In situ preparation of well-dispersed CuO nanocatalysts in heavy oil for catalytic aquathermolysis
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摘要
We developed an in situ synthesis strategy for preparing well-dispersed CuO nanoparticles as aquathermolysis catalyst for viscosity reduction in Shengli heavy oil(China). A Cu(OH)_2-contained microemulsion was employed as a carrier to disperse the precursor Cu(OH)_2 to the heavy oil phase. Under aquathermolysis condition(240 ℃, 2.5 MPa of N_2), the Cu(OH)_2 precursors would first be converted in situ to well-crystallized and size-homogeneous CuO nanoparticles naturally, catalyzed by which the viscosity of Shengli heavy oil could be reduced as much as 94.6%; simultaneously, 22.4% of asphaltenes were converted to light components. The agglomeration of the in situ prepared monoclinic CuO nanoparticles could be negligible throughout the catalytic reaction. Based on the characterization results of ~1 H NMR, elemental analysis and GC-MS of oil samples before and after catalytic aquathermolysis, the mechanism for viscosity reduction of heavy oil in the catalytic system was investigated.
We developed an in situ synthesis strategy for preparing well-dispersed CuO nanoparticles as aquathermolysis catalyst for viscosity reduction in Shengli heavy oil(China). A Cu(OH)_2-contained microemulsion was employed as a carrier to disperse the precursor Cu(OH)_2 to the heavy oil phase. Under aquathermolysis condition(240 ℃, 2.5 MPa of N_2), the Cu(OH)_2 precursors would first be converted in situ to well-crystallized and size-homogeneous CuO nanoparticles naturally, catalyzed by which the viscosity of Shengli heavy oil could be reduced as much as 94.6%; simultaneously, 22.4% of asphaltenes were converted to light components. The agglomeration of the in situ prepared monoclinic CuO nanoparticles could be negligible throughout the catalytic reaction. Based on the characterization results of ~1 H NMR, elemental analysis and GC-MS of oil samples before and after catalytic aquathermolysis, the mechanism for viscosity reduction of heavy oil in the catalytic system was investigated.
We developed an in situ synthesis strategy for preparing well-dispersed CuO nanoparticles as aquathermolysis catalyst for viscosity reduction in Shengli heavy oil(China). A Cu(OH)_2-contained microemulsion was employed as a carrier to disperse the precursor Cu(OH)_2 to the heavy oil phase. Under aquathermolysis condition(240 ℃, 2.5 MPa of N_2), the Cu(OH)_2 precursors would first be converted in situ to well-crystallized and size-homogeneous CuO nanoparticles naturally, catalyzed by which the viscosity of Shengli heavy oil could be reduced as much as 94.6%; simultaneously, 22.4% of asphaltenes were converted to light components. The agglomeration of the in situ prepared monoclinic CuO nanoparticles could be negligible throughout the catalytic reaction. Based on the characterization results of ~1 H NMR, elemental analysis and GC-MS of oil samples before and after catalytic aquathermolysis, the mechanism for viscosity reduction of heavy oil in the catalytic system was investigated.
引文
Abdullah M. Fe304/zeolite nanocomposites synthesized by microwave assisted coprecipitation and its performance in reducing viscosity of heavy oil. In:AIP conference proceedings. 2014. https://doi.org/10.1063/1.4866746.
Bano S, Ahmad SW, Woo SI, et al. Heavy oil hydroprocessing:effect of nanostructured morphologies of MoS2 as catalyst. React Kinet Mech Cat. 2015;114(2):473-87. https://doi.org/10.1007/s11144-014-0822-z.
Cao YB, Zhang LL, Xia DH. Catalytic aquathermolysis of Shengli heavy crude oil with an amphiphilic cobalt catalyst. Pet. Sci.2016;13(3):463-75. https://doi.org/10.1007/s12182-016-0103-8.
Chao K, Chen YL, Li J, et al. Upgrading and visbreaking of super-heavy oil by catalytic aquathermolysis with aromatic sulfonic copper. Fuel Process Technol. 2012;104:174-80. https://doi.org/10.1016/j.fupro c.2012.05.010.
Chen Y, Wang Y, Lu J, et al. The viscosity reduction of nano-kegginK3PMo12O40 in catalytic aquathermolysis of heavy oil. Fuel.2009;88(8):1426-34. https://doi.org/10.1016/j.fuel.2009.03.011.
Clark PD, Hyne JB. Steam-oil chemical reactions:mechanisms for the aquathermolysis of heavy oil. AOSTRA J Res. 1984;1(1):15-20.
Galukhin AV, Erokhin AA, Osin YN, et al. Catalytic aquathermolysis of heavy oil with iron tris(acetylacetonate):changes of heavy oil composition and in situ formation of magnetic nanoparticles. Energy Fuels. 2015;29(8):4768-73. https://doi.org/10.1021/acs.energyfuel s.5b00587.
Greff J, Babadagli T. Catalytic effects of nano-size metal ions in breaking asphaltene molecules during thermal recovery of heavy-oil. In:SPE annual technical conference and exhibition. Society of Petroleum Engineers; 2011. https://doi.org/10.2118/146604-MS.
Guo K, Li HL, Yu ZX. In situ heavy and extra-heavy oil recovery:a review.Fuel.2016;185:886-902.https://doi.org/10.1016/j.fuel.2016.08.047.
Hashemi R, Nassar NN, Pereira Almao P. In situ upgrading of Athabasca bitumen using multimetallic ultradispersed nanocatalysts in an oil sands packed-bed column:part 1. Produced liquid quality enhancement. Energy Fuels. 2013;28(2):1338-50. https://doi.org/10.1021/ef401716h.
Hashemi R, Nassar NN, Pereira Almao P. In situ upgrading of Athabasca bitumen using multimetallic ultradispersed nanocatalysts in an oil sands packed-bed column:part 2. Solid analysis and gaseous product distribution. Energy Fuels. 2014;28(2):1351-61. https://doi.org/10.1021/ef401719n.
Hou JJ, Li C, Gao H, et al. Recyclable oleic acid modified magnetic NiFe204 nanoparticles for catalytic aquathermolysis of Liaohe heavy oil. Fuel. 2017;200:193-8. https://doi.org/10.1016/j.fuel.2017.03.005.
Jiang DH, Xue JB, Wu LQ, et al. Photocatalytic performance enhancement of CuO/Cu2O heterostructures for photodegradation of organic dyes:effects of CuO morphology. Appl Catal B Environ.2017;211:199-204. https://doi.org/10.1016/j.apcatb.2017.04.034.
Kapadia PR, Kallos MS, Gates ID. A review of pyrolysis, aquathermolysis, and oxidation of Athabasca bitumen. Fuel Process Technol.2015;131:270-89. https://doi.org/10.1016/j.fuproc.2014.11.027.
Li J, Chen YL, Liu HC, et al. Influences on the aquathermolysis of heavy oil catalyzed by two different catalytic ions:Cu2+and Fe3+. Energy Fuels. 2013;27(5):2555-62. https://doi.org/10.1021/ef400328s.
Li GR, Chen Y, An Y, et al. Catalytic aquathermolysis of super-heavy oil:cleavage of C-S bonds and separation of light organosulfurs.Fuel Process Technol. 2016;153:94-100. https://doi.org/10.1016/j.fuproc.2016.06.007.
Lu CH, Qi LM, Yang JH, et al. Simple template-free solution route for the controlled synthesis of Cu(OH)2 and CuO nanostructures. J Phys Chem B. 2004; 108(46):17825-31. https://doi.org/10.1021/jp046772p.
Mohammad AA, Mamora DD. In situ upgrading of heavy oil under steam injection with tetralin and catalyst. In:International thermal operations and heavy oil symposium. Society of Petroleum Engineers;2008. https://doi.org/10.2118/117604-ms.
Muraza O, Galadima A. Aquathermolysis of heavy oil:a review and perspective on catalyst development. Fuel. 2015; 157:219-31. https://doi.org/10.1016/j.fuel.2015.04.065.
Nair S, Tatarchuk BJ. Supported silver adsorbents for selective removal of sulfur species from hydrocarbon fuels. Fuel. 2010;89(11):3218-25.https://doi.org/10.1016/j.fuel.2010.05.006.
Nezamzadeh-Ejhieh A, Amiri M. CuO supported Clinoptilolite towards solar photocatalytic degradation of p-aminophenol. Powder Technol.2013;235:279-88. https://doi.org/10.1016/j.powtec.2012.10.017.
Noorlaily P,Nugraha MI, Abdullah M,et al. Ethylene glycol route synthesis of nickel oxide nanoparticles as a catalyst in aquathermolysis.In:Materials science forum. Trans Tech Publication; 2013. https://doi.org/10.4028/www.scientific.net/msf.737.93.
Ovalles C, Rivero V, Salazar A. Downhole upgrading of orinoco basin extra-heavy crude oil using hydrogen donors under steam injection conditions. Effect of the presence of iron nanocatalysts. Catalysts.2015;5(1):286-97. https://doi.org/10.3390/cata15010286.
Qin WL, Xiao ZL. The researches on upgrading of heavy crude oil by catalytic aquathermolysis treatment using a new oil-soluble catalyst.In:Advanced materials research. Trans Tech Publications; 2013.https://doi.org/10.4028/www.scientific.net/AMR.608-609.1428.
Ren RL,Liu HC,Chen Y,et al. Improving the aquathermolysis efficiency of aromatics in extra-heavy oil by introducing hydrogen-donating ligands to catalysts. Energy Fuels. 2015;29(12):7793-9. https://doi.org/10.1021/acs.energyfuels.5b01256.
Santra S, Tapec R, Theodoropoulou N, et al. Synthesis and characterization of silica-coated iron oxide nanoparticles in microemulsion:the effect of nonionic surfactants. Langmuir. 2001;17(10):2900-6. https://doi.org/10.1021/la0008636.
Shokrlu YH, Babadagli T. Viscosity reduction of heavy oil/bitumen using micro-and nano-metal particles during aqueous and non-aqueous thermal applications. J. Pet. Sci. Eng. 2014;119:210-20. https://doi.org/10.1016/j.petrol.2014.05.012.
Shuwa S, Al-Hajri R, Jibril B, et al. Novel deep eutectic solvent-dissolved molybdenum oxide catalyst for the upgrading of heavy crude oil.Ind Eng Chem Res. 2015;54(14):3589-601. https://doi.org/10.1021/ie5050082.
Suzuki T, Itoh M, Takegami Y, et al. Chemical structure of tar-sand bitumens by 13C and 1H NMR spectroscopic methods. Fuel.1982;61(5):402-10. https://doi.org/10.1016/0016-2361(82)90062-X.
Wang H, Wu Y, He L, et al. Supporting tungsten oxide on zirconia by hydrothermal and impregnation methods and its use as a catalyst to reduce the viscosity of heavy crude oil. Energy Fuels.2012;26(11):6518-27. https://doi.org/10.1021/ef301064b.
Wang JQ, Liu L, Zhang LL, et al. Aquathermolysis of heavy crude oil with amphiphilic nickel and iron catalysts. Energy Fuels.2014;28(12):7440-7. https://doi.org/10.1021/ef502134p.
Wu Y,Li YF,Chen G,et al. Urea enhanced aquathermolysis of heavy oil catalyzed by hydroxamic acid-co(Ⅱ)complex at low temperature.In:MATEC web of conferences. EDP Sciences; 2016a. https://doi.org/10.1051/matecconf/20166706038.
Wu J, Yang SY, Liu QZ, et al. Cu nanoparticles inlaid mesoporous carbon aerogels as a high performance desulfurizer. Environ Sci Technol.2016b;50(10):5370-8. https://doi.org/10.1021/acs.est.5b03740.
Yang ZC, Liu XL, Li XH, et al. Preparation of silica supported nanoscale zero valence iron and its feasibility in viscosityreduction of heavy oil. Micro Nano Lett. 2014;9(5):355-8. https://doi.org/10.1049/mnl.2014.0083.
Yusuf A,Al-Hajri RS,Al-Waheibi YM,et al. In situ upgrading of Omani heavy oil with catalyst and hydrogen donor. J Anal Appl Pyrol. 2016;121:102-12. https://doi.org/10.1016/j.jaap.2016.07.010.
Bano S, Ahmad SW, Woo SI, et al. Heavy oil hydroprocessing:effect of nanostructured morphologies of MoS2 as catalyst. React Kinet Mech Cat. 2015;114(2):473-87. https://doi.org/10.1007/s11144-014-0822-z.
Cao YB, Zhang LL, Xia DH. Catalytic aquathermolysis of Shengli heavy crude oil with an amphiphilic cobalt catalyst. Pet. Sci.2016;13(3):463-75. https://doi.org/10.1007/s12182-016-0103-8.
Chao K, Chen YL, Li J, et al. Upgrading and visbreaking of super-heavy oil by catalytic aquathermolysis with aromatic sulfonic copper. Fuel Process Technol. 2012;104:174-80. https://doi.org/10.1016/j.fupro c.2012.05.010.
Chen Y, Wang Y, Lu J, et al. The viscosity reduction of nano-kegginK3PMo12O40 in catalytic aquathermolysis of heavy oil. Fuel.2009;88(8):1426-34. https://doi.org/10.1016/j.fuel.2009.03.011.
Clark PD, Hyne JB. Steam-oil chemical reactions:mechanisms for the aquathermolysis of heavy oil. AOSTRA J Res. 1984;1(1):15-20.
Galukhin AV, Erokhin AA, Osin YN, et al. Catalytic aquathermolysis of heavy oil with iron tris(acetylacetonate):changes of heavy oil composition and in situ formation of magnetic nanoparticles. Energy Fuels. 2015;29(8):4768-73. https://doi.org/10.1021/acs.energyfuel s.5b00587.
Greff J, Babadagli T. Catalytic effects of nano-size metal ions in breaking asphaltene molecules during thermal recovery of heavy-oil. In:SPE annual technical conference and exhibition. Society of Petroleum Engineers; 2011. https://doi.org/10.2118/146604-MS.
Guo K, Li HL, Yu ZX. In situ heavy and extra-heavy oil recovery:a review.Fuel.2016;185:886-902.https://doi.org/10.1016/j.fuel.2016.08.047.
Hashemi R, Nassar NN, Pereira Almao P. In situ upgrading of Athabasca bitumen using multimetallic ultradispersed nanocatalysts in an oil sands packed-bed column:part 1. Produced liquid quality enhancement. Energy Fuels. 2013;28(2):1338-50. https://doi.org/10.1021/ef401716h.
Hashemi R, Nassar NN, Pereira Almao P. In situ upgrading of Athabasca bitumen using multimetallic ultradispersed nanocatalysts in an oil sands packed-bed column:part 2. Solid analysis and gaseous product distribution. Energy Fuels. 2014;28(2):1351-61. https://doi.org/10.1021/ef401719n.
Hou JJ, Li C, Gao H, et al. Recyclable oleic acid modified magnetic NiFe204 nanoparticles for catalytic aquathermolysis of Liaohe heavy oil. Fuel. 2017;200:193-8. https://doi.org/10.1016/j.fuel.2017.03.005.
Jiang DH, Xue JB, Wu LQ, et al. Photocatalytic performance enhancement of CuO/Cu2O heterostructures for photodegradation of organic dyes:effects of CuO morphology. Appl Catal B Environ.2017;211:199-204. https://doi.org/10.1016/j.apcatb.2017.04.034.
Kapadia PR, Kallos MS, Gates ID. A review of pyrolysis, aquathermolysis, and oxidation of Athabasca bitumen. Fuel Process Technol.2015;131:270-89. https://doi.org/10.1016/j.fuproc.2014.11.027.
Li J, Chen YL, Liu HC, et al. Influences on the aquathermolysis of heavy oil catalyzed by two different catalytic ions:Cu2+and Fe3+. Energy Fuels. 2013;27(5):2555-62. https://doi.org/10.1021/ef400328s.
Li GR, Chen Y, An Y, et al. Catalytic aquathermolysis of super-heavy oil:cleavage of C-S bonds and separation of light organosulfurs.Fuel Process Technol. 2016;153:94-100. https://doi.org/10.1016/j.fuproc.2016.06.007.
Lu CH, Qi LM, Yang JH, et al. Simple template-free solution route for the controlled synthesis of Cu(OH)2 and CuO nanostructures. J Phys Chem B. 2004; 108(46):17825-31. https://doi.org/10.1021/jp046772p.
Mohammad AA, Mamora DD. In situ upgrading of heavy oil under steam injection with tetralin and catalyst. In:International thermal operations and heavy oil symposium. Society of Petroleum Engineers;2008. https://doi.org/10.2118/117604-ms.
Muraza O, Galadima A. Aquathermolysis of heavy oil:a review and perspective on catalyst development. Fuel. 2015; 157:219-31. https://doi.org/10.1016/j.fuel.2015.04.065.
Nair S, Tatarchuk BJ. Supported silver adsorbents for selective removal of sulfur species from hydrocarbon fuels. Fuel. 2010;89(11):3218-25.https://doi.org/10.1016/j.fuel.2010.05.006.
Nezamzadeh-Ejhieh A, Amiri M. CuO supported Clinoptilolite towards solar photocatalytic degradation of p-aminophenol. Powder Technol.2013;235:279-88. https://doi.org/10.1016/j.powtec.2012.10.017.
Noorlaily P,Nugraha MI, Abdullah M,et al. Ethylene glycol route synthesis of nickel oxide nanoparticles as a catalyst in aquathermolysis.In:Materials science forum. Trans Tech Publication; 2013. https://doi.org/10.4028/www.scientific.net/msf.737.93.
Ovalles C, Rivero V, Salazar A. Downhole upgrading of orinoco basin extra-heavy crude oil using hydrogen donors under steam injection conditions. Effect of the presence of iron nanocatalysts. Catalysts.2015;5(1):286-97. https://doi.org/10.3390/cata15010286.
Qin WL, Xiao ZL. The researches on upgrading of heavy crude oil by catalytic aquathermolysis treatment using a new oil-soluble catalyst.In:Advanced materials research. Trans Tech Publications; 2013.https://doi.org/10.4028/www.scientific.net/AMR.608-609.1428.
Ren RL,Liu HC,Chen Y,et al. Improving the aquathermolysis efficiency of aromatics in extra-heavy oil by introducing hydrogen-donating ligands to catalysts. Energy Fuels. 2015;29(12):7793-9. https://doi.org/10.1021/acs.energyfuels.5b01256.
Santra S, Tapec R, Theodoropoulou N, et al. Synthesis and characterization of silica-coated iron oxide nanoparticles in microemulsion:the effect of nonionic surfactants. Langmuir. 2001;17(10):2900-6. https://doi.org/10.1021/la0008636.
Shokrlu YH, Babadagli T. Viscosity reduction of heavy oil/bitumen using micro-and nano-metal particles during aqueous and non-aqueous thermal applications. J. Pet. Sci. Eng. 2014;119:210-20. https://doi.org/10.1016/j.petrol.2014.05.012.
Shuwa S, Al-Hajri R, Jibril B, et al. Novel deep eutectic solvent-dissolved molybdenum oxide catalyst for the upgrading of heavy crude oil.Ind Eng Chem Res. 2015;54(14):3589-601. https://doi.org/10.1021/ie5050082.
Suzuki T, Itoh M, Takegami Y, et al. Chemical structure of tar-sand bitumens by 13C and 1H NMR spectroscopic methods. Fuel.1982;61(5):402-10. https://doi.org/10.1016/0016-2361(82)90062-X.
Wang H, Wu Y, He L, et al. Supporting tungsten oxide on zirconia by hydrothermal and impregnation methods and its use as a catalyst to reduce the viscosity of heavy crude oil. Energy Fuels.2012;26(11):6518-27. https://doi.org/10.1021/ef301064b.
Wang JQ, Liu L, Zhang LL, et al. Aquathermolysis of heavy crude oil with amphiphilic nickel and iron catalysts. Energy Fuels.2014;28(12):7440-7. https://doi.org/10.1021/ef502134p.
Wu Y,Li YF,Chen G,et al. Urea enhanced aquathermolysis of heavy oil catalyzed by hydroxamic acid-co(Ⅱ)complex at low temperature.In:MATEC web of conferences. EDP Sciences; 2016a. https://doi.org/10.1051/matecconf/20166706038.
Wu J, Yang SY, Liu QZ, et al. Cu nanoparticles inlaid mesoporous carbon aerogels as a high performance desulfurizer. Environ Sci Technol.2016b;50(10):5370-8. https://doi.org/10.1021/acs.est.5b03740.
Yang ZC, Liu XL, Li XH, et al. Preparation of silica supported nanoscale zero valence iron and its feasibility in viscosityreduction of heavy oil. Micro Nano Lett. 2014;9(5):355-8. https://doi.org/10.1049/mnl.2014.0083.
Yusuf A,Al-Hajri RS,Al-Waheibi YM,et al. In situ upgrading of Omani heavy oil with catalyst and hydrogen donor. J Anal Appl Pyrol. 2016;121:102-12. https://doi.org/10.1016/j.jaap.2016.07.010.