The optimally performing Fischer-Tropsch catalyst

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Microkinetics simulations are presented based on DFT-determined elementary reaction steps of the Fischer-Tropsch (FT) reaction. The formation of long-chain hydrocarbons occurs on stepped Ru surfaces with CH as the inserting monomer, whereas planar Ru only produces methane because of slow CO activation. By varying the metal-carbon and metal-oxygen interaction energy, three reactivity regimes are identified with rates being controlled by CO dissociation, chain-growth termination, or water removal. Predicted surface coverages are dominated by CO, C, or O, respectively. Optimum FT performance occurs at the interphase of the regimes of limited CO dissociation and chain-growth termination. Current FT catalysts are suboptimal, as they are limited by CO activation and/or O removal. State-of-the-art quantum-chemical reaction data were used in a microkinetics simulations study to elucidate the different fundamental kinetic regimes underlying Fischer-Tropsch activity and selectivity. Based on the nature of the rate-controlling steps, three regimes were identified: I) monomer formation, II) chain-growth termination, and III) water formation.

TaalEngels
Pagina's12746-12750
Aantal pagina's5
TijdschriftAngewandte Chemie - International Edition
Volume53
Nummer van het tijdschrift47
DOI's
StatusGepubliceerd - 1 nov 2014

Vingerafdruk

Carbon Monoxide
Catalysts
Monomers
Chemical activation
Metals
Discrete Fourier transforms
Water
Chemical reactions
Methane
Hydrocarbons
Kinetics
Carbon
Oxygen

Trefwoorden

    Citeer dit

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    title = "The optimally performing Fischer-Tropsch catalyst",
    abstract = "Microkinetics simulations are presented based on DFT-determined elementary reaction steps of the Fischer-Tropsch (FT) reaction. The formation of long-chain hydrocarbons occurs on stepped Ru surfaces with CH as the inserting monomer, whereas planar Ru only produces methane because of slow CO activation. By varying the metal-carbon and metal-oxygen interaction energy, three reactivity regimes are identified with rates being controlled by CO dissociation, chain-growth termination, or water removal. Predicted surface coverages are dominated by CO, C, or O, respectively. Optimum FT performance occurs at the interphase of the regimes of limited CO dissociation and chain-growth termination. Current FT catalysts are suboptimal, as they are limited by CO activation and/or O removal. State-of-the-art quantum-chemical reaction data were used in a microkinetics simulations study to elucidate the different fundamental kinetic regimes underlying Fischer-Tropsch activity and selectivity. Based on the nature of the rate-controlling steps, three regimes were identified: I) monomer formation, II) chain-growth termination, and III) water formation.",
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    The optimally performing Fischer-Tropsch catalyst. / Filot, I.A.W.; van Santen, R.A.; Hensen, E.J.M.

    In: Angewandte Chemie - International Edition, Vol. 53, Nr. 47, 01.11.2014, blz. 12746-12750.

    Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

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