Selective Oxidation of Ethane to Acetaldehyde and Acrolein over Silica-Supported Vanadium Catalysts Using Oxygen as Oxidant

Zhang, Zhao; Yamada, Yusuke; Teng, Yun‐Lei; Ueda, Atsushi; Nakagawa, Kiyoharu; Kobayashi, Tetsuhiko

doi:10.1006/jcat.1999.2740

Cited by 56 publications

(53 citation statements)

References 50 publications

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“…However, the other band characteristic of the vibration of the terminal VpO group of V 2 O 5 at 1018 cm −1 was not detected. These findings are similar to those reported by Zhao et al (2000) for a sample with a high loading of vanadium (10 wt%) on SiO 2 .…”

Section: Ft-ir Analysessupporting

confidence: 91%

Structure and Reactivity of a V₂O₅/Al₂O₃ Catalyst Modified with Cerium in the Oxidative Dehydrogenation of Cyclohexane

AbdelDayem

2004

Adsorption Science & Technology

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ABSTRACT:The oxidative dehydrogenation (ODH) of cyclohexane with air was studied on a 10 w/w% V 2 O 5 /Al 2 O 3 catalyst modified by different weight percentage (wt%) cerium loadings. The catalysts employed were characterized by N 2 adsorption, O 2 chemisorption, TEM, XRD and FT-IR spectroscopy. Benzene and cyclohexene were the main components of the products, with the benzene and cyclohexene selectivities depending on the wt% cerium loading, the order of cerium and vanadium impregnation, and the reaction temperature. The best cyclohexane conversion and good benzene selectivity were obtained at 500°C using a vanadium catalyst modified by 10 wt% cerium. The same catalyst exhibited a maximum selectivity for cyclohexene at 300°C.Different types of vanadyl species present in the system were identified by IR measurements. Thus, vanadium-oxygen clusters were detected in the V 2 O 5 /Al 2 O 3 material, although such clusters were not found in the cerium-vanadium catalysts. Polymeric CeVO 4 species were detected in cerium-modified V 2 O 5 /Al 2 O 3 catalysts by XRD. The concentration of these species depended on the wt% cerium loading and the order of cerium and vanadium impregnation on alumina. The selectivity of cerium-modified V 2 O 5 /Al 2 O 3 catalysts towards cyclohexene was attributed mainly to the presence of such polymeric CeVO 4 species. Oxygen chemisorption and electronic microscopic studies attributed the marked improvement in cyclohexane conversion of the cerium-vanadium samples to the presence of relatively high-dispersed vanadium species.

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Section: Ft-ir Analysessupporting

confidence: 91%

Structure and Reactivity of a V₂O₅/Al₂O₃ Catalyst Modified with Cerium in the Oxidative Dehydrogenation of Cyclohexane

AbdelDayem

2004

Adsorption Science & Technology

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“…The dependencies of these rates on C 2 H 6 , O 2 , and H 2 O concentrations are identical on supported VO x and V 2 O 5 powders, suggesting that similar active centers are present on both surfaces. C 2 H 6 -C 2 D 6 and C 2 H 6 -D 2 O reactants undergo ODH reactions without forming C 2 H 6-x D x or C 2 H 4-x D x mixed isotopomers, suggesting that C-H bond activation steps are irreversible. The absence of C 2 H 4-x D x mixed isotopomers suggests that activation of ethene C-H bonds leads only to combustion products.…”

Section: Discussionmentioning

confidence: 99%

“…Several other reaction schemes and mechanisms have been proposed for ethane ODH on vanadia and other active oxides. [1][2][3][4][5][6][7][8][9] Previous studies on VO x -SiO 2 have provided the most detailed mechanistic picture for ethane reactions, [6][7][8][9] but for catalysts leading to more complex reaction products, including acetone and acetaldehyde.…”

Section: Introductionmentioning

confidence: 99%

Ethane Oxidative Dehydrogenation Pathways on Vanadium Oxide Catalysts

et al. 2002

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Kinetic and isotopic tracer and exchange measurements were used to determine the identity and reversibility of elementary steps involved in ethane oxidative dehydrogenation (ODH) on VO x /Al 2 O 3 and VO x /ZrO 2 . C 2 H 6 -C 2 D 6 -O 2 and C 2 H 6 -D 2 O-O 2 react to form alkenes and CO x without concurrent formation of C 2 H 6-x D x or C 2 H 4-x D x isotopomers, suggesting that C-H bond cleavage in ethane and ethene is an irreversible and kinetically relevant step in ODH and combustion reactions. Primary ethane ODH reactions show normal kinetic isotopic effects (k C-H /k C-D ) 2.4); similar values were measured for ethane and ethene combustion (1.9 and 2.8, respectively). 16 The alkyl species formed in these steps desorb irreversibly as ethene and the resulting O-H groups recombine to form H 2 O and reduced V centers in reversible desorption steps. These reduced V centers reoxidize by irreversible dissociative chemisorption of O 2 . A pseudo-steady state analysis of these elementary steps together with these reversibility assumptions led to a rate expression that accurately describes the observed inhibition of ODH rates by water and the measured kinetic dependence of ODH rates on C 2 H 6 and O 2 pressures. This kinetic analysis suggests that surface oxygen, OH groups, and oxygen vacancies are the most abundant reactive intermediates during ethane ODH on active VO x domains.

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“…The use of vanadium-supported catalysts for oxidative dehydrogenations, for instance, is largely described: reactions like methanol to formaldehyde [14], ethane to acetaldehyde/acrolein [15], ethyl benzene to styrene [16], to quote few examples, can be effectively carried out by a proper choice of the preparation methods, inorganic supports and reaction conditions. Different approaches based on post-synthesis modifications were proposed in the literature in order to introduce vanadium centres within the interlayer space of clays.…”

Section: Introductionmentioning

confidence: 99%

On the Properties of a Novel V-Containing Saponite Catalyst for Propene Oxidative Dehydrogenation

et al. 2009

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Selective Oxidation of Ethane to Acetaldehyde and Acrolein over Silica-Supported Vanadium Catalysts Using Oxygen as Oxidant

Cited by 56 publications

References 50 publications

Structure and Reactivity of a V₂O₅/Al₂O₃ Catalyst Modified with Cerium in the Oxidative Dehydrogenation of Cyclohexane

Structure and Reactivity of a V₂O₅/Al₂O₃ Catalyst Modified with Cerium in the Oxidative Dehydrogenation of Cyclohexane

Ethane Oxidative Dehydrogenation Pathways on Vanadium Oxide Catalysts

On the Properties of a Novel V-Containing Saponite Catalyst for Propene Oxidative Dehydrogenation

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Selective Oxidation of Ethane to Acetaldehyde and Acrolein over Silica-Supported Vanadium Catalysts Using Oxygen as Oxidant

Cited by 56 publications

References 50 publications

Structure and Reactivity of a V2O5/Al2O3 Catalyst Modified with Cerium in the Oxidative Dehydrogenation of Cyclohexane

Structure and Reactivity of a V2O5/Al2O3 Catalyst Modified with Cerium in the Oxidative Dehydrogenation of Cyclohexane

Ethane Oxidative Dehydrogenation Pathways on Vanadium Oxide Catalysts

On the Properties of a Novel V-Containing Saponite Catalyst for Propene Oxidative Dehydrogenation

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Structure and Reactivity of a V₂O₅/Al₂O₃ Catalyst Modified with Cerium in the Oxidative Dehydrogenation of Cyclohexane

Structure and Reactivity of a V₂O₅/Al₂O₃ Catalyst Modified with Cerium in the Oxidative Dehydrogenation of Cyclohexane