DuPont's n-butane oxidation process uses a proprietary attrition-resistant vanadyl pyrophosphate (VPP) catalyst and circulating fluidized bed (CFB) technology for the selective oxidation of n-butane to maleic anhydride. In the redox mode, n-butane feed plus recycle gas are fed to the riser side of the CFB, and air is fed to the regenerator. To optimize both activity and selectivity, oxygen may be fed to the riser side together with n-butane. These conditions fall within the n-butane flammability envelope, and localized combustion reactions were experienced during operation of a pilot plant utilizing this reactor technology. Complementary experimental and theoretical investigations were conducted using a laboratory fluidized bed reactor and an elementary step kinetic model to study the local reaction behavior near an oxygen sparger placed in a fluidized bed of solid VPP catalyst and to evaluate the effect of operating conditions on the onset of combustion in the homogeneous gas phase regions of the reactor. The laboratory fluidized bed reactor was operated at temperatures of 320-390 degrees C, pressures of 3-4 bar, freeboard residence times of 4-8 s, and n-butane and oxygen compositions of 4-10 and 1-6%, respectively. For the low solids regions of the reactor, both experimental and modeling results demonstrated pronounced pressure and temperature effects on the onset of combustion in this range of operating conditions and that decreasing the residence time delays the onset of complete combustion to longer time or higher relative molecular oxygen compositions. Kinetic model predictions also showed a significant influence of reactant composition and reactor pressure on oxidation induction time. (C) 2010 Elsevier B.V. All rights reserved,
机构:
Alma Mater Studiorum Univ Bologna, Dipartimento Chim Ind & Mat, I-40136 Bologna, Italy
INSTM, Res Unit Bologna, Bologna, ItalyAlma Mater Studiorum Univ Bologna, Dipartimento Chim Ind & Mat, I-40136 Bologna, Italy
Luciani, Silvia
Cavani, Fabrizio
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Alma Mater Studiorum Univ Bologna, Dipartimento Chim Ind & Mat, I-40136 Bologna, Italy
INSTM, Res Unit Bologna, Bologna, ItalyAlma Mater Studiorum Univ Bologna, Dipartimento Chim Ind & Mat, I-40136 Bologna, Italy
Cavani, Fabrizio
Dal Santo, Vladimiro
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CNR, Ist Sci & Tecnol Mol, I-20133 Milan, ItalyAlma Mater Studiorum Univ Bologna, Dipartimento Chim Ind & Mat, I-40136 Bologna, Italy
Dal Santo, Vladimiro
Dimitratos, Nikolaos
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Univ Milan, Dipartimento Chim Inorgan Metallorgan & Analit L, I-20133 Milan, ItalyAlma Mater Studiorum Univ Bologna, Dipartimento Chim Ind & Mat, I-40136 Bologna, Italy
Dimitratos, Nikolaos
Rossi, Michele
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Univ Milan, Dipartimento Chim Inorgan Metallorgan & Analit L, I-20133 Milan, ItalyAlma Mater Studiorum Univ Bologna, Dipartimento Chim Ind & Mat, I-40136 Bologna, Italy
机构:
China Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R ChinaChina Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China
Xu, Jiale
Li, Ning
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China Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R ChinaChina Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China
Li, Ning
Li, Xiuyi
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China Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R ChinaChina Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China
Li, Xiuyi
Ji, Renjie
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China Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R ChinaChina Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China
Ji, Renjie
Yan, Xiaoyu
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China Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R ChinaChina Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China
Yan, Xiaoyu
Huang, Rui
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China Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R ChinaChina Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China
Huang, Rui
Li, Chunyi
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China Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R ChinaChina Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China
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Univ Calif Berkeley, Dept Chem & Phys, Berkeley, CA 94720 USA
Univ Cent Florida, Dept Chem, Orlando, FL 32816 USAUniv Calif Berkeley, Dept Chem & Phys, Berkeley, CA 94720 USA
Popolan-Vaida, Denisia M.
Eskola, Arkke J.
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Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA
Univ Helsinki, Dept Chem, Helsinki 00014, FinlandUniv Calif Berkeley, Dept Chem & Phys, Berkeley, CA 94720 USA
Eskola, Arkke J.
Rotavera, Brandon
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Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA
Univ Georgia, Dept Chem, Athens, GA 30602 USA
Univ Georgia, Coll Engn, Athens, GA 30602 USAUniv Calif Berkeley, Dept Chem & Phys, Berkeley, CA 94720 USA
Rotavera, Brandon
Lockyear, Jessica F.
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Univ Calif Berkeley, Dept Chem & Phys, Berkeley, CA 94720 USAUniv Calif Berkeley, Dept Chem & Phys, Berkeley, CA 94720 USA
Lockyear, Jessica F.
Wang, Zhandong
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King Abdullah Univ Sci & Technol KAUST, Clean Combust Res Ctr CCRC, Thuwal 239556900, Saudi Arabia
Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R ChinaUniv Calif Berkeley, Dept Chem & Phys, Berkeley, CA 94720 USA
Wang, Zhandong
Sarathy, S. Mani
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King Abdullah Univ Sci & Technol KAUST, Clean Combust Res Ctr CCRC, Thuwal 239556900, Saudi ArabiaUniv Calif Berkeley, Dept Chem & Phys, Berkeley, CA 94720 USA
Sarathy, S. Mani
Caravan, Rebecca L.
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Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA
Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USAUniv Calif Berkeley, Dept Chem & Phys, Berkeley, CA 94720 USA
Caravan, Rebecca L.
Zador, Judit
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Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USAUniv Calif Berkeley, Dept Chem & Phys, Berkeley, CA 94720 USA
Zador, Judit
Sheps, Leonid
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Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USAUniv Calif Berkeley, Dept Chem & Phys, Berkeley, CA 94720 USA
Sheps, Leonid
Lucassen, Arnas
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Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA
Phys Tech Bundesanstalt, D-38116 Braunschweig, GermanyUniv Calif Berkeley, Dept Chem & Phys, Berkeley, CA 94720 USA
Lucassen, Arnas
Moshammer, Kai
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Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA
Phys Tech Bundesanstalt, D-38116 Braunschweig, GermanyUniv Calif Berkeley, Dept Chem & Phys, Berkeley, CA 94720 USA
机构:
Lulea Univ Technol, Div Chem Engn, SE-97187 Lulea, Sweden
Monash Univ, Dept Chem Engn, Clayton, Vic 3800, AustraliaLulea Univ Technol, Div Chem Engn, SE-97187 Lulea, Sweden
Rownaghi, Ali Asghar
Taufiq-Yap, Yun Hin
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Univ Putra Malaysia, Fac Sci, Ctr Excellence Catalysis Sci & Technol, Serdang 43400, Selangor, MalaysiaLulea Univ Technol, Div Chem Engn, SE-97187 Lulea, Sweden
Taufiq-Yap, Yun Hin
Rezaei, Fateme
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Lulea Univ Technol, Div Chem Engn, SE-97187 Lulea, SwedenLulea Univ Technol, Div Chem Engn, SE-97187 Lulea, Sweden
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Xi An Jiao Tong Univ, State Key Lab Multiphase Flows Power Engn, Xian 710049, Peoples R ChinaXi An Jiao Tong Univ, State Key Lab Multiphase Flows Power Engn, Xian 710049, Peoples R China
Pan, Lun
Hu, Erjiang
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Xi An Jiao Tong Univ, State Key Lab Multiphase Flows Power Engn, Xian 710049, Peoples R ChinaXi An Jiao Tong Univ, State Key Lab Multiphase Flows Power Engn, Xian 710049, Peoples R China
Hu, Erjiang
Zhang, Jiaxiang
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Xi An Jiao Tong Univ, State Key Lab Multiphase Flows Power Engn, Xian 710049, Peoples R ChinaXi An Jiao Tong Univ, State Key Lab Multiphase Flows Power Engn, Xian 710049, Peoples R China
Zhang, Jiaxiang
Tian, Zemin
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Xi An Jiao Tong Univ, State Key Lab Multiphase Flows Power Engn, Xian 710049, Peoples R ChinaXi An Jiao Tong Univ, State Key Lab Multiphase Flows Power Engn, Xian 710049, Peoples R China
Tian, Zemin
Li, Xiaotian
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Xi An Jiao Tong Univ, State Key Lab Multiphase Flows Power Engn, Xian 710049, Peoples R ChinaXi An Jiao Tong Univ, State Key Lab Multiphase Flows Power Engn, Xian 710049, Peoples R China
Li, Xiaotian
Huang, Zuohua
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Xi An Jiao Tong Univ, State Key Lab Multiphase Flows Power Engn, Xian 710049, Peoples R ChinaXi An Jiao Tong Univ, State Key Lab Multiphase Flows Power Engn, Xian 710049, Peoples R China