scholarly journals Influence of the support on rhodium speciation and catalytic activity of rhodium-based catalysts for total oxidation of methane

2020 ◽  
Vol 10 (17) ◽  
pp. 6035-6044
Author(s):  
Yu Zhang ◽  
Peter Glarborg ◽  
Martin Peter Andersson ◽  
Keld Johansen ◽  
Thomas Klint Torp ◽  
...  

In Rh-catalysts for CH4-oxidation, Si-rich zeolite supports yield the more active Rh2O3 nanoparticle form and the highest SO2 and H2O tolerance.

2010 ◽  
Vol 59 (9) ◽  
pp. 1713-1719 ◽  
Author(s):  
A. Yu. Stakheev ◽  
A. M. Gololobov ◽  
I. E. Beck ◽  
G. O. Bragina ◽  
V. I. Zaikovsky ◽  
...  

Catalysts ◽  
2021 ◽  
Vol 11 (4) ◽  
pp. 427
Author(s):  
Marius Stoian ◽  
Vincent Rogé ◽  
Liliana Lazar ◽  
Thomas Maurer ◽  
Jacques C. Védrine ◽  
...  

Methane, discovered in 1766 by Alessandro Volta, is an attractive energy source because of its high heat of combustion per mole of carbon dioxide. However, methane is the most abundant hydrocarbon in the atmosphere and is an important greenhouse gas, with a 21-fold greater relative radiative effectiveness than CO2 on a per-molecule basis. To avoid or limit the formation of pollutants that are dangerous for both human health and the atmospheric environment, the catalytic combustion of methane appears to be one of the most promising alternatives to thermal combustion. Total oxidation of methane, which is environmentally friendly at much lower temperatures, is believed to be an efficient and economically feasible way to eliminate pollutants. This work presents a literature review, a statu quo, on catalytic methane oxidation on transition metal oxide-modified ceria catalysts (MOx/CeO2). Methane was used for this study since it is of great interest as a model compound for understanding the mechanisms of oxidation and catalytic combustion on metal oxides. The objective was to evaluate the conceptual ideas of oxygen vacancy formation through doping to increase the catalytic activity for methane oxidation over CeO2. Oxygen vacancies were created through the formation of solid solutions, and their catalytic activities were compared to the catalytic activity of an undoped CeO2 sample. The reaction conditions, the type of catalysts, the morphology and crystallographic facets exposing the role of oxygen vacancies, the deactivation mechanism, the stability of the catalysts, the reaction mechanism and kinetic characteristics are summarized.


Materials ◽  
2021 ◽  
Vol 14 (10) ◽  
pp. 2495
Author(s):  
Daniela Pietrogiacomi ◽  
Maria Cristina Campa ◽  
Ida Pettiti ◽  
Simonetta Tuti ◽  
Giulia Luccisano ◽  
...  

Ni/ZrO2 catalysts, active and selective for the catalytic partial oxidation of methane to syngas (CH4-CPO), were prepared by the dry impregnation of zirconium oxyhydroxide (Zhy) or monoclinic ZrO2 (Zm), calcination at 1173 K and activation by different procedures: oxidation-reduction (ox-red) or direct reduction (red). The characterization included XRD, FESEM, in situ FTIR and Raman spectroscopies, TPR, and specific surface area measurements. Catalytic activity experiments were carried out in a flow apparatus with a mixture of CH4:O2 = 2:1 in a short contact time. Compared to Zm, Zhy favoured the formation of smaller NiO particles, implying a higher number of Ni sites strongly interacting with the support. In all the activated Ni/ZrO2 catalysts, the Ni–ZrO2 interaction was strong enough to limit Ni aggregation during the catalytic runs. The catalytic activity depended on the activation procedures; the ox-red treatment yielded very active and stable catalysts, whereas the red treatment yielded catalysts with oscillating activity, ascribed to the formation of Niδ+ carbide-like species. The results suggested that Ni dispersion was not the main factor affecting the activity, and that active sites for CH4-CPO could be Ni species at the boundary of the metal particles in a specific configuration and nuclearity.


Author(s):  
Tran Thi Thu Huyen ◽  
Dang Thi Minh Hue ◽  
Nguyen Thi Tuyet Mai ◽  
Tran Thi Luyen ◽  
Nguyen Thi Lan

Gases of m-xylene is one of the popurlar toxic pollutants in the exhaust gases, it is emitted into the environment from factories and engines because the fuel in the engine does not burn completely. The best solution in order to remove this toxic gases of m-xylene to protect the environment is transforming them completely into CO2 and H2O by catalysts. Perovskite of LaMnO3 is one of the catalysts that was synthesized and studied the catalytic properties in total oxidation of m-xylene in our previous report. Obtained results showed that the LaMnO3 perovskite has good catalytic characterizations such as large surface area and the amount of α-oxygen adsorbed on the catalyst is large too. So, it exhibits a good catalytic activity in total oxidation of m-xylene at relatively low reaction temperature. In present work, the reaction order  and kinetics of this reaction are determined. The obtained results demonstrated that the reaction order value with respect to m-xylene is equal to about 1, to oxygene is proximately equal to 0 and the order of reaction is equal to about 1. Based on reaction order data, it was thought that the pathway of m-xylene oxidation by air oxygen  over LaMnO3 may be followed through which the Langmuir - Hinshelwood mechanism. Keywords Catalyst, perovskite, oxidation, m-xylene, kinetics References [1] Penã M.A and Fierro J.L.G (2001), << Chemical Stuctures and Performance of Perovskite Oxide>>, Chem. Rev, 101, pp 1981-2018. [2] Seiyama T., Yamazoe N. and Eguchi K. (1985), <<Characterization and Activity of some Mixed Metal Oxide Catalysts>>, Ind. Eng. Chem. Prod. Res. Dev., 24, pp. 19-27.[3] [3] Van Santen R. A., Neurock M. (2006), Molecular Heterogeneous catalysis, Wiley – VCH, pp.62-244. [4] Petrovics, Terlecki - Baricevic A., Karanovic Lj., Kirilov - Stefanov P. , Zdujic M., Dondur V., Paneva D., Mitov I., Rakic V. (2008), <<LaMO3 (M = Mg, Ti, Fe) perovskite type oxides : Preparation, Characterization and Catalytic Properties in Methane deep Oxidation>>, Appl. Catal. B, Env., 79, pp. 186-198. [5] Spinicci R., Tofanari A., Faticanti M., Pettiti I. and Porta P. (2001), <<Hexane Total Oxidation on LaMO3 (M = Mn, Co, Fe) perovskite-type oxides>>, J. Mole. Catal., 176, pp. 247-252. [6] Trần Thị Thu Huyền, Nguyễn Thị Minh Hiền, Nguyễn Hữu Phú (2006), <<Study on the preparation of perovskite oxides La1-xSrxMnO3 (x = 0; 0,3; 0,5) by sol - gel citrate method and their catalytic activity for m-xylene toltal oxidation>>, Hội nghị xúc tác và hấp phụ toàn quốc lần thứ IV, Tp. Hồ Chí Minh, Tr. 477-482.[7] Trần Thị Thu Huyền, Nguyễn Thị Minh Hiền, Nguyễn Hữu Phú (2009), <<Nghiên cứu động học của phản ứng oxi hóa hoàn toàn m-xylen trên các xúc tác perovskit LaMnO3 và La0,7A0,3MnO3 (A = Sr, Ca, Mg)>>, Tạp chí Hóa học, T.47 (6A), Tr 132-136.[8] Geoffrey C. Bond, Catherine Louis, David T. Thompson (2006), <<Catalysis by Gold>>, Catalytic Science Series-Vol.6.


Catalysts ◽  
2020 ◽  
Vol 10 (8) ◽  
pp. 922
Author(s):  
Kevin Keller ◽  
Patrick Lott ◽  
Henning Stotz ◽  
Lubow Maier ◽  
Olaf Deutschmann

Water, which is an intrinsic part of the exhaust gas of combustion engines, strongly inhibits the methane oxidation reaction over palladium oxide-based catalysts under lean conditions and leads to severe catalyst deactivation. In this combined experimental and modeling work, we approach this challenge with kinetic measurements in flow reactors and a microkinetic model, respectively. We propose a mechanism that takes the instantaneous impact of water on the noble metal particles into account. The dual site microkinetic model is based on the mean-field approximation and consists of 39 reversible surface reactions among 23 surface species, 15 related to Pd-sites, and eight associated with the oxide. A variable number of available catalytically active sites is used to describe light-off activity tests as well as spatially resolved concentration profiles. The total oxidation of methane is studied at atmospheric pressure, with space velocities of 160,000 h−1 in the temperature range of 500–800 K for mixtures of methane in the presence of excess oxygen and up to 15% water, which are typical conditions occurring in the exhaust of lean-operated natural gas engines. The new approach presented is also of interest for modeling catalytic reactors showing a dynamic behavior of the catalytically active particles in general.


Catalysts ◽  
2020 ◽  
Vol 10 (6) ◽  
pp. 613
Author(s):  
Hussein Mahdi S. Al-Aani ◽  
Mihaela M. Trandafir ◽  
Ioana Fechete ◽  
Lucia N. Leonat ◽  
Mihaela Badea ◽  
...  

To improve the catalytic performance of an active layered double hydroxide (LDH)-derived CuCeMgAlO mixed oxide catalyst in the total oxidation of methane, it was promoted with different transition-metal cations. Thus, two series of multicationic mixed oxides were prepared by the thermal decomposition at 750 °C of their corresponding LDH precursors synthesized by coprecipitation at constant pH of 10 under ambient atmosphere. The first series of catalysts consisted of four M(3)CuCeMgAlO mixed oxides containing 3 at.% M (M = Mn, Fe, Co, Ni), 15 at.% Cu, 10 at.% Ce (at.% with respect to cations), and with Mg/Al atomic ratio fixed to 3. The second series consisted of four Co(x)CuCeMgAlO mixed oxides with x = 1, 3, 6, and 9 at.% Co, while keeping constant the Cu and Ce contents and the Mg/Al atomic ratio. All the mixed oxides were characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM) coupled with X-ray energy dispersion analysis (EDX), X-ray photoelectron spectroscopy (XPS), nitrogen adsorption-desorption at −196 °C, temperature-programmed reduction under hydrogen (H2-TPR), and diffuse reflectance UV-VIS spectroscopy (DR UV-VIS), while thermogravimetric and differential thermal analyses (TG-DTG-DTA) together with XRD were used for the LDH precursors. The catalysts were evaluated in the total oxidation of methane, a test reaction for volatile organic compounds (VOC) abatement. Their catalytic performance was explained in correlation with their physicochemical properties and was compared with that of a reference Pd/Al2O3 catalyst. Among the mixed oxides studied, Co(3)CuCeMgAlO was found to be the most active catalyst, with a temperature corresponding to 50% methane conversion (T50) of 438 °C, which was only 19 °C higher than that of a reference Pd/Al2O3 catalyst. On the other hand, this T50 value was ca. 25 °C lower than that observed for the unpromoted CuCeMgAlO system, accounting for the improved performance of the Co-promoted catalyst, which also showed a good stability on stream.


1999 ◽  
Vol 2 (3) ◽  
pp. 104-111
Author(s):  
Ahmad Suseno ◽  
Triyono Triyono ◽  
Bambang Setiaji

Effects of Ce addition on Pt/γ - Al2O3 catalysts preparation and their catalytic activity on oxidation of methane have been investigated. In this study, the catalysts were prepared by impregnating chloride salt solution of palladium and sulphate salt of cerium on γ-AI2O3 support. Characterization of catalysts was conducted by gas sorption method to determine surface area, pore radius and pore volume. The test of catalytic activity on oxidation of methane was carried out in a flow reactor system at a temperature range from 350°C to 600°C. Products of reaction were analysed by non-dispersive IR spectroscopy. It was observed that the surface area, pore radius and pore volume decrease with the addition of cerium. The results of oxidation process showed that Pd-Ce/γ-Al2O3 catalyst can be used for oxidation of methane up to 90.62% conversion


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