CO as a Promoting Spectator Species of CxHy Conversions Relevant

Oct 10, 2018 - Luk, Mondelli, Mitchell, Siol, Stewart, Curulla Ferré, and Pérez-Ramírez. 2018 8 (10), pp 9604–9618. Abstract: The identification ...
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CO as a Promoting Spectator Species of CxHy Conversions Relevant for Fischer-Tropsch Chain Growth on Cobalt: Evidence from Temperature Programmed Reaction and Reflection Absorption Infrared Spectroscopy C.J. (Kees-Jan) Weststrate, and J. W. (Hans) Niemantsverdriet ACS Catal., Just Accepted Manuscript • DOI: 10.1021/acscatal.8b02743 • Publication Date (Web): 10 Oct 2018 Downloaded from http://pubs.acs.org on October 10, 2018

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ACS Catalysis

CO as a Promoting Spectator Species of CxHy Conversions Relevant for Fischer-Tropsch Chain Growth on Cobalt: Evidence from Temperature Programmed Reaction and Reflection Absorption Infrared Spectroscopy

C.J. Weststrate1,*, J.W. Niemantsverdriet1,2 1SynCat@DIFFER,

2

Syngaschem BV, P.O. Box 6336, 5600 HH Eindhoven, The Netherlands

SynCat@Beijing, Synfuels China Technology Co. Ltd., Leyuan South Street II, No. 1, Huairou District, 101407 Beijing, China

ABSTRACT

Cobalt-catalyzed low temperature Fischer-Tropsch synthesis is a prime example of an industrially relevant reaction in which CxHy intermediates involved in chain growth react in the presence of a large quantity of COad. In this study we use a Co(0001) single crystal model catalyst to investigate how CO, adsorbed alongside CxHy adsorbates, affects their reactivity. Temperature programmed reaction spectroscopy was used to determine the hydrogen content of the CxHy intermediates formed at different temperatures and Infrared absorption spectroscopy was used to obtain more specific information on the chemical identity of the various reaction intermediates formed. Ethene,

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propene and but-1-ene precursors decompose below 200 K. The 1-alkyne adsorbate is identified as major product, while some alkylidyne species form as well when the initial alkene coverage is high. The surface hydrogen atoms produced in the low temperature decomposition step start leaving the surface >300 K. When an alkyne(/Had)-covered surface is heated in the presence of CO the alkyne adsorbates are hydrogenated to the corresponding alkylidyne, at temperatures