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

Lömker, Patrick; Degerman, David; Goodwin, Christopher M.; Shipilin, Mikhail; Amann, Peter; Rodrigues, Gabriel L. S.; Garcia-Martinez, Fernando; Rameshan, Raffael; Gladh, Jörgen; Wang, Hsin-Yi; Soldemo, Markus; Holm, Alexander; Tober, Steffen; Schober, Jan-Christian; Jacobse, Leon; Vonk, Vedran; Gleißner, Robert; Noei, Heshmat; Hegedues, Zoltan; Stierle, Andreas; Schlueter, Christoph; Nilsson, Anders

doi:10.1038/s41467-025-56082-8

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

Journal Article · Fri Jan 24 00:00:00 EST 2025 · Nature Communications

DOI:https://doi.org/10.1038/s41467-025-56082-8· OSTI ID:2575642

^[1]; Degerman, David ^[2]; ^[3]; Shipilin, Mikhail ^[2]; Amann, Peter ^[4]; ^[2]; Garcia-Martinez, Fernando ^[5]; Rameshan, Raffael ^[6]; ^[7]; Wang, Hsin-Yi ^[2]; ^[2]; ^[8]; ^[9]; Schober, Jan-Christian ^[5]; Jacobse, Leon ^[10]; ^[5]; Gleißner, Robert ^[5]; Noei, Heshmat ^[5]; ^[5]; ^[9] more »

Stockholm Univ. (Sweden); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
Stockholm Univ. (Sweden)
Stockholm Univ. (Sweden); ALBA Synchrotron Light Source, Cerdanyola del Valles (Spain)
Technical Univ. of Darmstadt (Germany); Stockholm Univ. (Sweden)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
Montanuniversität Leoben, Leoben (Austria)
Stockholm Univ. (Sweden); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE)
Stockholm Univ. (Sweden); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE); Linköping Univ., Norrköping (Sweden)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany)
Fritz Haber Institute of the Max Planck Society, Berlin (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)

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$(0001)$ and Co$$(10\bar{1}4)$$, and in-situ high energy surface X-ray diffraction of Co$(0001)$ 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/-C_xH_y 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.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 2575642

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 16; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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