A radiotracer (14C) and catalytic study of thiophene hydrodesulfurization on the clean and carbided Mo(100) single-crystal surface

Bussell, Mark E.

doi:10.1016/0021-9517(87)90214-4

Cited by 46 publications

(8 citation statements)

References 18 publications

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“…The literature related to a wide spectrum of reactions whose mechanistic details have been clarified using surface analytical methodologies is extensive. These reactions include the isomerization and cyclization of alkanes, − ,− the hydrogenation of olefins, − cyclohexane dehydrogenation, ,− cyclotrimerization of acetylene, − the water-gas shift reaction, − methanol synthesis, − and thiophene hydrodesulfurization. − A common theme in these studies has been to establish through single-crystal studies a direct relationship between the structure of the catalytic surface and the specific catalytic function exhibited by that surface.…”

Section: Metal Single Crystals As Model Catalystsmentioning

confidence: 99%

Correlations between Surface Science Models and “Real-World” Catalysts

Goodman

1996

J. Phys. Chem.

158

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Over the past two decades the "pressure and material gaps" separating ultrahigh-vacuum surface science and technical catalysis has been bridged by coupling an apparatus for the measurement of reaction kinetics at elevated pressures with an ultrahigh-vacuum system for surface analysis. Studies with this combined methodology have provided an atomic-level understanding of various aspects of heterogeneous catalysis such as structure/activity relationships, the role of promoters and inhibitors on catalytic activity, and the nature of the metal-metal bond in mixed-metal catalysts. These investigations have demonstrated the relevance of single-crystal studies for modeling the behavior of high surface area supported catalysts as well as the power of surface analytical techniques for characterizing adsorbed reactants and intermediates.

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Section: Metal Single Crystals As Model Catalystsmentioning

confidence: 99%

Correlations between Surface Science Models and “Real-World” Catalysts

Goodman

1996

J. Phys. Chem.

158

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“…An inhibiting effect of heptane on HDS of five kinds of sulfur compound mixtures (dimethyl disulfide, diethyl disulfide, benzenethiol, thiacyclopentane, and thiophene) at 370 °C and 20-30 MPa has been reported (Phillipson, 1971). It has been reported that the presence of cis-2butene does not have any particular influence on thiophene HDS on a single crystal of Mo at 340 °C and atmospheric pressure (Bussell and Somorjai, 1987). An inhibiting effect of naphthalene or tetralin on HDS of 4,6-dimethyldibenzothiophene at 2.5 MPa has been observed (Isoda et al, 1994).…”

Section: Introductionmentioning

confidence: 99%

Hydrodesulfurization of Catalytic Cracked Gasoline. 1. Inhibiting Effects of Olefins on HDS of Alkyl(benzo)thiophenes Contained in Catalytic Cracked Gasoline

Hatanaka

Yamada

Sadakane³

1997

Ind. Eng. Chem. Res.

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The HDS reaction feature of CCG on Co−Mo/γ-Al2O3 was investigated in detail to make clear the important factors for the deep HDS of CCG. Two kinds of CCG, which are produced from different origins and contain 229 and 61 ppm sulfur, respectively, were examined. GC-AED analyses showed that both CCG contain 11 alkylthiophenes, 2 alkylbenzothiophenes, 3 alkylthiacyclopentanes, and 2 disulfides. In the reaction at 210 °C, 1.6 MPa using a conventional flow reactor of pilot scale, the total sulfur content decreased from 229 to 127 ppm, whereas 22 ppm of thiols was produced. The HDS reactivities of alkylbenzothiophenes were higher than those of alkylthiophenes, and HDS reactivity decreased with increasing the number of alkyl groups. The reactivities of these sulfur compounds in CCG were much lower than those of the corresponding pure compounds obtained by the individual reaction of pure sulfur compounds. The low reactivity of sulfur compounds in CCG was found to be ascribed to the inhibiting effect of olefins in CCG by comparing the HDS reactivity of thiophene in different solvents including olefins. The inhibiting effect of olefin seems to be caused by two types of adsorption of olefin, that is, weak adsorption and strong adsorption.

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“…From the kinetic studies on thiophene HDS and successive butene hydrogenation by recirculation flow reactor on Co-Mo/γ-Al 2 O 3 at 235-265 °C and atmospheric pressure, it was proposed that H 2 S affects the HDS reaction by competitive adsorption to the HDS active site; however, butene does not affect HDS and moves to the hydrogenation active site, which is different from the HDS active site (Satterfield and Roberts, 1968). The H 2 S and cis-2-butene (reaction products of thiophene HDS) addition study was also carried out in thiophene HDS on the Mo(100) single-crystal surface, and only H 2 S showed inhibition on HDS (Bussell and Somorjai, 1987). In this way, most of these works have indicated that the HDS-active site is different from butene hydrogenation active site.…”

Section: Introductionmentioning

confidence: 99%

Hydrodesulfurization of Catalytic Cracked Gasoline. 2. The Difference between HDS Active Site and Olefin Hydrogenation Active Site

Hatanaka

Yamada

Sadakane³

1997

Ind. Eng. Chem. Res.

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The inhibiting effect of olefin on CCG HDS (found in our previous report) was further investigated from a mechanistic point of view. A small amount of thiophene (corresponding to ca. 100 wt ppm of sulfur content) and varying amounts of olefins (diisobutylene and 1-octene) dissolved in toluene were hydrotreated on Co−Mo/Al2O3 at 150 °C at 1.3 MPa. Both the total HDS (thiophene HDS minus thiol and sulfide formation) and thiophene HDS were strongly inhibited by a small amount of olefin (1 mol %). However, when the olefin content was increased over 20 mol %, thiophene HDS rather recovered while the total HDS monotonously decreased. Both isoolefin and n-olefin can interact with the thiophene HDS active site, resulting in the inhibition on thiophene HDS. The interaction between the HDS active site and olefins was further studied by examining the effect of H2S, an well-known inhibitor for HDS, on hydrogenation of olefins. The hydrogenation of n-olefin as well as thiophene HDS was sensitively inhibited by H2S, while the hydrogenation of 2,4,4-trimethyl-2-pentene was promoted. The interaction was also studied by examining the effects of Co, an well-known promoter for HDS, on HDS and olefin reaction over different Co/(Co + Mo) ratio catalysts. HDS was promoted by Co; however, isoolefin hydrogenation was retarded slightly and n-olefin hydrogenation was largely retarded. Three types of active sites for thiophene HDS, n-olefin hydrogenation, and isoolefin hydrogenation, were proposed.

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A radiotracer (14C) and catalytic study of thiophene hydrodesulfurization on the clean and carbided Mo(100) single-crystal surface

Cited by 46 publications

References 18 publications

Correlations between Surface Science Models and “Real-World” Catalysts

Correlations between Surface Science Models and “Real-World” Catalysts

Hydrodesulfurization of Catalytic Cracked Gasoline. 1. Inhibiting Effects of Olefins on HDS of Alkyl(benzo)thiophenes Contained in Catalytic Cracked Gasoline

Hydrodesulfurization of Catalytic Cracked Gasoline. 2. The Difference between HDS Active Site and Olefin Hydrogenation Active Site

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