Reaction kinetic behavior of sulfated-zirconia catalysts for butane isomerization

Hong, Zhe; Fogash, K.B.; Dumesic, James A.

doi:10.1016/s0920-5861(99)00050-4

Cited by 60 publications

(38 citation statements)

References 100 publications

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“…Pt/SZ is a catalyst for which many aspects are still under discussion [7][8][9][10][11][12][13][14]. Regarding the Pt state, Sayari and Dicko [37] and Zhao et al [38] show that Pt is metallic.…”

Section: Isomerization Reactions Mechanismsmentioning

confidence: 99%

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Isomerization of 3-methyl(3-13C)pentane over platinum supported sulphated zirconias: reaction mechanisms

Demirci

Garin

2007

Catal Lett

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This paper studies the isomerization mechanisms of 3-methyl(3-13 C)pentane over Pt supported sulphated zirconias (SZs). Pt hydrogenates the reaction intermediates that desorbs, hinders successive isomerizations from occurring and reduces the isomerization steps to two (three with Pt-free SZs). The isomerization is a monomolecular process to which Pt does not participate. Lastly, it is suggested that the ratio between the proportions of methyl migration and ethyl migration could be appreciated as a catalyst intrinsic characteristic.

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Section: Isomerization Reactions Mechanismsmentioning

confidence: 99%

“…The addition of Pt provides bifunctional properties to the catalyst. However, the role of Pt, the nature of the active site and the reaction mechanisms are still under discussion [7][8][9][10][11][12][13][14].…”

Section: Introductionmentioning

confidence: 99%

Isomerization of 3-methyl(3-13C)pentane over platinum supported sulphated zirconias: reaction mechanisms

Demirci

Garin

2007

Catal Lett

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“…[1,22] Steady-state isotopic transient kinetic analysis (SSITKA) studies, for example, have shown the loss of active sites due to site blocking by coke or oligomer formation to be significant. [23] Likewise, studies by Hong et al [24] have demonstrated that the presence of olefins in the feed leads to a higher SZ deactivation rate and produces coke deposits on the surface, whereas other studies have found that small amounts of alkenes promote the reaction initially. [5,23] UV/Vis diffuse reflectance spectroscopy has suggested the formation of carbonaceous species, especially unsaturated ones, during the isomerization of n-butane.…”

Section: Introductionmentioning

confidence: 99%

An Integrated Catalytic and Transient Study of Sulfated Zirconias: Investigation of the Reaction Mechanism and the Role of Acidic Sites in n‐Butane Isomerization

Breitkopf¹

2009

ChemCatChem

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The transient temporal analysis of products (TAP) pulse method has been applied to investigate the isomerization of n‐butane on sulfated zirconias at very low pressure. By combining these results with findings from XRD, XPS, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), temperature‐programmed desorption (TPD), and catalytic studies at atmospheric pressure, a wide range of pressure conditions can be accessed to study the influence of surface sulfate groups on the isomerization activity and the mechanism of this reaction. The catalytic activity of powder catalysts has been correlated to the surface site density of sulfates, with pyrosulfate structures playing a major role in the initiation of the reaction. The complex interplay between sulfate‐free and sulfate‐covered zirconia surfaces for the adsorption of alkanes has been investigated in detail, with TAP pulse experiments showing a monomolecular reaction pathway at low n‐butane partial pressures. Moreover, TAP pulse experiments have allowed detection of the reaction products of this initiation process, including butene and water, and have shown their influence on the deactivation of sulfated zirconias. Heats of adsorption have been calculated from the TAP pulse experiments.

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“…Sulfated metal oxides, especially sulfated zirconia, which is active for alkanes activation at low temperature, have been studied for more than two decades and the results have been reviewed [1][2][3][4][5][6][7][8]. However, several topics, such as the structure of the active sites, the acid strength and the mechanism of alkane isomerization are still subject of debate.…”

Section: Introductionmentioning

confidence: 99%

Influence of calcination procedure on the catalytic property of sulfated zirconia

Li¹,

Nagaoka²,

Simon³

et al. 2007

Catal Lett

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Calcination parameters, such as atmosphere, duration and catalyst bed depth have a marked influence on the catalytic and spectroscopic properties of sulfated zirconia. Sulfated zirconia calcined in nitrogen or synthetic airflow, in deep bed, exhibited comparable activity in n-butane isomerization at 373 K, which suggests that oxygen is not necessary for formation of active sites. Catalysts calcined in shallow bed are catalytically inactive. Thus, the bed depth is concluded to be crucial for the formation of active sites. The samples calcined in shallow bed possessed lower sulfate content and the S=O stretching vibration was located at lower frequency. Calcination in the presence of water vapor also led to lower catalytic activity, sulfate content, and BET area. Extended calcination reduced gradually the activity and the sulfate content, which underlines the labile property of the active sites. A new interpretation of the function of the calcination step is proposed and compared with models described in the literature.

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Reaction kinetic behavior of sulfated-zirconia catalysts for butane isomerization

Cited by 60 publications

References 100 publications

Isomerization of 3-methyl(3-13C)pentane over platinum supported sulphated zirconias: reaction mechanisms

Isomerization of 3-methyl(3-13C)pentane over platinum supported sulphated zirconias: reaction mechanisms

An Integrated Catalytic and Transient Study of Sulfated Zirconias: Investigation of the Reaction Mechanism and the Role of Acidic Sites in n‐Butane Isomerization

Influence of calcination procedure on the catalytic property of sulfated zirconia

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