In-situ probing of the Fischer-Tropsch reaction on Co single crystal surfaces up to 1 bar

Abstract The surface chemistry of the Fischer-Tropsch catalytic reaction over Co has still several unknows. Here, we report an in-situ X-ray photoelectron spectroscopy study of Co $$\left(0001\right)$$ 0001 and Co( $$10\bar{1}4$$ 10 1 ¯ 4 ), and in-situ high energy surface X-ray diffraction of Co $$...

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Main Authors: Patrick Lömker, David Degerman, Christopher M. Goodwin, Mikhail Shipilin, Peter Amann, Gabriel L. S. Rodrigues, Fernando Garcia-Martinez, Raffael Rameshan, Jörgen Gladh, Hsin-Yi Wang, Markus Soldemo, Alexander Holm, Steffen Tober, Jan-Christian Schober, Leon Jacobse, Vedran Vonk, Robert Gleißner, Heshmat Noei, Zoltan Hegedues, Andreas Stierle, Christoph Schlueter, Anders Nilsson
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-56082-8
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author Patrick Lömker
David Degerman
Christopher M. Goodwin
Mikhail Shipilin
Peter Amann
Gabriel L. S. Rodrigues
Fernando Garcia-Martinez
Raffael Rameshan
Jörgen Gladh
Hsin-Yi Wang
Markus Soldemo
Alexander Holm
Steffen Tober
Jan-Christian Schober
Leon Jacobse
Vedran Vonk
Robert Gleißner
Heshmat Noei
Zoltan Hegedues
Andreas Stierle
Christoph Schlueter
Anders Nilsson
author_facet Patrick Lömker
David Degerman
Christopher M. Goodwin
Mikhail Shipilin
Peter Amann
Gabriel L. S. Rodrigues
Fernando Garcia-Martinez
Raffael Rameshan
Jörgen Gladh
Hsin-Yi Wang
Markus Soldemo
Alexander Holm
Steffen Tober
Jan-Christian Schober
Leon Jacobse
Vedran Vonk
Robert Gleißner
Heshmat Noei
Zoltan Hegedues
Andreas Stierle
Christoph Schlueter
Anders Nilsson
author_sort Patrick Lömker
collection DOAJ
description Abstract The surface chemistry of the Fischer-Tropsch catalytic reaction over Co has still several unknows. Here, we report an in-situ X-ray photoelectron spectroscopy study of Co $$\left(0001\right)$$ 0001 and Co( $$10\bar{1}4$$ 10 1 ¯ 4 ), and in-situ high energy surface X-ray diffraction of Co $$\left(0001\right),$$ 0001 , during the Fischer-Tropsch reaction at 0.15 bar - 1 bar and 406 K - 548 K in a H2/CO gas mixture. We find that these Co surfaces remain metallic under all conditions and that the coverage of chemisorbed species ranges from 0.4–1.7 monolayers depending on pressure and temperature. The adsorbates include CO on-top, C/-CxHy and various longer hydrocarbon molecules, indicating a rate-limiting direct CO dissociation pathway and that only hydrocarbon species participate in the chain growth. The accumulation of hydrocarbon species points to the termination step being rate-limiting also. Furthermore, we demonstrate that the intermediate surface species are highly dynamic, appearing and disappearing with time delays after rapid changes in the reactants’ composition.
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spelling doaj-art-a0534538c44d41b592e7787b1fdf3cd92025-01-26T12:40:30ZengNature PortfolioNature Communications2041-17232025-01-0116111010.1038/s41467-025-56082-8In-situ probing of the Fischer-Tropsch reaction on Co single crystal surfaces up to 1 barPatrick Lömker0David Degerman1Christopher M. Goodwin2Mikhail Shipilin3Peter Amann4Gabriel L. S. Rodrigues5Fernando Garcia-Martinez6Raffael Rameshan7Jörgen Gladh8Hsin-Yi Wang9Markus Soldemo10Alexander Holm11Steffen Tober12Jan-Christian Schober13Leon Jacobse14Vedran Vonk15Robert Gleißner16Heshmat Noei17Zoltan Hegedues18Andreas Stierle19Christoph Schlueter20Anders Nilsson21Department of Physics, Stockholm UniversityDepartment of Physics, Stockholm UniversityDepartment of Physics, Stockholm UniversityDepartment of Physics, Stockholm UniversityDepartment of Physics, Stockholm UniversityDepartment of Physics, Stockholm UniversityPhoton Science, Deutsches Elektronen-Synchrotron DESYLehrstuhl für Physikalische Chemie, Montanuniversität LeobenDepartment of Physics, Stockholm UniversityDepartment of Physics, Stockholm UniversityDepartment of Physics, Stockholm UniversityDepartment of Physics, Stockholm UniversityCentre for X-Ray and Nanoscience CXNS, Deutsches Elektronen-Synchrotron DESY, 22607Centre for X-Ray and Nanoscience CXNS, Deutsches Elektronen-Synchrotron DESY, 22607Centre for X-Ray and Nanoscience CXNS, Deutsches Elektronen-Synchrotron DESY, 22607Centre for X-Ray and Nanoscience CXNS, Deutsches Elektronen-Synchrotron DESY, 22607Centre for X-Ray and Nanoscience CXNS, Deutsches Elektronen-Synchrotron DESY, 22607Centre for X-Ray and Nanoscience CXNS, Deutsches Elektronen-Synchrotron DESY, 22607Photon Science, Deutsches Elektronen-Synchrotron DESYCentre for X-Ray and Nanoscience CXNS, Deutsches Elektronen-Synchrotron DESY, 22607Photon Science, Deutsches Elektronen-Synchrotron DESYDepartment of Physics, Stockholm UniversityAbstract The surface chemistry of the Fischer-Tropsch catalytic reaction over Co has still several unknows. Here, we report an in-situ X-ray photoelectron spectroscopy study of Co $$\left(0001\right)$$ 0001 and Co( $$10\bar{1}4$$ 10 1 ¯ 4 ), and in-situ high energy surface X-ray diffraction of Co $$\left(0001\right),$$ 0001 , during the Fischer-Tropsch reaction at 0.15 bar - 1 bar and 406 K - 548 K in a H2/CO gas mixture. We find that these Co surfaces remain metallic under all conditions and that the coverage of chemisorbed species ranges from 0.4–1.7 monolayers depending on pressure and temperature. The adsorbates include CO on-top, C/-CxHy and various longer hydrocarbon molecules, indicating a rate-limiting direct CO dissociation pathway and that only hydrocarbon species participate in the chain growth. The accumulation of hydrocarbon species points to the termination step being rate-limiting also. Furthermore, we demonstrate that the intermediate surface species are highly dynamic, appearing and disappearing with time delays after rapid changes in the reactants’ composition.https://doi.org/10.1038/s41467-025-56082-8
spellingShingle Patrick Lömker
David Degerman
Christopher M. Goodwin
Mikhail Shipilin
Peter Amann
Gabriel L. S. Rodrigues
Fernando Garcia-Martinez
Raffael Rameshan
Jörgen Gladh
Hsin-Yi Wang
Markus Soldemo
Alexander Holm
Steffen Tober
Jan-Christian Schober
Leon Jacobse
Vedran Vonk
Robert Gleißner
Heshmat Noei
Zoltan Hegedues
Andreas Stierle
Christoph Schlueter
Anders Nilsson
In-situ probing of the Fischer-Tropsch reaction on Co single crystal surfaces up to 1 bar
Nature Communications
title In-situ probing of the Fischer-Tropsch reaction on Co single crystal surfaces up to 1 bar
title_full In-situ probing of the Fischer-Tropsch reaction on Co single crystal surfaces up to 1 bar
title_fullStr In-situ probing of the Fischer-Tropsch reaction on Co single crystal surfaces up to 1 bar
title_full_unstemmed In-situ probing of the Fischer-Tropsch reaction on Co single crystal surfaces up to 1 bar
title_short In-situ probing of the Fischer-Tropsch reaction on Co single crystal surfaces up to 1 bar
title_sort in situ probing of the fischer tropsch reaction on co single crystal surfaces up to 1 bar
url https://doi.org/10.1038/s41467-025-56082-8
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