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  In Situ Hydrocracking of Fischer–Tropsch Hydrocarbons: CO-Prompted Diverging Reaction Pathways for Paraffin and α-Olefin Primary Products

Duyckaerts, N., Trotus, I.-T., Swertz, A.-C., Schüth, F., & Prieto, G. (2016). In Situ Hydrocracking of Fischer–Tropsch Hydrocarbons: CO-Prompted Diverging Reaction Pathways for Paraffin and α-Olefin Primary Products. ACS Catalysis, 6(6), 4229-4238. doi:10.1021/acscatal.6b00904.

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 Creators:
Duyckaerts, Nicolas1, Author              
Trotus, Ioan-Teodor1, Author              
Swertz, Ann-Christin1, 2, Author              
Schüth, Ferdi1, Author              
Prieto, Gonzalo3, Author              
Affiliations:
1Research Department Schüth, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445589              
2Service Department Lehmann (EMR), Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445625              
3Research Group Prieto, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2243639              

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Free keywords: synthetic fuels; gas-to-liquid; multifunctional catalysis; process intensification; product distribution; olefin oligomerization; ZSM-5; platinum
 Abstract: The single-step production of wax-free liquid hydrocarbons from syngas (H2 + CO) via integration of Fischer–Trospch (FT) and hydrocracking catalysts represents an attractive approach toward process intensification in compact gas-to-liquid technologies. Despite current, intensive efforts on the development of hybrid (multifunctional) catalysts to this end, not much is known about the reactivity of different FT primary products on hydrocracking catalysts under syngas. Using model compounds, the individual and collective reactivities of n-paraffin and α-olefin FT primary products were systematically studied on a Pt/nano-H-ZSM-5 hydrocracking catalyst under H2 (standard hydrocracking) and syngas (in situ hydroprocessing) atmospheres. Under H2, both reactants show indistinguishable reactivity as rapid olefin hydrogenation precedes hydrocracking. Under syngas, however, inhibition of (de)hydrogenation functionalities by CO poisoning of metal sites leads to a notable divergence of the reaction pathways for n-paraffins and α-olefins. Under these conditions, α-olefins showed enhanced reactivity, as an initial dehydrogenative activation step is not required, and contributed to moderate secondary cracking, likely via enhanced competitive adsorption on the acid sites. Besides, CO poisoning restored the intrinsic activity of the zeolite for the oligomerization of short-chain (α-)olefins, providing an additional net chain-growth pathway, which contributes to reducing the overall yield to undesired gas (C4–) hydrocarbons. These findings emphasize the key role of not only the chain-length distribution, but also the olefinic content of the FT primary hydrocarbons for the ultimate product distribution, and suggest guidelines for the design of multifunctional catalysts for the single-step synthesis of liquid hydrocarbons from syngas.

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Language(s): eng - English
 Dates: 2016-05-232016-07-01
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acscatal.6b00904
 Degree: -

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Title: ACS Catalysis
  Abbreviation : ACS Catal.
Source Genre: Journal
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Publ. Info: Washington, DC : ACS
Pages: - Volume / Issue: 6 (6) Sequence Number: - Start / End Page: 4229 - 4238 Identifier: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435