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28 results on '"Oxidative dehydrogenation of ethane"'

1. MnOx promoted phase-pure M1 MoVNbTe oxide for ethane oxidative dehydrogenation.

Author

Chen, Xin, Dang, Dan, An, Hang, Chu, Bozhao, and Cheng, Yi

Subjects
OXIDES, ETHANES, DEHYDROGENATION, CATALYSTS, MANGANESE
Abstract

Highlights • Improved performance of MoVNbTeO x catalyst in ODH process by inserting oxygen into catalyst lattice through manganese ions. • Revealed the phase-pure M1 catalyst properties before and after the introduction of MnO x. • Proposed an inference of oxygen diffusion process during preparation by detailed characterization and controlled trial Abstract M1 phase of MoVNbTe oxide catalyst is a promising catalyst for oxidative dehydrogenation of ethane (ODHE) process. Raising V5+ concentration in the catalyst is an effective way to improve the catalytic performance while thermal oxidation in air has limited effect on the increase of vanadium valence state. In this work, manganese is introduced into the catalyst system, acting as oxygen facilitator, making M1 oxidized by gas phase oxygen at lower temperature during the preparation process. The influence of manganese addition amount and combination method on catalyst activity is studied. BET, XPS, SEM, TEM, ICP, TPR, and TPD characterizations are performed to study the correlation between catalyst properties and catalytic performance. Corresponding to the valence state increment, the catalyst promoted by MnO x gives an improved catalytic performance, e.g. , over 20% improvement in ODHE process at 400 °C based on the ethane conversion. Graphical abstract Image, graphical abstract [ABSTRACT FROM AUTHOR]

Published
2019
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2. Alkali metal and alkaline earth metal perovskites for oxidative coupling of methane and oxidative dehydrogenation of ethane.

Author

Xu, Junwei, Ouyang, Rumeng, Zhong, Xusheng, Fang, Xiuzhong, Xu, Xianglan, and Wang, Xiang

Subjects
*ALKALINE earth metals, *ALKALI metals, *DEHYDROGENATION, *ETHANES, *PEROVSKITE, *CATALYSIS, *CATALYSTS
Abstract

• Alkali and alkaline earth perovskites have similar active sites for OCM and ODHE. • Moderate and strong basic sites assist OCM and moderate basic sites expedite ODHE. • V f affects CH 4 , C 2 H 6 , and O 2 conversions, while χ A + χ B affects basicity. • Crystal phase transition and metal-oxygen energy alter moderate basic sites. • Moderate V f , low electronegativity, and variable crystal phase augment reactivity. In this study, alkali metal and alkaline earth metal perovskites have been synthesized using simple preparation methods for catalyzing the oxidative coupling of methane (OCM) and oxidative dehydrogenation of ethane (ODHE). The influence of their structural parameters (such as tolerance factor t, unit cell free volume (V f), electronegativity of A- and B-site elements, average metal-oxygen energy, and crystalline phase transition) on basic sites and reaction performance is also systematically investigated. The results show that these two perovskites have similar active sites for OCM and ODHE reactions, with the moderate and strong basic sites favoring the OCM reaction and the moderate basic site facilitating the ODHE reaction. The surface basicity of these perovskites reflects the electron-donating ability of lattice oxygen, which in turn affects the production of reactive oxygen species (O 2 −, O 2 2−, and O−). Moderate basic sites are abundant and closely related to oxygen vacancies, with high oxygen vacancy concentrations generating abundant reactive oxygen species. Meanwhile, V f values of perovskites govern the CH 4 , C 2 H 6 , and O 2 conversions, the electronegativity of elements affects the catalyst basicity, and the average metal-oxygen energy and crystalline phase transition alter the moderate basic sites. Overall, it concludes that perovskites should meet the following conditions to achieve excellent catalytic performance for OCM and ODHE: moderate V f , low electronegativity of A- and B-site elements, low average metal oxygen energy, and a crystalline structure that changes with temperature. [Display omitted] [ABSTRACT FROM AUTHOR]

Published
2023
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3. A simple approach to describe hydrodynamics and its effect on heat and mass transport in an industrial wall-cooled fixed bed catalytic reactor: ODH of ethane on a MoVNbTeO formulation.

Author

Aparicio-Mauricio, Gustavo, Ruiz, Richard S., López-Isunza, Felipe, and Castillo-Araiza, Carlos O.

Subjects
*PACKED bed reactors, *FIXED bed reactors, *HYDRODYNAMICS, *HEAT transfer, *MASS transfer, *DEHYDROGENATION, *ETHANES
Abstract

The incorporation of hydrodynamics in an industrial wall-cooled packed bed reactor model is essential to describe the performance of highly exothermic oxidation reactions. Although the conventional hydrodynamic approach (CHA), Navier-Stokes equations coupled to Darcy-Forchheimer terms, has been the most used approximation to describe velocity profiles in these packed bed reactors, it is itself inconsistent and the computation time for its numerical solution, when coupled to the reactor model, is still demanding. This work is aimed at developing a practical but reliable hydrodynamic approach (PHA) to describe velocity profiles in packed bed reactors presenting a low tube to particle diameter ratio. In this approach, velocity profiles are described at the core and close to the wall of the reactor. The core model makes use of the Darcy-Forchheimer equation (DFE), and the wall model makes use of Navier-Stokes equations (NSE) using an effective viscosity to account for turbulence. The PHA predicts similar results to those obtained by the CHA and properly fits velocity observations from packed beds with a tube to particle diameter ratio (d t /d p ) ranging from 3 to 6. The PHA allows the estimation of both turbulent viscosity (μ t ) involved in the viscous term of the NSE and parameters influencing viscous (α) and inertial (β) flow resistances in Darcy and Forchheimer terms, respectively. Then, hydrodynamics is coupled to a heat transport model accounting for conductive anisotropy to fit temperature observations in absence of reaction from a pilot-scale packed bed reactor with a d t /d p = 3.048. Hydrodynamics and heat transfer results are, then, transferred to a pseudo heterogeneous reactor model to simulate the behavior of a novel technology to perform the oxidative dehydrogenation of ethane on a multimetallic MoVNbTeO formulation. This is the first study modeling this reactor system accounting for hydrodynamics, information that is essential for its conceptual design in future studies. Finally, it is worth stressing that the PHA, coupled to the heat transport model or the reactor model, leads to significantly lower computation times than the CHA, which is attributed to the analytical rather than numerical solution of the former. [ABSTRACT FROM AUTHOR]

Published
2017
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4. Oxidative dehydrogenation of ethane over a Mo-V-Nb-Te-O mixed-oxide catalyst in a cyclic mode.

Author

Mishanin, I., Kalenchuk, A., Maslakov, K., Lunin, V., Koklin, A., Finashina, E., and Bogdan, V.

Subjects
*MOLYBDENUM catalysts, *MIXED oxide catalysts, *DEHYDROGENATION, *ETHANES, *REACTIVITY (Chemistry), *OXYGEN
Abstract

The oxidative dehydrogenation of ethane (ODE) into ethylene over a Mo-V-Nb-Te-O mixedoxide catalyst in a cyclic mode with alternate feeding of ethane and air has been investigated. The amount of oxide-phase oxygen involved in the reaction has been estimated by titrating the oxygen of the active phase of the catalyst with ethane. The reactivity of this oxygen increases with an increasing temperature. The amount active oxygen involved in ODE at 360-400°C is 0.2-0.6 mmol/g. [ABSTRACT FROM AUTHOR]

Published
2017
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5. Flexible NiZr-based structured catalysts for ethylene production through ODH of ethane: Catalytic performance enhancement.

Author

Bortolozzi, J.P., Banús, E.D., Courtalón, N.L., Ulla, M.A., Milt, V.G., and Miró, E.E.

Subjects
*NICKEL catalysts, *CRYSTAL structure, *ETHYLENE, *ETHANES, *DEHYDROGENATION, *CRYSTAL growth
Abstract

Flexible structured catalysts based on Ni and Zr deposited on a ceramic paper made of SiO 2 -Al 2 O 3 and ZrO 2 fibers showed to be active and selective for the Oxidative Dehydrogenation of Ethane. Zirconium promoter strongly interacted with nickel oxide and produced structural changes that affected the NiO redox behavior, crystal growth and lattice order which enhanced selectivity towards ethylene. The variation of the concentration of the precursor solution used and the addition of zirconia short fibers, affected the catalytic performance. The lower the concentration of the solution used to incorporate the catalyst, the better the catalytic performance. The addition of zirconia fibers also showed beneficial effects on ethylene production. [ABSTRACT FROM AUTHOR]

Published
2016
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6. NiCe/γ-Al2O3 coated onto cordierite monoliths applied to Oxidative Dehydrogenation of Ethane (ODE).

Author

Brussino, P., Bortolozzi, J.P, Milt, V.G., Banús, E.D., and Ulla, M.A.

Subjects
*NICKEL compounds, *ALUMINUM oxide, *SURFACE coatings, *CORDIERITE, *OXIDATION, *DEHYDROGENATION, *ETHANES
Abstract

The present work investigates the preparation of NiCe/γ-Al 2 O 3 coated cordierite monoliths for oxidative dehydrogenation of ethane (ODE) reaction through a two steps procedure: the primer deposition of a γ-Al 2 O 3 coating consisting in a mixture of micro and nanoparticles via the washcoating method and the latter incorporation of the active phase by impregnation. Moreover, a modification in these two steps was made: the suppression of some calcination steps to save energy in the manufacture process. The structured catalysts, named as Ni(X)Ce(Y)-M, where X = 13 or 19 wt%. Ni and Y = 5 or 8 wt%. Ce respectively, with respect to the alumina loading, were characterized by SEM/EDX, XRD, FTIR, LRS and XPS, and their catalytic activity was tested in the ODE reaction. Furthermore, their mechanical resistance to vibration was studied. Similar results corresponding to the un-promoted system are also presented for comparison. It was found that the co-impregnation of nickel and cerium was affected by the suppression of some calcinations: a preferential absorption of Ce rather than Ni occurred, generating at the end a catalytic coating with a higher Ce/Ni ratio than that of the precursor solution and a lower Ni loading than that of Ni(13)-M. On the other side, in the NiCe-based catalysts the properties of the active sites remained the same despite the increment in the active phase, at a fixed Ce/Ni nominal atomic ratio of 0.17. In the case of the Ni(19)Ce(8)-M system, although the Ni/Al atomic ratios were found lower than those of the nominal ones by EDX and XPS and ethylene selectivity decayed, ethane conversion resulted markedly higher, leading to an improved ethylene yield. [ABSTRACT FROM AUTHOR]

Published
2016
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7. The nickel-support interaction as determining factor of the selectivity to ethylene in the oxidative dehydrogenation of ethane over nickel oxide/alumina catalysts

Author

Jose Nieto, Agustín de Arriba, Benjamín Solsona, E. García-González, Rachid Issaadi, Yousra Abdelbaki, D. Delgado, and Ministerio de Ciencia, Innovación y Universidades (España)

Subjects
Ethylene, 010405 organic chemistry, Chemistry, Process Chemistry and Technology, Nickel oxide, Inorganic chemistry, Non-blocking I/O, Oxalic acid, Alumina, chemistry.chemical_element, Catalyst characterization (XPS, HREM, UV raman and UV-vis-DRS), 010402 general chemistry, 01 natural sciences, Catalysis, ODH, 0104 chemical sciences, Crystallinity, chemistry.chemical_compound, Nickel, Dehydrogenation, Oxidative dehydrogenation of ethane
Abstract

[EN] Nickel oxides supported on gamma-alumina (Ni-loading from 5 to 30 wt% NiO) have been synthesized and tested in the oxidative dehydrogenation (ODH) of ethane in order to determine the importance of the NiO-support interaction. The best performance was achieved by the catalyst with 15 wt% NiO; higher NiO-loadings lead to the formation of unselective bulk-like NiO and lower Ni-loadings present high proportion of free alumina surface sites. The presence of oxalic acid and/or niobium in the synthesis gel resulted in the formation of NiO particles with similar size, but higher crystallinity and reducibility than the standard 15 wt% NiO catalyst. The obtained results have revealed that, in addition to NiO crystal size, the nickel oxide-support interaction determines the catalytic performance of these catalysts., Authors would like to acknowledge the Ministerio de Ciencia, Innovacion y Universidades in Spain through projects CRTl2018-099668-B-C21, MAT2017-84118-C2-1-R and PID2019-106662RB-C44 and Ministry of Higher Education and Scientific Research of Algeria for the National Exceptional Program for the fellowships. A.A. acknowl-edges Severo Ochoa Excellence Program for his fellowship (BES-2017-080329) . EGG acknowledges Dr. E. Urones for the valuable assistance in the use of electron microscopy facilities as well as to the CNME (Spain) .

Published
2021

8. Comparison of Ni and Ni–Ce/Al2O3 catalysts in granulated and structured forms: Their possible use in the oxidative dehydrogenation of ethane reaction.

Author

Bortolozzi, J.P., Weiss, T., Gutierrez, L.B., and Ulla, M.A.

Subjects
*ALUMINUM oxide, *NICKEL catalysts, *GRANULATION (Metalwork), *DEHYDROGENATION, *OXIDATION of ethanes, *CHEMICAL reactions
Abstract

Highlights: [•] Ni and Ni–Ce/Al2O3 coatings on metallic foams were active and selective for the ODE. [•] The cerium addition increased considerably the ethylene productivity. [•] Catalytic features of the structured systems depend on the calcination temperature. [•] The presence of chromium in the catalytic coatings mainly affects the selectivity. [•] The structured systems showed higher ethylene productivity than powder catalysts. [ABSTRACT FROM AUTHOR]

Published
2014
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9. Optimizing the efficiency of MoVTeNbO catalysts for ethane oxidative dehydrogenation to ethylene

Author

Nguyen, T.T., Aouine, M., and Millet, J.M.M.

Subjects
*METAL catalysts, *METALLIC oxides, *ETHANES, *DEHYDROGENATION, *OXIDATION, *ETHYLENE, *SLURRY, *HEAT treatment of metals
Abstract

Abstract: MoVTe(Sb)NbO catalysts have been prepared using the slurry method and tested as catalysts for the oxidative dehydrogenation of ethane. The influence of both the addition of silica to the starting slurry during the preparation and of a final heat treatment under nitrogen at 873K after the dissolution of the M2 phase formed concomitantly to the active M1 active phase has been studied. While the parameters change the texture of the catalysts without modification of the catalytic sites, they have opposite effects on catalytic properties. The addition of silica increases the conversion without modifying the selectivity to ethylene and the final heat treatment decreases the conversion but increases the selectivity. These effects have been explained respectively by a decrease of the agglomeration and sintering of the M1 phase crystallites and a decrease of the number of small pores, where total oxidation takes place. These effects could be leveraged to optimize the preparation protocol and obtain more efficient catalysts for the oxidative dehydrogenation of ethane. [Copyright &y& Elsevier]

Published
2012
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10. Oxidative dehydrogenation of ethane over NiO–CeO2 mixed oxides catalysts

Author

Solsona, Benjamín, Concepción, Patricia, Hernández, Selene, Demicol, Benjamin, and Nieto, José M. López

Subjects
*METAL catalysts, *DEHYDROGENATION, *OXIDATION, *ETHANES, *METALLIC oxides, *CARBON oxides
Abstract

Abstract: In this paper we present the synthesis, characterization and catalytic behaviour in the oxidative dehydrogenation of ethane of NiO–CeO2 mixed oxides. The addition of cerium oxide to NiO strongly modifies its catalytic performance, although the changes in the catalytic behaviour depend on the catalyst composition. The incorporation of low amounts of cerium oxide to NiO multiplies the productivity to ethylene in the oxidative dehydrogenation of ethane by a factor of ca. 7, which is the result of an increase in both catalytic activity and selectivity to ethylene. The enhanced activity has been related to the remarkable increase of the surface area of catalyst and the low crystal sizes of NiO that takes place when a tiny amount of cerium oxide is incorporated to the NiO. The higher selectivity to ethylene has been related to the modification of the nature of Ni–O species, which implies a lower production of carbon oxides. On the other hand, high activity and selectivity is also observed over catalysts rich in cerium (with Ni/Ce ratios between 0.2 and 3). In this case, a different mechanism can be proposed in which the high capacity of CeO2 to bomb oxygen from bulk to surface and the partial formation of NiO and Ce1−x Ni x O2 facilitates a faster reoxidation of active Ni-sites by a synergic effect improving catalytic activity. [Copyright &y& Elsevier]

Published
2012
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11. Oxidative dehydrogenation of ethane over Ni–W–O mixed metal oxide catalysts

Author

Solsona, B., López Nieto, J.M., Concepción, P., Dejoz, A., Ivars, F., and Vázquez, M.I.

Subjects
*DEHYDROGENATION, *OXIDATION, *ETHANES, *NICKEL catalysts, *EVAPORATION (Chemistry), *NICKEL nitrate, *AMMONIUM paratungstate, *X-ray diffraction, *NANOPARTICLES, *CHEMICAL decomposition, *ETHYLENE, *LEWIS acids
Abstract

Abstract: Ni–W–O mixed oxides were prepared through the evaporation of aqueous solutions of nickel nitrate and ammonium tungstate and calcined in air at 500°C for 2h. The catalysts were characterized by several techniques (N2 adsorption, X-ray diffraction, temperature-programmed reduction, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy of adsorbed CO, and 18O/16O isotope exchange) and tested in the oxidative dehydrogenation of ethane. The catalytic activity and catalyst reducibility decrease when the W content increases. Thus, nickel sites seem to be the active centers for ethane activation in these catalysts. However, the selectivity to ethylene strongly changes depending on the Ni/W ratio. In W-rich catalysts, in which NiWO4 and WO3 are mainly observed, a strong influence of ethane conversion on the selectivity to ethylene is observed. However, in Ni-rich catalysts, in which NiO crystallites and WO x nanoparticles are mainly observed, ethane conversion hardly influences the selectivity to ethylene. It has been demonstrated that the nature of the Ni sites and the characteristics and number of the acid sites determine the catalytic behavior of these catalysts. The presence of Lewis acid sites with high acid strength in W-rich catalysts facilitates the decomposition of ethylene during ethane oxidation. [Copyright &y& Elsevier]

Published
2011
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12. Oxidative dehydrogenation of ethane to ethene on alumina-supported molybdenum-based catalysts modified by vanadium and phosphorus

Author

Haddad, N., Bordes-Richard, E., Hilaire, L., and Barama, A.

Subjects
*DEHYDROGENATION, *ETHANES, *ALKENES, *X-ray photoelectron spectroscopy
Abstract

Abstract: Gamma-alumina-supported MoO x , MoVO x (Mo/V=11) and MoVPO x (Mo/V=11, V/P=1) catalysts were prepared and their properties studied by several techniques (EDX-SEM, XRD, XPS, LRS, TPR). Acid–base and catalytic properties were determined by carrying out 2-propanol decomposition and oxidative dehydrogenation of ethane to ethene, respectively. In situ X-ray diffraction and X-ray photoelectron spectroscopy after pre-treatment were carried out in redox conditions (with H2/N2, C2H6/N2 as reducing and O2/N2 as oxidant). The catalytic performance increases along MoO x

Published
2007
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13. Oxidative dehydrogenation of ethane with carbon dioxide over Cr2O3/SBA-15 catalysts: the influence of sulfate modification of the support

Author

P.S. Sai Prasad, K.S. Rama Rao, P. Thirumala Bai, S. Srinath, N. Lingaiah, K. Upendar, and T. V. Sagar

Subjects
Diffuse reflectance infrared fourier transform, Inorganic chemistry, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Catalysis, Ethylene, chemistry.chemical_compound, X-ray photoelectron spectroscopy, Chromium oxide, Desorption, Dehydrogenation, Sulfate, Fourier transform infrared spectroscopy, Oxidative dehydrogenation of ethane, Spectroscopy, lcsh:Petroleum refining. Petroleum products, General Environmental Science, Ethane, Sulfated SBA-15, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Carbon dioxide, chemistry, lcsh:TP690-692.5, General Earth and Planetary Sciences, 0210 nano-technology
Abstract

Unmodified and sulfate-modified SBA-15-supported Cr2O3 catalysts were prepared by impregnation method. The physico-chemical properties of the supports and catalysts were determined by nitrogen adsorption/desorption, powder X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), laser-Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), UV–Vis diffuse reflectance spectroscopy (UV-DRS), inductively coupled plasma optical emission spectroscopy (ICP-OES), transmission electron microscopy (TEM) and temperature-programmed reduction (TPR) techniques. Oxidative dehydrogenation of ethane to ethylene (ODE) with CO2 as oxidant was carried out on these catalysts in a fixed-bed reactor at temperatures in the range of 600–700 °C and at atmospheric pressure. The changes in structural and textural properties because of sulfate modification were identified. Sulfate modification affected the nature of interaction of CrO x species with the SBA-15 support. During the evaluation, it was observed that sulfate modification enhances ethane conversion and ethylene selectivity of the catalyst. Better dispersion of CrO x and the increase in Cr6+/Cr3+ ratio seem to be the reasons for the higher performance of the sulfate-modified catalysts compared to that of the unmodified catalyst.

Published
2017

14. Vanadium-metal(IV)phosphates as catalysts for the oxidative dehydrogenation of ethane

Author

Lisi, L., Ruoppolo, G., Casaletto, M.P., Galli, P., Massucci, M.A., Patrono, P., and Pinzari, F.

Subjects
*CHEMICAL inhibitors, *DEHYDROGENATION, *ETHANES, *VANADIUM
Abstract

Abstract: Vanadium-exchanged Ti, Zr, and Sn-pyrophosphates have been prepared as cubic phase and tested for the oxidative dehydrogenation of ethane in the temperature range 550–700°C in a fixed bed reactor. The catalysts have been characterised by XRD, XPS, BET surface area and TPR experiments. Vanadium exchange does not modify the cubic structure of the materials but thermal treatment under reducing or reaction conditions results in a significant loss of Sn-pyrophosphate structure, whereas Ti and Zr-pyrophosphates remain stable. All samples are active for the reaction and vanadium-Ti-pyrophosphate provides the best catalytic performances. The exchanged catalysts show a very good selectivity to ethylene, even at quite high ethane conversion, which has been attributed to the great vanadium site isolation. [Copyright &y& Elsevier]

Published
2005
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15. Experimental equipment for high-throughput synthesis and testing of catalytic materials

Author

Hahndorf, Ina, Buyevskaya, Olga, Langpape, Martin, Grubert, Gerd, Kolf, Stephan, Guillon, Emmanuelle, and Baerns, Manfred

Subjects
*CATALYSTS, *ROBOTS, *DEHYDROGENATION, *ETHANES
Abstract

A set-up for fast parallel preparation and testing of catalytic materials is presented. A commercial synthesis robot is used for automated parallel preparation of catalyst libraries. An adapted method for the synthesis of supported multicomponent catalytic material by sequential impregnation of an alumina support with different precursor solutions is described. It is shown that the catalytic performance of the materials prepared with the synthesis robot is comparable to manually prepared materials. In testing materials for the oxidative dehydrogenation of light alkanes to olefins a 64 multi-channel ceramic reactor module was used being connected to a fast GC/MS analysis. The reactor module is suitable for parallel testing of heterogeneous catalysts for various gas-phase reactions close to conventional laboratory conditions. Reliability and efficiency of the reactor are illustrated for the oxidative dehydrogenation of propane and ethane. [Copyright &y& Elsevier]

Published
2002
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16. Flexible NiZr-based structured catalysts for ethylene production through ODH of ethane: Catalytic performance enhancement

Author

Maria Alicia del H. Ulla, Juan Pablo Bortolozzi, Viviana Guadalupe Milt, Eduardo Ernesto Miro, Ezequiel David Banus, and N. L. Courtalón

Subjects
Ethylene production, Recubrimientos y Películas, Ethylene, Materials science, Catalytic Ceramic paper, Inorganic chemistry, chemistry.chemical_element, INGENIERÍAS Y TECNOLOGÍAS, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Redox, Catalysis, chemistry.chemical_compound, Ingeniería de los Materiales, Zr promoter, Dehydrogenation, Cubic zirconia, Oxidative dehydrogenation of ethane, Zirconium, Ni catalysts, Nickel oxide, Non-blocking I/O, General Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, chemistry, 0210 nano-technology
Abstract

Flexible structured catalysts based on Ni and Zr deposited on a ceramic paper made of SiO2-Al2O3andZrO2fibers showed to be active and selective for the Oxidative Dehydrogenation of Ethane. Zirconiumpromoter strongly interacted with nickel oxide and produced structural changes that affected the NiOredox behavior, crystal growth and lattice order which enhanced selectivity towards ethylene. The varia-tion of the concentration of the precursor solution used and the addition of zirconia short fibers, affectedthe catalytic performance. The lower the concentration of the solution used to incorporate the catalyst,the better the catalytic performance. The addition of zirconia fibers also showed beneficial effects on ethylene production. Fil: Bortolozzi, Juan Pablo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina Fil: Banus, Ezequiel David. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina Fil: Courtalón, N. L.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina Fil: Ulla, Maria Alicia del H.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina Fil: Milt, Viviana Guadalupe. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina Fil: Miro, Eduardo Ernesto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina

Published
2016

17. Nickel oxide supported on porous clay heterostructures as selective catalysts for the oxidative dehydrogenation of ethane

Author

M. D. Soriano, E. Rodríguez Castellón, Juan Antonio Cecilia, Patricia Concepción, José Jiménez-Jiménez, V. Torres, Said Agouram, Benjamín Solsona, J.M. López Nieto, and Ana Dejoz

Subjects
Ethylene, Materials science, Catalysts, Nickel oxide, Non-blocking I/O, Inorganic chemistry, chemistry.chemical_element, Nickel oxide supported, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Catalysis, 0104 chemical sciences, chemistry.chemical_compound, chemistry, Porous Clay Heterostructures, Dehydrogenation, Oxidative dehydrogenation of ethane, 0210 nano-technology, Dispersion (chemistry), Selectivity, Titanium
Abstract

[EN] Porous clay heterostructures (PCH) have shown to be highly efficient supports for nickel oxide in the oxidative dehydrogenation of ethane. Thus NiO supported on silica with a PCH structure shows productivity towards ethylene three times higher than if NiO is supported on a conventional silica. This enhanced productivity is due to the increase in the catalytic activity and especially to the drastic increase in the selectivity to ethylene. Additionally, PCH silica partially modified with titanium in the columns (PCH-Ti) have also been synthesized and used as supports for NiO. An enhanced activity and selectivity to ethylene was found over NiO supported over PCH-Ti compared to the corresponding catalysts supported over the Ti-free PCH. The enhanced catalytic performance has been related to the high dispersion of nickel oxide particles on the support, which leads to a lower reducibility of the nickel oxide, hindering the oxidation of ethane into carbon oxides. More interestingly, the particle morphology plays an important role on the catalyst selectivity since a higher distortion of the NiO crystal lattice parameter meant an enhanced selectivity to ethylene., The authors would like to acknowledge the DGICYT in Spain (CTQ2012-37925-C03-1, CTQ2012-37925-C03-2 and CTQ2012-37925-C03-3) and the FEDER for financial support. We also thank the University of Valencia and SCSIE-UV for assistance.

Published
2016

18. FeCrAlloy Monoliths Coated with Ni/Al2O3 Applied to the Low-Temperature Production of Ethylene

Author

Mario Montes, Paula Brussino, Maria Alicia del H. Ulla, Juan Pablo Bortolozzi, Oihane Sanz, and Ezequiel David Banus

Subjects
Recubrimientos y Películas, Ethylene, Scanning electron microscope, 02 engineering and technology, lcsh:Chemical technology, Heterogeneous catalysis, 01 natural sciences, lcsh:Chemistry, chemistry.chemical_compound, oxidative dehydrogenation of ethane, Ingeniería de los Materiales, ethylene, lcsh:TP1-1185, FeCrAlloy monoliths, structured catalysts, Monolith, geography.geographical_feature_category, 021001 nanoscience & nanotechnology, ethane, ETHYLENE, ce, 0210 nano-technology, Selectivity, purl.org/becyt/ford/2.5 [https], o mixed oxides, Materials science, OXIDATIVE DEHYDROGENATION OF ETHANE, chemistry.chemical_element, INGENIERÍAS Y TECNOLOGÍAS, 010402 general chemistry, Catalysis, FeCrALLOY MONOLITHS, oxidative dehydrogenation, ceramic papers, Ni/Al2O3, Dehydrogenation, Physical and Theoretical Chemistry, conversion, geography, nio/al2o3, reactors, nio catalysts, 0104 chemical sciences, Ingeniería Química, Nickel, purl.org/becyt/ford/2.4 [https], lcsh:QD1-999, chemistry, Chemical engineering, purl.org/becyt/ford/2 [https]
Abstract

This paper investigates the oxidative dehydrogenation of ethane to produce ethylene at low temperatures (500 &deg, C) in metallic structured substrates. To check this point, the FeCrAlloy&reg, monoliths with different channel sizes (289&ndash, 2360 cpsi) were prepared. The monoliths were coated with a Ni/Al2O3 catalyst (by washcoating of alumina and the latter nickel impregnation) and characterized by Scanning Electron Microscopy and Energy-Dispersive X-ray analysis (SEM-EDX), Temperature-Programmed Reduction (TPR), X-ray Diffraction (XRD) and X-ray Photoelectron Spectroscopy (XPS). The catalytic results showed that all monoliths coated with ~300 mg of catalyst presented similar ethane conversion (15%) at 450 &deg, C. However, the lowest selectivity to ethylene was found for the monolith with the lower channel size and the higher geometric surface area, where a heterogeneous catalyst layer with Ni enriched islands was generated. Therefore, it can be said that the selectivity to ethylene is linked to the distribution of Ni species on the support (alumina). Nevertheless, in all cases the selectivity was high (above 70%). On the other hand, the stability in reaction tests of one of the coated monoliths was done. This structured catalyst proved to be more stable under reaction conditions than the powder catalyst, with an initial slight drop in the first 8 h but after that, constant activity for the 152 h left.

Published
2018

19. NiO diluted in high surface area TiO2 as efficient catalysts for the oxidative dehydrogenation of ethane

Author

Benjamín Solsona, Enrique Rodríguez-Castellón, Said Agouram, M. D. Soriano, D. Delgado, M.I. Vázquez, J.M. López Nieto, and Rut Sanchis

Subjects
Anatase, Inorganic chemistry, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Catalysis, Ethylene, Surface coverage, NiO diluted in TiO2, Dehydrogenation, Oxidative dehydrogenation of ethane, Titanium oxide, Chemistry, Process Chemistry and Technology, Nickel oxide, Non-blocking I/O, 021001 nanoscience & nanotechnology, Nickel oxide catalysts, 0104 chemical sciences, Nickel, (ODH), 0210 nano-technology, Titanium
Abstract

[EN] Catalysts consisting of NiO diluted in high surface area TiO2 can be as efficient in the oxidative dehydrogenation of ethane as the most selective NiO-promoted catalysts reported previously in the literature. By selecting the titania matrix and the NiO loading, yields to ethylene over 40% have been obtained. In the present article, three different titanium oxides (TiO2) have been employed as supports or diluters of nickel oxide and have been tested in the oxidative dehydrogenation of ethane to ethylene. All TiO2 used present anatase as the main crystalline phase and different surface areas of 11,55 and 85 m(2) g(-1). It has been observed that by selecting an appropriate nickel loading and the titanium oxide extremely high selectivity towards ethylene can be obtained. Thus, nickel oxide supported on TiO2 with high surface areas (i.e. 55 and 85 m(2) g(-1)) have resulted to give the best catalytic performance although the optimal nickel loading is different for each case. The optimal catalyst has been obtained for NiO-loadings up to 5-10 theoretical monolayers regardless of the TiO2 employed. Free TiO2 is inactive whereas unsupported NiO is active and unselective (forming mainly carbon dioxide) and, therefore, unmodified NiO particles have to be avoided in order to obtain the optimal catalytic performance. The use of low surface area titania (11 m(2) g(-1)) have led to the lowest selectivity to olefin due to the presence of an excess of free NiO particles. (C) 2017 Elsevier B.V. All rights reserved., The authors would like to acknowledge the DGICYT in Spain CTQ2012-37925-C03-2, CTQ2015-68951-C3-1-R, CTQ2015-68951-C3-3-R and SEV-2012-0267 Projects for financial support. D.D. also thanks Severo Ochoa Excellence fellowship (SVP-2014-068669). We also thank the University of Valencia (UV-INV-AE-16-484416 project) and SCSIE-UV for assistance

Published
2017

20. Oxidative dehydrogenation of ethane: A study over the structure and robustness of Ni–W–O catalysts

Author

Ana Dejoz, Benjamín Solsona, J.M. López Nieto, Isabel Vázquez, Said Agouram, and F. Ivars

Subjects
inorganic chemicals, Ethylene, Hydrogen, General Chemical Engineering, Catalyst support, Inorganic chemistry, Energy Engineering and Power Technology, chemistry.chemical_element, Catalysis, Methane, chemistry.chemical_compound, Dehydrogenation, Nickel tungsten, Oxidative dehydrogenation of ethane, Oxide catalysts, Ethane, Chemistry, organic chemicals, Nickel oxide, Coke, Fuel Technology, Ni-W-O, Oxidative dehydrogenation
Abstract

[EN] The robustness of one selected Ni-W-O catalyst has been studied in the oxidative dehydrogenation of ethane. This catalyst initially deactivates for the first 10 h online decreasing 15% of its catalytic activity compared to its initial stable catalytic activity. However from 10 to 60 h online the catalytic activity keeps almost stable. On the other hand, it has been shown that the Ni-W-O catalyst cannot tolerate an oxygen-free atmosphere (C-2 and He) as nickel oxide is transformed into metallic nickel. Methane and hydrogen as well as abundant coke were formed on the surface of the catalyst in these O-free conditions. However a re-calcination in air leads to the removal of coke, the catalytic performance in the oxidative dehydrogenation of ethane being almost completely restored., Financial support from DGICYT in Spain (Projects CTQ2012-37925-C03-01 and CTQ2012-37925-C03-03) is gratefully acknowledged. The authors also want to thank the SCSIE, University of Valencia, for providing HRTEM facilities.

Published
2014

21. NiCe/γ-Al 2 O 3 coated onto cordierite monoliths applied to Oxidative Dehydrogenation of Ethane (ODE)

Author

Viviana Guadalupe Milt, Ezequiel David Banus, Maria Alicia del H. Ulla, Paula Brussino, and Juan Pablo Bortolozzi

Subjects
NICKEL-CERIUM OXIDES, Materials science, Recubrimientos y Películas, OXIDATIVE DEHYDROGENATION OF ETHANE, Inorganic chemistry, chemistry.chemical_element, Cordierite, 02 engineering and technology, INGENIERÍAS Y TECNOLOGÍAS, engineering.material, 010402 general chemistry, 01 natural sciences, Catalysis, law.invention, X-ray photoelectron spectroscopy, law, Ingeniería de los Materiales, Calcination, Dehydrogenation, NICKEL OXIDE, General Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Ingeniería Química, Nickel, Cerium, chemistry, Otras Ingeniería Química, engineering, CORDIERITE MONOLITHS, Atomic ratio, 0210 nano-technology, Nuclear chemistry
Abstract

The present work investigates the preparation of NiCe/γ-Al2O3 coated cordierite monoliths for oxidative dehydrogenation of ethane (ODE) reaction through a two steps procedure: the primer deposition of a γ-Al2O3 coating consisting in a mixture of micro and nanoparticles via the washcoating method and the latter incorporation of the active phase by impregnation. Moreover, a modification in these two steps was made: the suppression of some calcination steps to save energy in the manufacture process. The structured catalysts, named as Ni(X)Ce(Y)-M, where X = 13 or 19 wt%. Ni and Y = 5 or 8 wt%. Ce respectively, with respect to the alumina loading, were characterized by SEM/EDX, XRD, FTIR, LRS and XPS, and their catalytic activity was tested in the ODE reaction. Furthermore, their mechanical resistance to vibration was studied. Similar results corresponding to the un-promoted system are also presented for comparison. It was found that the co-impregnation of nickel and cerium was affected by the suppression of some calcinations: a preferential absorption of Ce rather than Ni occurred, generating at the end a catalytic coating with a higher Ce/Ni ratio than that of the precursor solution and a lower Ni loading than that of Ni(13)-M. On the other side, in the NiCe-based catalysts the properties of the active sites remained the same despite the increment in the active phase, at a fixed Ce/Ni nominal atomic ratio of 0.17. In the case of the Ni(19)Ce(8)-M system, although the Ni/Al atomic ratios were found lower than those of the nominal ones by EDX and XPS and ethylene selectivity decayed, ethane conversion resulted markedly higher, leading to an improved ethylene yield. Fil: Brussino, Paula. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina Fil: Bortolozzi, Juan Pablo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina Fil: Milt, Viviana Guadalupe. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina Fil: Banus, Ezequiel David. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina Fil: Ulla, Maria Alicia del H.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina

Published
2016

22. Optimizing both catalyst preparation and catalytic behaviour for the oxidative dehydrogenation of ethane of Ni-Sn-O catalysts

Author

Ana Dejoz, Benjamín Solsona, Patricia Concepción, M. D. Soriano, Said Agouram, M.I. Vázquez, and J.M. López Nieto

Subjects
inorganic chemicals, Ethylene, 010405 organic chemistry, Catalyst support, Inorganic chemistry, Oxalic acid, Catalytic behaviour, General Chemistry, Ni-Sn-O oxide catalysts, 010402 general chemistry, 01 natural sciences, Catalysis, 0104 chemical sciences, Catalyst preparation, chemistry.chemical_compound, Ammonium hydroxide, chemistry, Nitric acid, Dehydrogenation, Oxidative dehydrogenation of ethane, Glyoxylic acid
Abstract

[EN] Bulk Ni-Sn-O catalysts have been synthesized, tested in the oxidative dehydrogenation of ethane and characterized by several physicochemical techniques. The catalysts have been prepared by evaporation of the corresponding salts using several additives in the synthesis gel, i.e. ammonium hydroxide, nitric acid, glyoxylic acid or oxalic acid, in the synthesis gel. The catalysts were finally calcined at 500 degrees C in air. Important changes in the catalytic behaviour have been observed depending on the additive. In fact, an important improvement in the catalytic performance is observed especially when some additives, such as glyoxylic or oxalic acid, are used. Thus the productivity to ethylene multiplies by 6 compared to the reference Ni-Sn-O catalyst if appropriate templates are used, and this is the result of an improvement in both the catalytic activity and the selectivity to ethylene. This improved performance has been explained in terms of the decrease of the crystallite size (and the increase in the surface area of catalyst) as well as the modification of the lattice parameter of nickel oxide., The authors would like to acknowledge the DGICYT in Spain (CTQ2015-68951-C3-1-R and CTQ2012-37925-C03-2) for financial support. We also thank the University of Valencia and SCSIE-UV for assistance

Published
2016

23. Oxidative dehydrogenation of ethane over NiO–CeO2 mixed oxides catalysts

Author

S. Hernández, Patricia Concepción, Benjamín Solsona, Benjamin Demicol, and Jose Nieto

Subjects
Cerium oxide, Ethylene, Catalyst characterization (XPS, TPR, XRD, Raman, FTIR of adsorbed CO, oxygen isotopic-exchange), Inorganic chemistry, Non-blocking I/O, chemistry.chemical_element, General Chemistry, Catalysis, Cerium(IV) oxide–cerium(III) oxide cycle, chemistry.chemical_compound, Cerium, chemistry, Dehydrogenation, Oxidative dehydrogenation of ethane, Nickel oxide, Selectivity
Abstract

[EN] In this paper we present the synthesis, characterization and catalytic behaviour in the oxidative dehydrogenation of ethane of NiO-CeO2 mixed oxides. The addition of cerium oxide to NiO strongly modifies its catalytic performance, although the changes in the catalytic behaviour depend on the catalyst composition. The incorporation of low amounts of cerium oxide to NiO multiplies the productivity to ethylene in the oxidative dehydrogenation of ethane by a factor of ca. 7, which is the result of an increase in both catalytic activity and selectivity to ethylene. The enhanced activity has been related to the remarkable increase of the surface area of catalyst and the low crystal sizes of NiO that takes place when a tiny amount of cerium oxide is incorporated to the NiO. The higher selectivity to ethylene has been related to the modification of the nature of Ni-O species, which implies a lower production of carbon oxides. On the other hand, high activity and selectivity is also observed over catalysts rich in cerium ( with Ni/ Ce ratios between 0.2 and 3). In this case, a different mechanism can be proposed in which the high capacity of CeO2 to bomb oxygen from bulk to surface and the partial formation of NiO and Ce1-xNixO2 facilitates a faster reoxidation of active Ni-sites by a synergic effect improving catalytic activity. (C) 2011 Elsevier B.V. All rights reserved., The authors would like to thank the DGICYT in Spain (Project CTQ2009-14495) for financial support. SH thanks a fellowship from DGICYT.

Published
2012

24. Comparison of Ni and Ni-Ce/Al2O3 catalysts in granulated and structured forms: Their possible use in the oxidative dehydrogenation of ethane reaction

Author

Maria Alicia del H. Ulla, T. Weiss, Juan Pablo Bortolozzi, and Laura Beatriz Gutierrez

Subjects
NICKEL-CERIUM OXIDES, Ethylene, Recubrimientos y Películas, OXIDATIVE DEHYDROGENATION OF ETHANE, General Chemical Engineering, Inorganic chemistry, chemistry.chemical_element, INGENIERÍAS Y TECNOLOGÍAS, Industrial and Manufacturing Engineering, Catalysis, chemistry.chemical_compound, Ingeniería de los Materiales, Environmental Chemistry, Dehydrogenation, METALLIC FOAMS, NICKEL OXIDE, Chemistry, Nickel oxide, General Chemistry, STRUCTURED CATALYSTS, Ingeniería Química, Cerium, Nickel, Reagent, Otras Ingeniería Química, Crystallite
Abstract

Ni and Ni-Ce/Alumina catalysts in structured form were prepared, characterized by different techniques and tested in the oxidative dehydrogenation of ethane (ODE). In order to gain further insight into active species, catalysts in granulated form were also synthesized, characterized and evaluated in the same reaction test. The results indicated that the Ni and Ni-Ce/Al2O3 granulated catalysts were active and selective for this reaction. The addition of cerium using two atomic ratios (Ce/Ni = 0.11 and 0.25) significantly increased the ethylene productivity by kg of nickel mainly motivated by the marked increment in ethane conversion. This behavior could be explained by the smaller nickel oxide crystallite size and the incorporation of nickel into the ceria lattice. The structured systems showed similar active species but achieved a better performance in terms of ethane conversion and ethylene productivity, compared with the granulated forms. The higher catalytic activity could be associated with the presence of lower crystallite sizes of the active phases and also related to a better utilization of active sites due to a higher accessibility of the reagents to the catalyst surface. The existence of certain species (mainly chromium oxide) in the coverage also contributed to obtain higher conversion even though the selectivity to ethylene decreased. Lower temperature treatments applied to the structured support (550°C instead of 700°C) reduced the amount of these undesired species that favor the total oxidation of ethane. Fil: Bortolozzi, Juan Pablo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina Fil: Weiss, T.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina Fil: Gutierrez, Laura Beatriz. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina Fil: Ulla, Maria Alicia del H.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina

Published
2014

25. Novel catalytic ceramic papers applied to oxidative dehydrogenation of ethane

Author

D. Terzaghi, Ezequiel David Banus, Maria Alicia del H. Ulla, Viviana Guadalupe Milt, Juan Pablo Bortolozzi, and Laura Beatriz Gutierrez

Subjects
NICKEL-CERIUM OXIDES, Ethylene, Materials science, NICKEL OXIDE, OXIDATIVE DEHYDROGENATION OF ETHANE, Nickel oxide, Inorganic chemistry, Non-blocking I/O, chemistry.chemical_element, General Chemistry, INGENIERÍAS Y TECNOLOGÍAS, CATALYTIC CERAMIC PAPERS, Catalysis, Ingeniería Química, chemistry.chemical_compound, Cerium, chemistry, visual_art, visual_art.visual_art_medium, Atomic ratio, Dehydrogenation, Ceramic
Abstract

The aim of this work was the development of novel structured catalysts applied to the oxidative dehydrogenation of ethane. Different Ni-based catalytic formulations promoted with cerium were incorporated onto ceramic papers and were tested in the reaction. Ceramic papers presented an interconnected 3D-network of silica-alumina fibers almost totally covered by the binder agent (Al2O3) and provided an adequate environment for the deposition of the catalyst. The catalytic results indicated that the paper with Ce/Ni = 0.17 atomic ratio showed the highest ethylene productivity, due to the presence of the smallest crystalline domain size of NiO and the partial incorporation of the Ni cation into the ceria lattice. Fil: Bortolozzi, Juan Pablo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; Argentina Fil: Banus, Ezequiel David. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; Argentina Fil: Terzaghi, D.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; Argentina Fil: Gutierrez, Laura Beatriz. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; Argentina Fil: Milt, Viviana Guadalupe. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; Argentina Fil: Ulla, Maria Alicia del H.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; Argentina

Published
2013

26. Rare Earth-doped Ceria Catalysts for ODHE Reaction in a Catalytic Modified MIEC Membrane Reactor

Author

José M. Serra, María Balaguer, Julio Garcia-Fayos, and M. Pilar Lobera

Subjects
Materials science, Inorganic chemistry, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, 7. Clean energy, 01 natural sciences, Oxygen, Catalysis, Inorganic Chemistry, Membrane reactors, Dehydrogenation, Physical and Theoretical Chemistry, Oxidative dehydrogenation of ethane, Heterogeneous catalysis, Membrane reactor, Organic Chemistry, Cerium, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Thermogravimetry, Membrane, chemistry, 13. Climate action, Limiting oxygen concentration, 0210 nano-technology, Cobalt
Abstract

[EN] An intensification process for the selective oxidation of hydrocarbons integrates a catalytic reactor and an oxygen separation membrane. This work presents the study of oxidative dehydrogenation of ethane at 1123 K in a catalytic membrane reactor based on mixed ionic-electronic conducting (MIEC) membranes. The surface of a membrane made of Ba0.5Sr0.5Co0.8Fe0.2O3-d has been activated using different porous catalytic layers based on rare earth-doped cerias (fluorite structure) and the porous catalytic coating was deposited by screen printing (coating around 15 mu m). The different catalyst formulations were developed by partial substitution of Ce and were synthesized by co-precipitation followed by cobalt impregnation when required. Specifically, seven different catalysts based on the system Ce1-xLnxO2-d (x=0.1 or 0.2; Ln=Tb, Pr, Er, Gd, and Tb+Er), including the effect of cobalt addition (2?% molar) in Ce0.8Tb0.2O2-d, were studied. The ceria catalysts were studied by XRD, SEM, DC-conductivity as a function of oxygen partial pressure, and the high-temperature stability in a CO2 environment was assessed using thermogravimetry. Then, the influence of the ceria catalytic coating on the oxygen permeation flux through the MIEC membrane was studied using argon and methane as the sweep gas in the permeate side. Finally, oxidative dehydrogenation of ethane reaction tests were performed at 1123 K, as a function of the ethane concentration in the feed. The use of a disk-shaped membrane in the reactor made it possible to prevent the direct contact of gaseous oxygen and hydrocarbons and thus to increase the ethylene yield. High ethylene yields (up to approximate to 84?%) were obtained using a catalytic coating based on 20?% Tb-doped ceria including macropores produced by the addition of graphite platelets in the screen printing ink. The high yields obtained in this kind of catalytic membrane are attributed to the combination of: the high catalytic activity; the control of the oxygen concentration in the gas phase (reaction chamber); and the appropriate fluid dynamics, enabling the fast ethylene evacuation., Financial support by the Spanish Ministry for Science and Innovation (ENE2011-24761 FPI BES-2009-015835 grants), EU through FP7 NASA-OTM Project (NMP3-SL-2009-228701), and the Helmholtz Association of German Research Centres through the Helmholtz Alliance MEM-BRAIN (Initiative and Networking Fund) is kindly acknowledged.

Published
2012
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27. Oxidative dehydrogenation of ethane over Ni-W-O mixed metal oxides catalysts

Author

Ana Dejoz, Mabel Vazquez, Patricia Concepción, Benjamín Solsona, J.M. López Nieto, and F. Ivars

Subjects
inorganic chemicals, Ethylene, XRD, Inorganic chemistry, chemistry.chemical_element, TPR, Heterogeneous catalysis, Catalysis, chemistry.chemical_compound, Tungstate, XPS, Dehydrogenation, Physical and Theoretical Chemistry, Oxidative dehydrogenation of ethane, Raman, chemistry.chemical_classification, FTIR of adsorbed CO, Oxygen isotopic exchange, Nickel tungsten metal oxide catalysts, Nickel oxide, Acid strength, Nickel, chemistry, Catalyst characterization, Ethylene oxidation
Abstract

Ni-W-O mixed oxides were prepared through the evaporation of aqueous solutions of nickel nitrate and ammonium tungstate and calcined in air at 500 degrees C for 2 h. The catalysts were characterized by several techniques (N(2) adsorption, X-ray diffraction, temperature-programmed reduction, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy of adsorbed CO, and (18)O/(16)O isotope exchange) and tested in the oxidative dehydrogenation of ethane. The catalytic activity and catalyst reducibility decrease when the W content increases. Thus, nickel sites seem to be the active centers for ethane activation in these catalysts. However, the selectivity to ethylene strongly changes depending on the Ni/W ratio. In W-rich catalysts, in which NiWO(4) and WO(3) are mainly observed, a strong influence of ethane conversion on the selectivity to ethylene is observed. However, in Ni-rich catalysts, in which NiO crystallites and WO(x) nanoparticles are mainly observed, ethane conversion hardly influences the selectivity to ethylene. It has been demonstrated that the nature of the Ni sites and the characteristics and number of the acid sites determine the catalytic behavior of these catalysts. The presence of Lewis acid sites with high acid strength in W-rich catalysts facilitates the decomposition of ethylene during ethane oxidation. (C) 2011 Elsevier Inc. All rights reserved., Financial support from DGICYT in Spain (Project CTQ-2009-14495) and Generalitat Valenciana (ACOMP/2010/091) is gratefully acknowledged.

Published
2011

28. Oxidative dehydrogenation of ethane to ethene on alumina-supported molybdenum-based catalysts modified by vanadium and phosphorus

Author

Elisabeth Bordes-Richard, Akila Barama, Lionel Hilaire, Naima Haddad, Laboratoire de Chimie du Gaz Naturel, Université des Sciences et de la Technologie Houari Boumediene [Alger] (USTHB), Unité de Catalyse et Chimie du Solide - UMR 8181 (UCCS), Centrale Lille Institut (CLIL)-Université d'Artois (UA)-Centrale Lille-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Lille, Laboratoire des Matériaux, Surfaces et Procédés pour la Catalyse (LMSPC), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Université des Sciences et de la Technologie Houari Boumediene = University of Sciences and Technology Houari Boumediene [Alger] (USTHB), Université d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Unité de Catalyse et de Chimie du Solide - UMR 8181 (UCCS), Université d'Artois (UA)-Ecole Centrale de Lille-Ecole Nationale Supérieure de Chimie de Lille (ENSCL)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), and Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS)

Subjects
Molybdena, Inorganic chemistry, Vanadium, chemistry.chemical_element, 02 engineering and technology, General Chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 010402 general chemistry, 021001 nanoscience & nanotechnology, Heterogeneous catalysis, 01 natural sciences, Redox, Catalysis, Vanadium oxide, 0104 chemical sciences, Structure–activity relationships, In situ experiments, chemistry, X-ray photoelectron spectroscopy, Molybdenum, Dehydrogenation, 0210 nano-technology, Oxidative dehydrogenation of ethane, Vanadia
Abstract

Gamma-alumina-supported MoO x , MoVO x (Mo/V = 11) and MoVPO x (Mo/V = 11, V/P = 1) catalysts were prepared and their properties studied by several techniques (EDX-SEM, XRD, XPS, LRS, TPR). Acid–base and catalytic properties were determined by carrying out 2-propanol decomposition and oxidative dehydrogenation of ethane to ethene, respectively. In situ X-ray diffraction and X-ray photoelectron spectroscopy after pre-treatment were carried out in redox conditions (with H 2 /N 2 , C 2 H 6 /N 2 as reducing and O 2 /N 2 as oxidant). The catalytic performance increases along MoO x x x series. Analyses of MoVPO x show that part of Mo is stabilised as Al 2 (MoO 4 ) 3 and that the surface is made up from single or mixed Mo and V oxospecies. Vanadium increases the reducibility of the catalyst as shown by TPD and XPS. Both the acid–base and redox properties are responsible for the catalytic properties of MoVPO x , which are also related to the coordination of Mo active species.

Published
2007

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