The effect of the Ce content on the oxidative dehydrogenation of propane over CrOy-CeO2/γ-Al2O3 catalysts

doi:10.1016/j.cjche.2020.04.022

中国化学工程学报 ›› 2020, Vol. 28 ›› Issue (12): 3035-3043.DOI: 10.1016/j.cjche.2020.04.022

• Catalysis, Kinetics and Reaction Engineering • 上一篇下一篇

The effect of the Ce content on the oxidative dehydrogenation of propane over CrO_y-CeO₂/γ-Al₂O₃ catalysts

Cheng Zuo¹, Man Wu¹, Qingjie Guo^1,2

1 Key Laboratory of Clean Chemical Processing of Shandong Province, College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China;
2 State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering, College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan 750021, China

收稿日期:2020-01-28 修回日期:2020-04-17 出版日期:2020-12-28 发布日期:2021-01-11
通讯作者: Qingjie Guo
基金资助:
The authors gratefully acknowledge the support from the National Key Research and Development Program (2018YFB0605401), Key Research and Development Program of the Ningxia Hui Autonomous Region (2018BCE01002), and National Natural Science Foundation of China (21868025).

The effect of the Ce content on the oxidative dehydrogenation of propane over CrO_y-CeO₂/γ-Al₂O₃ catalysts

Cheng Zuo¹, Man Wu¹, Qingjie Guo^1,2

1 Key Laboratory of Clean Chemical Processing of Shandong Province, College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China;
2 State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering, College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan 750021, China

Received:2020-01-28 Revised:2020-04-17 Online:2020-12-28 Published:2021-01-11
Contact: Qingjie Guo
Supported by:
The authors gratefully acknowledge the support from the National Key Research and Development Program (2018YFB0605401), Key Research and Development Program of the Ningxia Hui Autonomous Region (2018BCE01002), and National Natural Science Foundation of China (21868025).

摘要/Abstract

摘要： A series of CrO_y (17.5 wt%)-CeO₂ (X wt%)/γ-Al₂O₃ catalysts (X=0, 0.5, 2, 5, 8) with various Ce contents were prepared by a wetness impregnation method and were applied to the dehydrogenation of propane to propylene at 550℃ and 0.1 MPa. The prepared catalysts were characterized by BET, H₂-TPR, O₂-TPD, XPS, XRD, SEM-EDS and Raman spectroscopy. Among the prepared catalysts, the 17.5Cr-2Ce/Al catalyst with the largest amount of lattice oxygen exhibited the best catalytic performance for the dehydrogenation of propane to propylene with lattice oxygen. The decreased presence of oxygen defects and reducibility were the factors responsible for the improved dehydrogenation activity of the catalysts. The CeO₂ layer could inhibit the evolution of lattice oxygen (O^2-) to electrophilic oxygen species (O₂^-), and the oxygen defects on the catalyst surface were reduced. The inhibited lattice oxygen evolution prevented the deep oxidation of propane or propylene, the average CO_x selectivity decreased from 24.41% (17.5Cr/Al) to 5.71% (17.5Cr-2Ce/Al), and the average propylene selectivity increased from 60.15% (17.5Cr/Al) to 85.05% (17.5Cr-2Ce/Al).

关键词: Oxidation, Selectivity, Propane, Propylene, Fluidized-bed, Oxygen carrier

Abstract: A series of CrO_y (17.5 wt%)-CeO₂ (X wt%)/γ-Al₂O₃ catalysts (X=0, 0.5, 2, 5, 8) with various Ce contents were prepared by a wetness impregnation method and were applied to the dehydrogenation of propane to propylene at 550℃ and 0.1 MPa. The prepared catalysts were characterized by BET, H₂-TPR, O₂-TPD, XPS, XRD, SEM-EDS and Raman spectroscopy. Among the prepared catalysts, the 17.5Cr-2Ce/Al catalyst with the largest amount of lattice oxygen exhibited the best catalytic performance for the dehydrogenation of propane to propylene with lattice oxygen. The decreased presence of oxygen defects and reducibility were the factors responsible for the improved dehydrogenation activity of the catalysts. The CeO₂ layer could inhibit the evolution of lattice oxygen (O^2-) to electrophilic oxygen species (O₂^-), and the oxygen defects on the catalyst surface were reduced. The inhibited lattice oxygen evolution prevented the deep oxidation of propane or propylene, the average CO_x selectivity decreased from 24.41% (17.5Cr/Al) to 5.71% (17.5Cr-2Ce/Al), and the average propylene selectivity increased from 60.15% (17.5Cr/Al) to 85.05% (17.5Cr-2Ce/Al).

Key words: Oxidation, Selectivity, Propane, Propylene, Fluidized-bed, Oxygen carrier

Cheng Zuo, Man Wu, Qingjie Guo. The effect of the Ce content on the oxidative dehydrogenation of propane over CrO_y-CeO₂/γ-Al₂O₃ catalysts[J]. 中国化学工程学报, 2020, 28(12): 3035-3043.

Cheng Zuo, Man Wu, Qingjie Guo. The effect of the Ce content on the oxidative dehydrogenation of propane over CrO_y-CeO₂/γ-Al₂O₃ catalysts[J]. Chinese Journal of Chemical Engineering, 2020, 28(12): 3035-3043.

参考文献

[1] U.S. Energy Information Administration (EIA), China Analysis Report, EIA, Washington, D.C, 2019-12-10http://www.eia.gov/.pdf.
[2] N. Zeeshan, Light alkane dehydrogenation to light olefin technologies:A comprehensive review, Rev. Chem. Eng. 6(3) (2015) 1-23.
[3] P. Michorczyk, J. Ogonowski, P. Kustrowski, Chromium oxide supported on MUM-41 as a highly active and selective catalyst for dehydrogenation of propane with CO₂, Appl. Catal. A-Gen 349(2008) 62-69.
[4] H.M. Wang, Y. Chen, X. Yan, W.Z. Lang, Y.J. Guo, Cr doped mesoporous silica spheres for propane dehydrogenation in the presence of CO₂:Effect of Cr adding time in solgel process, Micropor. Mesopor. Mat 284(5) (2019) 69-77.
[5] S. Tetsuya, S. Kenichi, T. Kentaro, T. Tanaka, Role of CO₂ in dehydrogenation of propane over Cr-based catalysts, Catal. Today 185(2012) 151-156.
[6] A. Marktus, R. Fateme, J. Abbas, F. Mark, Oxidative dehydrogenation of propane to propylene with carbon dioxide, Appl. Catal. B-Environ 52(1) (2017) 429-445.
[7] S.B. Wang, Z.H. Zhu, Catalytic conversion of alkanes to olefins by carbon dioxide oxidative dehydrogenation, Energy Fuel 18(2004) 1126-1139.
[8] A. Isabelle, V. Vladimir, A. Konstantinos, R. Marie-Francoise, V.D.V. Pascal, B. Vitaliy, B.M. Guy, The role of CO₂ in the dehydrogenation of propane over WO_x-VO_x/SiO₂, J. Catal. 335(2016) 1-10.
[9] B.J. Xu, B. Zheng, W. Hua, Chromium oxide supported on MUM-41 as a highly active and selective catalyst for dehydrogenation of propane with CO₂, Stud. Surf. Sci. Catal. 170(4) (2007) 1072-1079.
[10] C. Wei, L.J. Jie, P. Sebastien, Synthesis and performance of vanadium-based catalysts for the selective oxidation of light alkanes, Catal. Today 5(6) (2017) 145-157.
[11] S.H. Zhang, H.C. Liu, Oxidative dehydrogenation of propane over Mg-V-O oxides supported on MgO-coated silica:Structural evolution and catalytic consequence, Appl. Catal. A-Gen 573(11) (2019) 41-48.
[12] A. Sameer, I.L. Hugo, Propylene production via propane oxidative dehydrogenation over VO_x/γ-Al₂CO₃ catalyst, Fuel 128(14) (2014) 120-140.
[13] P. Michorczyk, P. Kustrowski, L. Chmielarz, Influence of redox properties on the activity of iron oxide catalysts in dehydrogenation of propane with CO₂, React. Kinet. Catal. L 82(5) (2004) 121-130.
[14] B.J. XU, B. Zheng, W. Hua, Support effect in dehydrogenation of propane in the presence of CO₂ over supported gallium oxide catalysts, J. Catal. 239(7) (2006) 470-477.
[15] M. Gheorghita, A. Rawa, Propane oxidative dehydrogenation over VO_x/SBA-15 catalysts, Catal. Today 306(2018) 260-267.
[16] F. Ma, S. Chen, Y.H. Li, H. Zhou, A.X. Xu, W.M. Lu, Nano-MgO supported CrO_x catalysts applied in propane oxidative dehydrogenation:Relationship between active chromium phases and propane reaction pathway, Appl. Surf. Sci. 313(2014) 654-659.
[17] L. Zhang, Z.Y. Wang, J. Song, Facile synthesis of SiO₂ supported GaN as an active catalyst for CO₂ enhanced dehydrogenation of propane, J. CO₂. Util 38(5) (2020) 306-313.
[18] Y.F. Gao, F. Haeri, F. He, F.X. Li, Alkali metal-promoted La_xSr_2-xFeO_4-δ redox catalysts for chemical looping oxidative dehydrogenation of ethane, ACS Catal. 8(3) (2018) 1757-1766.
[19] T.T. Miki, M. Ogawa, N. Haneda, A. Kakuta, S. Ueno, S. Tateishi, M. Matsuura, Enhanced oxygen storage capacity of cerium oxides in cerium dioxide/lanthanum sesquioxide/alumina containing precious metals, J. Phys. Chem. C 94(6) (1990) 6464-6467.
[20] P. Moriceau, B. Grzybowska, L. Gengembre, Y. Barbaux, Effect of cerium on the mobility of oxygen on manganese oxides, Appl. Catal. A-Gen 199(2000) 73-82.
[21] Q.J. Guo, J. Zhang, J.Y. Hao, Flow characteristics in an acoustic bubbling fluidized bed at high temperature, Chem. Eng. Process. 50(2011) 331-337.
[22] Y.K. Muhammad, A.G. Sameer, A.R. Shaikh, Fluidized bed oxidative dehydrogenation of ethane to ethylene over VO_x/Ce-γ-Al₂CO₃ catalysts:Reduction kinetics and catalyst activity, Mol. Catal 443(1) (2017) 78-91.
[23] M.R. Benjaram, K. Lakshmi, T. Gode, Novel nanocrystalline Ce_1-xLa_xO_2-δ (x=0.2) solid solutions:Structural characteristics and catalytic performance, J. Mol. Catal. A-Chem 319(2010) 52-57.
[24] J.M. López, A.L. Gilbank, T. García, B. Solsona, L.S. Agouram, The prevalence of surface oxygen vacancies over the mobility of bulk oxygen in nanostructured ceria for the total toluene oxidation, Appl. Catal. B-Environ, 174(5)(2015)403-412.
[25] A.B. Tatiana, V.D. Valerii, A.S. Valeriy, V.M. Grigory, Oxidative dehydrogenation of ethane with CO₂ over CrO_x catalysts supported on Al₂CO₃, ZrO₂, CeO₂ and Ce_xZr_1-xO₂, Catal. Today 33(2019) 71-80.
[26] T. Blasco, J.L. Nieto, Oxidative dehydrogenation of short chain alkanes on supported vanadium oxide catalysts, Appl. Catal. A-Gen 157(1997) 117-142.
[27] Y.F. Gao, M.N. Luke, F.X. Li, Li-promoted La_xSr_2-xFeO_4-δ core-shell redox catalysts for oxidative dehydrogenation of ethane under a cyclic redox scheme, ACS Catal. 6(2016) 7293-7302.
[28] A. Shafiefarhood, N. Galinsky, Y. Huang, Y. Chen, F.X. Li, Fe₂O₃@La_xSr_1-xFeO₃ coreshell redox catalyst for methane partial oxidation, ChemCatChem 6(9) (2014) 790-799.
[29] L.M. Neal, A. Shafiefarhood, F.X. Li, Dynamic methane partial oxidation using a Fe₂O₃@La_0.8Sr_0.2FeO_3-δ core-shell redox catalyst in the absence of gaseous oxygen, ACS Catal. 4(2014) 3560-3569.
[30] F.L. Normand, L. Hilaire, K.G. Kili, G.J. Krill, Oxidation state of cerium in cerium-based catalysts investigated by spectroscopic probes, J. Phys. Chem. C 92(1988) 2561-2568.
[31] Y. Kim, H. Schlegl, K. Kim, J.T.S. Irvine, J.H. Kim, X-ray photoelectron spectroscopy of Sm-doled layered Perovskite for intermediate temperature-operating solid oxide fuel cell, Appl. Surf. Sci. 288(11) (2014) 695-701.
[32] N.A. Merino, B.P. Barbero, P. Eloy, L.E. Cadús, La_1-xCa_xCoO₃ perovskite-type oxides:Identification of the surface oxygen species by XPS, Appl. Surf. Sci. 253(15) (2006) 1489-1493.
[33] A. Galtayries, R. Sporken, J. Riga, G. Blanchard, R. Caudano, XPS comparative study of ceria/zirconia mixed oxides:Powders and thin film characterisation, J. Electron. Spectrosc 5(9) (1998) 88-93.
[34] E.N. Ntainjua, T.E. Davies, T. Garcia, B. Solsona, S.H. Taylor, Influence of preparation conditions of nano-crystalline ceria catalysts on the total oxidation of naphthalene, a model polycyclic aromatic hydrocarbon, Catal. Lett. 141(3) (2011) 1732-1738.
[35] V. Balcaen, R. Roelant, H. Poelman, D. Poelman, G.B. Marin, Tap study on the active oxygen species in the total oxidation of propane over a CuO-CeO₂/γ-Al₂CO₃catalyst, Catal. Today 157(1) (2010) 49-54.
[36] A. Aranda, S. Agouram, J.M. López, A.M. Mastral, D.R. Sellick, B. Solsona, S.H. Taylor, T. García, Oxygen defects:The key parameter controlling the activity and selectivity of mesoporous copper-doped ceria for the total oxidation of naphthalene, Appl. Catal. B-Environ 127(2) (2012) 77-88.
[37] M.S. Parag, N.D. Andrew, E.D. Thomas, J.M. David, H.T. Stuart, Mechanochemical preparation of ceria-zirconia catalysts for the total oxidation of propane and naphthalene volatile organic compounds, Appl. Catal. B-Environ 253(6) (2019) 331-340.
[38] J. Haber, M. Witko, Quantum-chemical modelling of hydrocarbon oxidation on vanadium-based catalysts, Catal. Today 23(1) (1995) 1-6.
[39] J.M. Libre, Y. Barbaux, B. Grzybowska, J.P.A. Bonnelle, A surface potential study of adsorbed oxygen species on a Bi₂Mo₃O₁₂ catalyst, React. Kinet. Catal. L 20(5) (1982) 49-54.
[40] M. Che, A.J. Tench, Characterization and reactivity of molecular oxygen species on oxide surfaces, Adv. Catal. 14(6) (1982) 1-148.
[41] M. Che, A.J. Tench, Characterization and reactivity of mononuclear oxygen species on oxide surfaces, Adv. Catal. 31(1) (1982) 77-133.
[42] E.Z. Skoufa, A.A. Heracleous, On ethane ODH mechanism and nature of active sites over NiO-based catalysts via isotopic labeling and methanol sorption studies, J. Catal. 322(10) (2015) 118-129.
[43] G.A. Tribalis, S. Tsilomelekis, Molecular structure and reactivity of titania-supported transition metal oxide catalysts synthesized by equilibrium deposition filtration for the oxidative dehydrogenation of ethane, CR. Chim 19(1) (2016) 1226-1236.
[44] V. Balcaen, I. Sack, M. Olea, G.B. Marin, Transient kinetic modeling of the oxidative dehydrogenation of propane over a vanadia-based catalyst in the absence of O₂, Appl. Catal. A-Gen 15(4) (2009) 31-42.
[45] E.V. Kondratenko, A. Brückner, On the nature and reactivity of active oxygen species formed from O₂ and N₂O on VO_x/MCM-41 used for oxidative dehydrogenation of propane, J. Catal. 19(8) (2010) 111-116.

The effect of the Ce content on the oxidative dehydrogenation of propane over CrO_y-CeO₂/γ-Al₂O₃ catalysts

The effect of the Ce content on the oxidative dehydrogenation of propane over CrO_y-CeO₂/γ-Al₂O₃ catalysts

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