Combined experimental and kinetic modelling studies of the pathways of propane and <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si48.gif" display="inline" overflow="scroll"><mml:mi>n</mml:mi></mml:math>-butane aromatization over H-ZSM-5 catalyst

Nguyen, Luong Huu; Vazhnova, Tanya; Kolaczkowski, S.T.; Lukyanov, Dmitry B.

doi:10.1016/j.ces.2006.05.017

Cited by 37 publications

(14 citation statements)

References 30 publications

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“…Benzene has been detected as a minor product in a high pressure study of vanadium oxide/alumina catalysts for butane dehydrogenation [36], can form via the hydrogenolysis of the secondary-secondary C-C bond followed by oligomerization to benzene. Several authors have investigated zeolite based catalysts for the aromatisation of nbutane to benzene [41][42][43]. Shpiro et al [42] described the formation of aromatic compounds from n-butane over Pt/Ga containing zeolites and Nguyen et al [43] combined kinetic and experimental results to determine the mechanistic steps.…”

Section: N-butane Dehydrogenation On V Based Catalystsmentioning

confidence: 99%

“…Several authors have investigated zeolite based catalysts for the aromatisation of nbutane to benzene [41][42][43]. Shpiro et al [42] described the formation of aromatic compounds from n-butane over Pt/Ga containing zeolites and Nguyen et al [43] combined kinetic and experimental results to determine the mechanistic steps. They suggest that the main route is through dehydrogenation to an alkene, followed by oligimerisation, cyclisation then dehydrogenation.…”

Section: N-butane Dehydrogenation On V Based Catalystsmentioning

confidence: 99%

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The role of carbon species in heterogeneous catalytic processes: an in situ soft x-ray photoelectron spectroscopy study

Vass

Hävecker

Zafeiratos

et al. 2008

J. Phys.: Condens. Matter

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High pressure X-ray photoelectron spectroscopy (XPS) is used to characterize heterogeneous catalytic processes. The success of the new technique based on the possibility to correlate the catalytic activity and the electronic structure of an active surface. The dynamic character of a catalyst surface can be demonstrated impressively by this technique. In this contribution the basics of high pressure XPS will be discussed. Three examples of heterogeneous catalytic reactions are presented in this contribution. The selective hydrogenation of 1-pentyne over Pd based catalysts and the dehydrogenation of n-butane and the oxidation of ethylene over V based catalysts. It is shown, that the formation of subsurface carbons plays an important role in all the examples. The incorporated carbon changes the electronic structure of the surface and so controls the selectivity of the reaction. A change of the educts in the reaction atmosphere induces modifications of the electronic surface structure of the operation catalysts.

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Section: N-butane Dehydrogenation On V Based Catalystsmentioning

confidence: 99%

Section: N-butane Dehydrogenation On V Based Catalystsmentioning

confidence: 99%

The role of carbon species in heterogeneous catalytic processes: an in situ soft x-ray photoelectron spectroscopy study

Vass

Hävecker

Zafeiratos

et al. 2008

J. Phys.: Condens. Matter

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“…40 Another key point, evident from Figure 3a, is that ethene is formed in excess compared with hydrogen, indicating that it is produced not only in reaction 3. We suggest that the additional step for ethene formation in the initial catalytic cycle is the well known hydrogen transfer reaction 6,13,[29][30][31]35,52 that in our case could occur between ethane and methoxide groups, as illustrated by reaction 5. Thus, reactions 2, 4 and 5 lead to eq 6 that shows the stoichiometry of the catalytic cycle involving the protolytic cracking of the C−C bond in ethane with formation of methane and ethene.…”

Section: Transformation Of Ethanementioning

confidence: 86%

“…13 Qualitative analogies between the two reaction systems, which are illustrated for ethane reaction by Figure 1, are well documented for the protolytic cracking of C−C and C−H bonds in alkanes with three or more carbon atoms (C 3+ ). [5][6][7]11,12,18,[27][28][29][30][31][32][33][34][35] However, in the case with ethane, only limited experimental information is available. 28,36 It shows that the protolytic cracking of the C−C bond in ethane with formation of methane does indeed take place over acidic zeolites with the MFI structure, 37 but does not contain data regarding the mechanism of this reaction.…”

Section: Introductionmentioning

confidence: 99%

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Toward Better Understanding of the Catalytic Action of Acidic Zeolites: Investigation in Methane and Ethane Activation and Transformation

2012

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Studies of cracking reactions of alkanes with three or more carbon atoms have been central to the development of our understanding of the catalytic action of acidic zeolites, which are important catalysts in petrochemical and chemical industries. However, the mechanisms of the simplest cracking reactions, i.e. the cracking of the C−H and C−C bonds in methane and ethane, have only been studied theoretically, not experimentally. Here we show that ethane is converted over a H-MFI zeolite at 510-550 o C with formation of such primary products as ethene, hydrogen, methane and propane. To explain these results, we suggest and consider two catalytic cycles of the reaction. The first cycle involves protolytic cracking of the C−H bond with formation of hydrogen and ethoxide group, the latter decomposing into ethene and the zeolite acid site. We propose that the second cycle is initiated by the protolytic cracking of the C−C bond that results in formation of methane and a methoxide group as an intermediate. We theorize that this reacts with ethane molecules regenerating the zeolite acid site and producing (i) methane and ethene via hydrogen transfer and (ii) propane via a C−C bond formation reaction. Both suggested catalytic cycles are fully supported by the kinetic results of this study and are in a good agreement with recent theoretical work. We also demonstrate that the cracking of the C−H bond in methane (that could proceed via methoxide intermediate) does not occur over H-MFI zeolites up to 700 o C most likely due to high activation energy. The proposed involvement of methoxide groups, as active intermediates, in ethane transformation provides a basis and excellent opportunity for theoretical studies of such interesting reactions as hydrogen transfer and C−C bond formation with participation of these surface species.

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Chemical kinetic modeling of i‐butane and n‐butane catalytic cracking reactions over HZSM‐5 zeolite

et al. 2011

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A chemical kinetic model for i‐butane and n‐butane catalytic cracking over synthesized HZSM‐5 zeolite, with SiO2/Al2O3 = 484, and in a plug flow reactor under various operating conditions, has been developed. To estimate the kinetic parameters of catalytic cracking reactions of i‐butane and n‐butane, a lump kinetic model consisting of six reaction steps and five lumped components is proposed. This kinetic model is based on mechanistic aspects of catalytic cracking of paraffins into olefins. Furthermore, our model takes into account the effects of both protolytic and bimolecular mechanisms. The Levenberg–Marquardt algorithm was used to estimate kinetic parameters. Results from statistical F‐tests indicate that the kinetic models and the proposed model predictions are in satisfactory agreement with the experimental data obtained for both paraffin reactants. © 2011 American Institute of Chemical Engineers AIChE J, 58: 2456–2465, 2012

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Combined experimental and kinetic modelling studies of the pathways of propane and n-butane aromatization over H-ZSM-5 catalyst

Cited by 37 publications

References 30 publications

The role of carbon species in heterogeneous catalytic processes: an in situ soft x-ray photoelectron spectroscopy study

The role of carbon species in heterogeneous catalytic processes: an in situ soft x-ray photoelectron spectroscopy study

Toward Better Understanding of the Catalytic Action of Acidic Zeolites: Investigation in Methane and Ethane Activation and Transformation

Chemical kinetic modeling of i‐butane and n‐butane catalytic cracking reactions over HZSM‐5 zeolite

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