Effects of Lewis acidity of metal oxide promoters on the activity and selectivity of Co-based Fischer–Tropsch synthesis catalysts (English)

In: Journal of Catalysis   ;  338 ;  250-264  ;  2016
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Highlights Metal oxide-forming promoters enhance FTS turnover frequency and C5+ selectivity. Half monolayer coverage of promoter on Co nanoparticles maximizes promotion effects. Magnitude of promotion effects correlates positively with promoter Lewis acidity.

Abstract Metal oxides of Ce, Gd, La, Mn, and Zr were investigated as promoters for improving the activity and selectivity of Co-based FTS catalysts. The extent to which these promoters decrease the selectivity toward CH4 and increase the selectivity toward C5+ hydrocarbons was found to depend on both the loading and the composition of the oxide promoter. Elemental mapping by STEM–EDS revealed that the propensity for a given metal oxide to associate with Co affects the sensitivity of the product distribution to changes in promoter loading. For all promoters, a sufficiently high loading resulted in the product distributions becoming insensitive to further increases in promoter loading, very likely due to the formation of a half monolayer of promoter oxide over the Co surface. Simulations suggest that the fraction of Co active sites that are adjacent to the promoter moieties approaches unity at this degree of coverage. The oxidation state of the promoter metal cation under reaction conditions, determined by in situ XANES measurements, was used to calculate relative Lewis acidity of the promoter metal cation. A strong positive correlation was found between the C5+ product selectivity and the Lewis acidity of the promoter metal cations, suggesting that the promotional effects are a consequence of Lewis acid–base interactions between the reaction intermediates and the promoter metal cations. Rate data obtained at different pressures were used to estimate the apparent rate coefficient and the CO adsorption constant appearing in the Langmuir–Hinshelwood expression that describes the CO consumption kinetics for both unpromoted and the metal oxide-promoted catalysts. Both parameters exhibited positive correlations with the promoter Lewis acidity. These results are consistent with the hypothesis that the metal cations of the promoter act as Lewis acids that interact with the O atom of adsorbed CO to facilitate CO adsorption and dissociation.

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Metal organic frameworks as efficient heterogeneous catalysts for the oxidation of benzylic compounds with t-butylhydroperoxide
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Catalytic partial oxidation of methane on platinum investigated by spatial reactor profiles, spatially resolved spectroscopy, and microkinetic modeling
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Defect engineering of mesoporous nickel ferrite and its application for highly enhanced water oxidation catalysis
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An environmentally friendly Z-scheme WO3/CDots/CdS heterostructure with remarkable photocatalytic activity and anti-photocorrosion performance
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Role of silver species in H2-NH3-SCR of NOx over Ag/Al2O3 catalysts: Operando spectroscopy and DFT calculations
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Immobilizing heteropolyacids on zirconia-modified silica as catalysts for oleochemistry transesterification and esterification reactions
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Interactions in Alumina-Based Iron Oxide-Vanadium Oxide Catalysts under High Temperature Calcination and SO~2 Oxidation Conditions
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Recyclable solid catalysts for epoxidation of alkenes: Amino- and oniumsilica-immobilized [HPO4{W2O2(μ-O2)2(O2)2}]2− anion
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Cercosporin-bioinspired photoreductive activation of aryl halides under mild conditions
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Recyclable solid catalysts for epoxidation of alkenes: Amino- and oniumsilica-immobilized [HPO4{W2O2(m-O2)2(O2)2}]2- anion
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Boron Nitride: A Novel Support for Ruthenium-Based Ammonia Synthesis Catalysts
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Lean NO~x Catalysis over Sn/�-Al~2O~3 Catalysts
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Effects of Pretreatment Conditions on CO Oxidation over Supported Au Catalysts
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New Catalysts for Hydroprocessing: Bimetallic Oxynitrides MI-MII-O-N (MI, MII = Mo, W, V, Nb, Cr, Mn, and Co). Part I. Synthesis and Characterization
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Outstanding Performances of Magnesia-Supported Platinum-Tin Catalysts for Citral Selective Hydrogenation
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More about the future, less about the past
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V2O5-TiO2 Catalysts for the Vapor-Phase Oxidation of b-Picoline: Influence of the TiO2-Carrier
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Deuterium Tracer Studies on Hydrotreating Catalysts -- Isotopic Exchange between Hydrogen and Hydrogen Sulfide on Sulfided NiMo-Al2O3
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Developing multiple-site kinetic models in catalysis simulation: A case study of O2 + 2NO #8596 2NO2 oxidation#8211reduction chemistry on Pt(100) catalyst crystal facets
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A detailed spectroscopic analysis of the growth of oxy-carbon species on the surface of Pt/Al2O3 during propane oxidation
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Peculiarities Observed in H-D Exchange between Perdeuterioisobutane and H-Zeolites
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Structure and properties of PVMo11O40 heteropolyoxomolybdate supported on silica SBA-15 as selective oxidation catalyst
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Vanadium species supported on inorganic oxides as catalysts for propene epoxidation in the presence of N2O as an oxidant
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Self-assembly induced metal ionic-polymer derived Fe-Nx/C nanowire as oxygen reduction reaction electrocatalyst
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Reactive and inhibiting species in the electrocatalytic oxidation of glycerol on gold. A study combining in-situ visible reflectance and ATR-SEIRAS
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Sour water–gas shift reaction over Pt/CeZrO2 catalysts
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Catalytic reactions enhanced under microwave-induced local thermal non-equilibrium in a core–shell, carbon-filled zeolite@zeolite
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Binary metal (Ti, Cu) oxyhydroxy–organic (terephthalate) framework: An interface model nanocatalyst for hydrogen purification
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Microwave-assisted synthesis of palladium nanoparticles supported on graphene: A highly active and recyclable catalyst for carbon–carbon cross-coupling reactions
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Effect of calcination temperature on CrOx–Y2O3 catalysts for fluorination of 2-chloro-1,1,1-trifluoroethane to 1,1,1,2-tetrafluoroethane
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DFT and ATR-IR insight into the conformational flexibility of cinchonidine adsorbed on platinum: Proton exchange with metal
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Catalytic behavior of hydrothermally synthesized La0.5Sr0.5MnO3 single-crystal cubes in the oxidation of CO and CH4
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Epoxidation of propylene with H2 and O2 in the explosive regime in a packed-bed catalytic membrane reactor
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Pitfalls and best practices in measurements of the electrochemical surface area of platinum-based nanostructured electro-catalysts
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How is DMSP decomposed when catalyzed by RlDddP binuclear iron DMSP lyase?
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Strongly enhanced acidity and activity of amorphous silica–alumina by formation of pentacoordinated AlV species
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Sn-Beta zeolite hydrothermally synthesized via interzeolite transformation as efficient Lewis acid catalyst
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Amorphous Ti species in titanium silicalite-1: Structural features, chemical properties, and inactivation with sulfosalt
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Catalytic performance and characterization of Rh–CeO2-MgO catalysts for the catalytic partial oxidation of methane at short contact time
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Carbazole-decorated covalent triazine frameworks: Novel nonmetal catalysts for carbon dioxide fixation and oxygen reduction reaction
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WOx supported on γ-Al2O3 with different morphologies as model catalysts for alkanol dehydration
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An FTIR Spectroscopic Study of the Selective Oxidation of Nitrosobenzene to Nitrobenzene by Metal Oxides
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Increased Catalytic Activity Caused by Local Destruction of Linear Zeolite Channels: Effect of Reduction Temperature on Heptane Conversion over Platinum Supported in H-Mordenite
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Features and mechanism of atomic oxygen radical anion emission from yttria-stabilized zirconia electrolyte
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Comparative study on redox properties of nanosized CeO2 and CuO/CeO2 under CO/O2
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Priority Communication - Reactivity Enhancement by Molecular Traffic Control
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Synthesis and Characterization of Alkali-free, Ga-Substituted MCM-41 and Its Performance for n-Hexane Conversion
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Aromatization of n-Heptane on Pt-Alkali or Alkali-Earth Exchanged Beta Zeolite Catalysis: Catalyst Deactivation and Regeneration
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Enantioselective hydrogenation of ethyl pyruvate in biphasic liquid–liquid media by reusable surfactant-stabilized aqueous suspensions of platinum nanoparticles
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Characterization of WOx/CeO2 catalysts and their reactivity in the isomerization of hexane
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Selective Oxidation of Dimethylether to Formaldehyde on Small Molybdenum Oxide Domains
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Investigation of the catalytic activities of sulfated mesoporous Ti, Nb, and Ta oxides in 1-hexene isomerization
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Dependence of the kinetics of liquid-phase photocatalyzed reactions on oxygen concentration and light intensity
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Efficient liquid-phase hydrogenation of cinnamaldehyde to cinnamyl alcohol with a robust PtFe/HPZSM-5 catalyst
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Acceptorless dehydrogenation of amines and alcohols using simple ruthenium chloride
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Novel manganese oxide confined interweaved titania nanotubes for the low-temperature Selective Catalytic Reduction (SCR) of NOx by NH3
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Development of a molecular kinetic scheme for methane partial oxidation over a Rh/α-Al2O3 catalyst
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Pt vs. Au in water–gas shift reaction
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Photocatalytic water-splitting solar-to-hydrogen energy conversion: Novel LiMoO3(IO3) molybdenyl iodate based on WO3-type sheets
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A Solid Acidity Scale Based on the ^3^1p MAS-NMR Shift of Chemisorbed Triethylphosphine Oxide
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Synthesis, Characterization and Activity Studies of Carbon Supported Platinum Alloy Catalysts
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Bimetallic nano-Pd/PdO/Cu system as a highly effective catalyst for the Sonogashira reaction
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A facile method for the fabrication of hierarchical nanosized metal catalysts
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Impact of heterogeneities in silica-supported copper catalysts on their stability for methanol synthesis
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Selective Catalytic Reduction of NO with Methane on Gallium Catalysts
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Preparation and characterization of lanthanum-promoted cobalt–copper catalysts for the conversion of syngas to higher oxygenates: Formation of cobalt carbide
Wang, Zi / Kumar, Nitin / Spivey, James J. | 2016
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Supported Au Catalysts
over, Effects of Pretreatment Conditions on CO Oxidation / Park, Eun Duck / Lee, Jae Sung | 1999
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Propene hydrogenation over truncated octahedral Pt nanoparticles supported on alumina
Yoo, Jung Whan / Hathcock, David J. / El-Sayed, Mostafa A. | 2003
1
Comparison of Monolith-Supported Metals forthe Direct Oxidation of Methane to Syngas
Torniainen, P.M. / Chu, X. / Schmidt, L.D. | 1994
1
Tuning the π-electron delocalization degree of mesoporous carbon for hydrogen peroxide electrochemical generation
Liu, Haipeng / Zhu, Shengli / Cui, Zhenduo / Li, Zhaoyang / Wu, Shuilin / Liang, Yanqin | 2020
1
Facet-dependent electrocatalytic water splitting reaction on CeO2: A DFT + U study
Wu, Tiantian / López, Núria / Vegge, Tejs / Hansen, Heine Anton | 2020
1
The interplay between the suprafacial and intrafacial mechanisms for complete methane oxidation on substituted LaCoO3 perovskite oxides
Wang, Ting / Zhang, Chao / Wang, Jieyu / Li, Haiyan / Duan, Yan / Liu, Zheng / Lee, Jun Yan / Hu, Xiao / Xi, Shibo / Du, Yonghua et al. | 2020
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Synergy of nanoconfinement and promotion in the design of efficient supported iron catalysts for direct olefin synthesis from syngas
Gu, Bang / He, Shun / Peron, Deizi V. / Strossi Pedrolo, Debora R. / Moldovan, Simona / Ribeiro, Mauro C. / Lobato, Bruno / Chernavskii, Petr A. / Ordomsky, Vitaly V. / Khodakov, Andrei Y. | 2019
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Construction of porous nanoscale NiO/NiCo2O4 heterostructure for highly enhanced electrocatalytic oxygen evolution activity
Sun, Shanfu / Jin, Xiaoli / Cong, Bowen / Zhou, Xin / Hong, Weizhao / Chen, Gang | 2019
1
Atomic-Scale Structure of Co-Mo-S Nanoclusters in Hydrotreating Catalysts
Lauritsen, J. V. / Helveg, S. / Laegsgaard, E. / Stensgaard, I. / Clausen, B. S. / Topsoe, H. / Besenbacher, F. | 2001
1
Isobutane Dehydrogenation over Supported Platinum Acid-Base AlGaPON Catalysts
Delsarte, S. / Mauge, F. / Grange, P. | 2001
1
Characterization of WO~x/ZrO~2 by Vibrational Spectroscopy and n-Pentane Isomerization Catalysis
Scheithauer, M. / Cheung, T.-K. / Jentoft, R. E. / Grasselli, R. K. / Gates, B. C. / Knoezinger, H. | 1998
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Characterization of (V2O5-WO3) on TiOx-Al2O3 Catalysts by 1H-, 15N-, and 51V-Solid State NMR Spectroscopy
Mastikhin, V.M. / Terskikh, V.V. / Lapina, O.B. / Filimonova, S.V. / Seidl, M. / Knözinger, H. | 1995
1
Zirconia-supported 12-tungstophosphoric acid as a solid catalyst for the synthesis of linear alkyl benzenes
Devassy, B. M. / Lefebvre, F. / Halligudi, S. B. | 2005
1
Preparation and characterization of MCM-41-supported hydroxo-bridged dicupric-phenanthroline complex
Wong, S. T. / Lee, C. H. / Lin, T. S. / Mou, C. Y. | 2004
1
Thermal and catalytic formation of radicals during autoxidation
Neuenschwander, Ulrich / Hermans, Ive | 2011
1
Facile synthesis of polyaniline using gold catalyst
Chen, Zhi / Della Pina, Cristina / Falletta, Ermelinda / Lo Faro, Massimiliano / Pasta, Mauro / Rossi, Michele / Santo, Nadia | 2008
1
V~2O~5/TiO~2 Catalysts for the Vapor-Phase Oxidation of beta-Picoline: Influence of the TiO~2-Carrier
Heinz, D. / Hoelderich, W. F. / Krill, S. / Boeck, W. / Huthmacher, K. | 2000
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Polyethylene Formation on a Planar Surface Science Model of a Chromium Oxide Polymerization Catalyst
Thuene, P. C. / Loos, J. / Lemstra, P. J. / Niemantsverdriet, J. W. | 1999
1
The Influence of Sonication on the Palladium-Catalysed Dehydrdogenation of Tetrahydronaphthalene
Mason, T. J. / Lorimer, J. P. / Paniwnyk, L. / Wright, P. W. | 1994
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Catalyst design for highly efficient carbon dioxide hydrogenation to formic acid under buffering conditions
Weilhard, Andreas / Salzmann, Kevin / Navarro, Miquel / Dupont, Jairton / Albrecht, Martin / Sans, Victor | 2020
1
Selective catalytic oxidation of ammonia to nitrogen at low temperature on Pt/CuO/Al2O3
Olofsson, Göran / Reine Wallenberg, L. / Andersson, Arne | 2004
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