophene and dibenzothiophene from model diesel fuel. Res Chem Intermed.2015;41:9817-33. https://doi.org/10.1007/s11164-015-1986-5.
Li C, Jiang Z, Gao J, et al. Ultra-deep desulfurization of diesel:oxidation with a recoverable catalyst assembled in emulsion.Chem Eur J. 2004;10:2277-80. https://doi.org/10.1002/chem.200305679.
Lin L, Zhang Y, Zhang H, Lu F. Adsorption and solvent desorption behavior of ion-exchanged modified Y zeolites for sulfur removal and for fuel cell applications. J Colloid Interface Sci.2011;360:753-9. https://doi.org/10.1016/j.jcis.2011.04.075.
Nazal MK, Khaled M, Atieh MA, et al. The nature and kinetics of the adsorption of dibenzothiophene in model diesel fuel on carbonaceous materials loaded with aluminum oxide particles. Arab J Chem. 2015;2015:4. https://doi.org/10.1016/j.arabjc.2015.12.003(in press).
Ogunlaja AS,Coombes MJ, Torto N,Tshentu ZR. The adsorptive extraction of oxidized sulfur-containing compounds from fuels by using molecularly imprinted chitosan materials. React Funct Polym.2014;81:61-76. https://doi.org/10.1016/j.reactfunctpo lym.2014.04.006.
Press WH, Teukolsky SA, Vetterling WT, Flannery BP. Numerical recipes in FORTRAN, The art of scientific computing. 2nd ed.Cambridge:Cambridge University Press; 1992.
Rashtchi M, Mohebali GH, Akbarnejad MM, et al. Analysis of biodesulfurization of model oil system by the bacterium, strain RIPI-22. Biochem Eng J. 2006;29:169-73. https://doi.org/10.1016/j.bej.2005.08.034.
Ruthven DM. Principles of adsorption and adsorption processes. 1st ed.New York:Wiley; 1984.
Sano Y, Choi K, Korai Y, Mochida I. Adsorptive removal of sulfur and nitrogen species from a straight run gas oil over activated carbons for its deep hydrodesulfurization. Appl Catal B Environ.2004;49:219-25. https://doi.org/10.1016/j.apcatb.2003.12.007.
Sari A, Tuzen M, Citak D, Soylak M. Adsorption characteristics of Cu(Ⅱ)and Pb(Ⅱ)onto expanded perlite from aqueous solution.J Hazard Mater. 2007;148(1-2):387-94. https://doi.org/10.1016/j.jhazmat.2007.02.052.
Sentorun-Shalaby C, Saha SK, Ma X, Song C. Mesoporous-molecular sieve-supported nickel sorbents for adsorptive desulfurization of commercial ultra-low-sulfur diesel fuel. Appl Catal B.2011;101:718-26. https://doi.org/10.1016/j.apcatb.2010.11.014.
Shen Y. Selective adsorption for removing sulfur:a potential ultradeep desulfurization approach of jet fuels. RSC Adv.2012;2:1700-11. https://doi.org/10.1039/ClRA00944C.
Shi Y, Yang X, Tian F, Jia C, Chen Y. Effects of toluene on thiophene adsorption over NaY and Ce(IV)Y zeolites. J Nat Gas Chem.2012;21:421-5. https://doi.org/10.1016/S1003-9953(11)60385-X.
Shi Y, Zhang W, Zhang H, et al. Effect of cyclohexene on thiophene adsorption over NaY and LaNaY zeolites. Fuel Process Technol.2013;110:24-32. https://doi.org/10.1016/j.fuproc.2013.01.008.
Singh AP, Singh PC, Pandey KK, Singh VN. Adsorption of1-butanethiol from kerosene oil on red mud. Can J Chem Eng.1988;66:501-4. https://doi.org/10.1002/cjce.5450660324.
Song C. An overview of new approaches to deep desulfurization for ultra-clean gasoline diesel and jet fuel. Catal Today.2003;86:211-63. https://doi.org/10.1016/S0920-5861(03)00412-7.
Song H, Jiang BL, Song HL, Jin ZS, Su XL. Preparation of AgY zeolite and study on its adsorption equilibrium and kinetics. Res Chem Intermed. 2015;41:3 837-54. https://doi.org/10.1007/s11164-013-1493-5.
Song H, Cui XH, Song HL, Gao HJ, Li F. Characteristic and adsorption desulfurization performance of Ag-Ce bimetal ionexchanged Y zeolite. Ind Eng Chem Res. 2014;53:14552-7.https://doi.org/10.1021/ie404362f.
Srivastav A, Srivastava VC. Adsorptive desulfurization by activated alumina. J Hazard Mater. 2009;170:1133-40. https://doi.org/10.1016/j. jhazmat.2009.05.088.
Subhan F, Liu BS, Zhang QL, Wang WS. Production of ultra-lowsulfur gasoline:an equilibrium and kinetic analysis on adsorption of sulfur compounds over Ni/MMS sorbents. J Hazard Mater. 2012;239-240:370-80. https://doi.org/10.1016/j.jhazmat.2012.09.012.
Sun HY, Sun LP, Li F, Zhang L. Adsorption of benzothiophene from fuels on modified NaY zeolites. Fuel Process Technol.2015;134:284-9. https://doi.org/10.1016/j.fuproc.2015.02.010.
Tang M, Zhou L, Du M, et al. A novel reactive adsorption desulfurization Ni/MnO adsorbent and its hydrodesulfurization ability compared with Ni/ZnO. Catal Commun. 2015;61:37-40.https://doi.org/10.1016/j.catcom.2014.11.005.
Tian WH, Sun LB, Song XL, et al. Adsorptive desulfurization by copper species within confined space. Langmuir.2010;26:17398-404. https://doi.org/10.1021/la101856d.
Wang H, Song L, Jiang H, et al. Effects of olefin on adsorptive desulfurization of gasoline over Ce(Ⅳ)Y zeolites. Fuel Process Technol. 2009a;90:835-8. https://doi.org/10.1016/j.fuproc.2009.03.004.
Wang J, Xu F,Xie W,et al. The enhanced adsorption of dibenzothiophene onto cerium/nickel-exchanged zeolite Y.J Hazard Mater. 2009b;163:538-43. https://doi.org/10.1016/j.jhazmat.2008.07.027.
Wang Y, Yang RT. Desulfurization of liquid fuels by adsorption on carbon-based sorbents and ultrasound-assisted sorbent regeneration. Langmuir. 2007;23:3 825-31. https://doi.org/10.1021/la063364z.
Yin Y,Xue D,Liu X,et al. Unusual ceria dispersion formed in confined space:a stable and reusable adsorbent for aromatic sulfur capture. Chem Commun. 2012;48:9495-7. https://doi.org/10.1039/C2CC35388A.
Zhang X, Tang D, Zhang M, Yang R. Synthesis of NaX zeolite:influence of crystallization time, temperature and batch molar ratio SiO2/Al2O3 on the particulate properties of zeolite crystals.Powder Technol. 2013;235:322-8. https://doi.org/10.1016/j.pow tec.2012.10.046.
Bakhtiari Gh, Abdouss M, Bazmi M, Royaee SJ. High efficiency desulfurization of gas condensate by adsorption method on improved zeolite. AFINIDAD. 2016b;574:148-55.
Chen H, Wang Y, Yang FH, Yang RT. Desulfurization of high-sulfur jet fuel by mesoporousπ-complexation adsorbents. Chem Eng Sci. 2009;64:5240-6. https://doi.org/10.1016/j.ces.2009.08.031.
Cychosz KA, Wong-Foy AG, Matzger AJ. Liquid phase adsorption by microporous coordination polymers:removal of organosulfur compounds. J Am Chem Soc. 2008;130:6938-9. https://doi.org/10.1021/ja802121u.
Duan L,Gao X,Meng X,et al. Adsorption, co-adsorption, and reactions of sulfur compounds, aromatics,olefins over Ceexchanged Y zeolite. J Phys Chem C. 2012;116:25748-56.https://doi.org/10.1021/jp303040m.
Ghassabzadeh H, Torab-Mostaedi M, Mohaddespour A, et al. Characterizations of Co(Ⅱ)and Pb(Ⅱ)removal process from aqueous solutions using expanded perlite. Desalination. 2010;261:73-9.https://doi.org/10.1016/j.desal.2010.05.028.
Hasan Z, Jeon J, Jhung SH. Oxidative desulfurization of benzothiophene and thiophene with WOx/ZrO2 catalysts:effect of calcination temperature of catalysts. J Hazard Mater.2012;205-206:216-21. https://doi.org/10.1016/j.jhazmat.2011.12.059.
Hemandez-Maldonado AJ, Yang FH, Qi G, Yang RT. Desulfurization of transportation fuels byπ-complexation sorbents:Cu(Ⅰ)-,Ni(Ⅱ)-, and Zn(Ⅱ)-zeolites. Appl Catal B Environ.2005;56:111-26. https://doi.org/10.1016/j.apcatb.2004.06.023.
Jiang J, Ng FTT. Production of low sulfur diesel fuel via adsorption:an equilibrium and kinetic study on the adsorption ofdibenzothiophene onto NaY zeolite. Adsorption.2010;16:549-58. https://doi.org/10.1007/s10450-010-9259-5.
Khaled M. Adsorption performance of multiwall carbon nanotubes and graphene oxide for removal of thiophene and dibenzothiophene from model diesel fuel. Res Chem Intermed.2015;41:9817-33. https://doi.org/10.1007/s11164-015-1986-5.
Li C, Jiang Z, Gao J, et al. Ultra-deep desulfurization of diesel:oxidation with a recoverable catalyst assembled in emulsion.Chem Eur J. 2004;10:2277-80. https://doi.org/10.1002/chem.200305679.
Lin L, Zhang Y, Zhang H, Lu F. Adsorption and solvent desorption behavior of ion-exchanged modified Y zeolites for sulfur removal and for fuel cell applications. J Colloid Interface Sci.2011;360:753-9. https://doi.org/10.1016/j.jcis.2011.04.075.
Nazal MK, Khaled M, Atieh MA, et al. The nature and kinetics of the adsorption of dibenzothiophene in model diesel fuel on carbonaceous materials loaded with aluminum oxide particles. Arab J Chem. 2015;2015:4. https://doi.org/10.1016/j.arabjc.2015.12.003(in press).
Ogunlaja AS,Coombes MJ, Torto N,Tshentu ZR. The adsorptive extraction of oxidized sulfur-containing compounds from fuels by using molecularly imprinted chitosan materials. React Funct Polym.2014;81:61-76. https://doi.org/10.1016/j.reactfunctpo lym.2014.04.006.
Press WH, Teukolsky SA, Vetterling WT, Flannery BP. Numerical recipes in FORTRAN, The art of scientific computing. 2nd ed.Cambridge:Cambridge University Press; 1992.
Rashtchi M, Mohebali GH, Akbarnejad MM, et al. Analysis of biodesulfurization of model oil system by the bacterium, strain RIPI-22. Biochem Eng J. 2006;29:169-73. https://doi.org/10.1016/j.bej.2005.08.034.
Ruthven DM. Principles of adsorption and adsorption processes. 1st ed.New York:Wiley; 1984.
Sano Y, Choi K, Korai Y, Mochida I. Adsorptive removal of sulfur and nitrogen species from a straight run gas oil over activated carbons for its deep hydrodesulfurization. Appl Catal B Environ.2004;49:219-25. https://doi.org/10.1016/j.apcatb.2003.12.007.
Sari A, Tuzen M, Citak D, Soylak M. Adsorption characteristics of Cu(Ⅱ)and Pb(Ⅱ)onto expanded perlite from aqueous solution.J Hazard Mater. 2007;148(1-2):387-94. https://doi.org/10.1016/j.jhazmat.2007.02.052.
Sentorun-Shalaby C, Saha SK, Ma X, Song C. Mesoporous-molecular sieve-supported nickel sorbents for adsorptive desulfurization of commercial ultra-low-sulfur diesel fuel. Appl Catal B.2011;101:718-26. https://doi.org/10.1016/j.apcatb.2010.11.014.
Shen Y. Selective adsorption for removing sulfur:a potential ultradeep desulfurization approach of jet fuels. RSC Adv.2012;2:1700-11. https://doi.org/10.1039/ClRA00944C.
Shi Y, Yang X, Tian F, Jia C, Chen Y. Effects of toluene on thiophene adsorption over NaY and Ce(IV)Y zeolites. J Nat Gas Chem.2012;21:421-5. https://doi.org/10.1016/S1003-9953(11)60385-X.
Shi Y, Zhang W, Zhang H, et al. Effect of cyclohexene on thiophene adsorption over NaY and LaNaY zeolites. Fuel Process Technol.2013;110:24-32. https://doi.org/10.1016/j.fuproc.2013.01.008.
Singh AP, Singh PC, Pandey KK, Singh VN. Adsorption of1-butanethiol from kerosene oil on red mud. Can J Chem Eng.1988;66:501-4. https://doi.org/10.1002/cjce.5450660324.
Song C. An overview of new approaches to deep desulfurization for ultra-clean gasoline diesel and jet fuel. Catal Today.2003;86:211-63. https://doi.org/10.1016/S0920-5861(03)00412-7.
Song H, Jiang BL, Song HL, Jin ZS, Su XL. Preparation of AgY zeolite and study on its adsorption equilibrium and kinetics. Res Chem Intermed. 2015;41:3 837-54. https://doi.org/10.1007/s11164-013-1493-5.
Song H, Cui XH, Song HL, Gao HJ, Li F. Characteristic and adsorption desulfurization performance of Ag-Ce bimetal ionexchanged Y zeolite. Ind Eng Chem Res. 2014;53:14552-7.https://doi.org/10.1021/ie404362f.
Srivastav A, Srivastava VC. Adsorptive desulfurization by activated alumina. J Hazard Mater. 2009;170:1133-40. https://doi.org/10.1016/j. jhazmat.2009.05.088.
Subhan F, Liu BS, Zhang QL, Wang WS. Production of ultra-lowsulfur gasoline:an equilibrium and kinetic analysis on adsorption of sulfur compounds over Ni/MMS sorbents. J Hazard Mater. 2012;239-240:370-80. https://doi.org/10.1016/j.jhazmat.2012.09.012.
Sun HY, Sun LP, Li F, Zhang L. Adsorption of benzothiophene from fuels on modified NaY zeolites. Fuel Process Technol.2015;134:284-9. https://doi.org/10.1016/j.fuproc.2015.02.010.
Tang M, Zhou L, Du M, et al. A novel reactive adsorption desulfurization Ni/MnO adsorbent and its hydrodesulfurization ability compared with Ni/ZnO. Catal Commun. 2015;61:37-40.https://doi.org/10.1016/j.catcom.2014.11.005.
Tian WH, Sun LB, Song XL, et al. Adsorptive desulfurization by copper species within confined space. Langmuir.2010;26:17398-404. https://doi.org/10.1021/la101856d.
Wang H, Song L, Jiang H, et al. Effects of olefin on adsorptive desulfurization of gasoline over Ce(Ⅳ)Y zeolites. Fuel Process Technol. 2009a;90:835-8. https://doi.org/10.1016/j.fuproc.2009.03.004.
Wang J, Xu F,Xie W,et al. The enhanced adsorption of dibenzothiophene onto cerium/nickel-exchanged zeolite Y.J Hazard Mater. 2009b;163:538-43. https://doi.org/10.1016/j.jhazmat.2008.07.027.
Wang Y, Yang RT. Desulfurization of liquid fuels by adsorption on carbon-based sorbents and ultrasound-assisted sorbent regeneration. Langmuir. 2007;23:3 825-31. https://doi.org/10.1021/la063364z.
Yin Y,Xue D,Liu X,et al. Unusual ceria dispersion formed in confined space:a stable and reusable adsorbent for aromatic sulfur capture. Chem Commun. 2012;48:9495-7. https://doi.org/10.1039/C2CC35388A.
Zhang X, Tang D, Zhang M, Yang R. Synthesis of NaX zeolite:influence of crystallization time, temperature and batch molar ratio SiO2/Al2O3 on the particulate properties of zeolite crystals.Powder Technol. 2013;235:322-8. https://doi.org/10.1016/j.pow tec.2012.10.046.