The role of lattice oxygen in the oxidative dehydrogenation of ethane on alumina-supported vanadium oxide

Dinse, Arne; Schomäcker, Reinhard; Bell, Alexis T.

doi:10.1039/b821131k

Cited by 32 publications

(37 citation statements)

References 31 publications

(40 reference statements)

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“…10, the increase of oxalic acid concentration results in an obvious decrease in the catalytic ethylene selectivity. It has meant that the morphology change caused by oxalic acid treatment may be beneficial to deep oxidation to form CO 2 and CO. Lattice oxygen serves as an important factor of catalyst selectivity in the selective oxidation of alkanes [69]. Dai et al, proposed that the adsorbed oxygen species on a perovskite-type catalyst surface were prone to induce ethane complete oxidation, while lattice oxygen species were active for ethane selective oxidation [70,71].…”

Section: Catalyst Performance In Odhe Reactionmentioning

confidence: 99%

Phase-pure M1 MoVNbTeO x catalysts with tunable particle size for oxidative dehydrogenation of ethane

Chu

Chen

et al. 2016

Applied Catalysis A: General

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Section: Catalyst Performance In Odhe Reactionmentioning

confidence: 99%

Phase-pure M1 MoVNbTeO x catalysts with tunable particle size for oxidative dehydrogenation of ethane

Chu

Chen

et al. 2016

Applied Catalysis A: General

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“…The concept of lattice oxygen as source for selective atomic oxygen is central to most interpretations of selective oxidation reactions. In its unrestricted form [19,[79][80][81] the concept calls for free mobility of the resulting lattice defect throughout the catalyst. If this would be correct then it is hard to understand how supported or even grafted catalysts exhibiting only 2-dimensional rafts of active oxide would perform well as selective oxidation catalysts.…”

Section: The Empirical Conceptual Basismentioning

confidence: 99%

Selective Oxidation: From a Still Immature Technology to the Roots of Catalysis Science

Schlögl

2016

Top Catal

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The design of heterogeneous selective oxidation catalysts based upon complex metal oxides is governed at present by a set of empirical rules known as “pillars of oxidation catalysis”. They serve as practical guidelines for catalyst development and guide the reasoning about the catalyst role in the process. These rules are, however, not based upon atomistic concepts and thus preclude their immediate application in for example computer-aided search strategies. The present work extends the ideas of the pillar rules and develops the concept of considering a selective oxidation catalyst as enabler for the execution of a reaction network. The enabling function is controlled by mutual interactions between catalyst and reactants. The electronic structure of the catalyst is defined as a bulk semiconductor with a surface state arising form a terminating over layer being different from the structure of the bulk. These components that can be identified by in situ analytical methods form a chemical system with feedback loops, which is responsible for generating selectivity during execution of the reaction network. This concept is based upon physical observables and could allow for a design strategy based upon a kinetic description that combines the processes between reactants with the processes between catalyst and reactants. Such kinetics is not available at present. Few of the constants required are known but many of them are accessible to experimental determination with in situ techniques

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“…Magnesium oxide was reported to be a good support which suppresses Ni deactivation [5] and is a good candidate to improve ODHE because of its basic nature helping ethylene to desorb and preventing it from further oxidation [22]. According to the dependence of the initial catalytic activity in the oxidative dehydrogenation to the oxygen capacity of catalyst, employing MgO which benefits high lattice oxygen seems to be efficient [19,23]. Magnesia has been widely used as a support because of its high surface area and good stability.…”

Section: Introductionmentioning

confidence: 98%

Sol–gel preparation of NiO/ZrO2(x)–MgO(100−x) nanocatalyst used in CO2/O2 oxidative dehydrogenation of ethane to ethylene: influence of Mg/Zr ratio on catalytic performance

Nezhad

Haghighi

Jodeiri

et al. 2016

J Sol-Gel Sci Technol

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A series of NiO/MgO-ZrO 2 mixed oxide catalysts were prepared using the sol-gel method in which the content of MgO and ZrO 2 was varied and the NiO amount was maintained around 5 wt%. The synthesized samples were characterized by XRD, FESEM, PSD, TEM, EDX dot-mapping, FTIR and the BET techniques and tested for the dehydrogenation of ethane in the presence of CO 2 with limited amount of O 2 . Irrespective of the various Mg/Zr ratios, the uniform dispersion of NiO as a common feature of all synthesized samples was evident from the XRD and EDX results. As indicated by XRD and FESEM analyses, a decrease in the size of nanocrystallites and particles and also an increase in the specific surface area were found when MgO phase is present in the sample. The catalytic evaluations revealed that the existence of basic MgO leads to more efficient performance of zirconia especially at higher temperatures. Hence, using both ZrO 2 and MgO increased the ethane conversion and the ethylene yield. This could be attributed to the effect of high reducibility and low surface acidity. It was observed that among the synthesized catalysts, NiO/ZrO 2(75) -MgO (25) was the most active catalyst with an ethane conversion of 66.35 %. However, NiO/ZrO 2(25) -MgO (75) exhibited the best catalytic performance in the oxidative dehydrogenation of ethane with an ethylene yield of 56.9 % at 650°C. The smaller particle and crystallite size, the narrower particle size distribution, uniform dispersion of the active species and higher surface area with efficient base-acid characteristics seem to be responsible for the superior performance of NiO/ZrO 2(25) -MgO (75) catalyst.Graphical Abstract CO 2 /O 2 oxidative dehydrogenation of ethane was investigated over a series of sol-gel synthesized Ni/ZrO 2 -MgO catalysts differing in Mg/Zr ratio. The presence of MgO alongside zirconia contributed to obtain better textural properties and satisfying ethylene yield. The variation of Mg/Zr ratio indicates that there is optimum MgO content in Ni/ZrO 2(25) -MgO (75) for the best catalytic activity. It is found that Ni/ZrO 2(25) -MgO (75) nanocatalyst, with weight ratio of MgO/ZrO 2 :3/1, effectively dehydrogenated ethane to ethylene in the presence of CO 2 /O 2 at 650°C, giving 56.9 % ethylene yield. This is due to higher surface area, smaller particles and narrow distribution of particle size.

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The role of lattice oxygen in the oxidative dehydrogenation of ethane on alumina-supported vanadium oxide

Cited by 32 publications

References 31 publications

Phase-pure M1 MoVNbTeO x catalysts with tunable particle size for oxidative dehydrogenation of ethane

Phase-pure M1 MoVNbTeO x catalysts with tunable particle size for oxidative dehydrogenation of ethane

Selective Oxidation: From a Still Immature Technology to the Roots of Catalysis Science

Sol–gel preparation of NiO/ZrO2(x)–MgO(100−x) nanocatalyst used in CO2/O2 oxidative dehydrogenation of ethane to ethylene: influence of Mg/Zr ratio on catalytic performance

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