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Selective hydrogenation of CO on Fe3S4{111}: a computational study

Roldan Martinez, Alberto and De Leeuw, Nora Henriette 2017. Selective hydrogenation of CO on Fe3S4{111}: a computational study. Faraday Discussions 197 , pp. 325-336. 10.1039/C6FD00224B

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Abstract

Fischer-Tropsch (FT) synthesis has been a recursive method to form valuable molecules from syngas. Metal surfaces have been extensively studied as a FT catalyst, among them, iron presented several phases under reaction conditions, oxide and carbides, as active sites for the FT and reverse water gas shift reaction. We present the CO reduction on an iron sulfide phase with spinel structure, Fe3S4, considering also the pathways where C-O dissociates leaving CHX species on the surface, which may feed longer aliphatic chains via FT process. We analysed the thermodynamic and kinetic availability of each step leading to O, OH species co-adsorbed on the surface as well as the formation of H2O from the hydrogenation of the alcohol group in the molecule. This detailed analysis let to energy profiles, on both active sites of the surface, and conclude that this Fe3S4 surface is high selectivity towards the formation of methanol, in full agreement with experimental results. These findings point out that the C-C bond formation on greigite takes place through an hydroxycarbene FT mechanism.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Advanced Research Computing @ Cardiff (ARCCA)
Cardiff Catalysis Institute (CCI)
Chemistry
Subjects: Q Science > QD Chemistry
Publisher: Royal Society of Chemistry
ISSN: 1359-6640
Funders: Engineering and Physical Sciences Research Council (EPSRC)
Date of First Compliant Deposit: 10 January 2017
Date of Acceptance: 8 November 2016
Last Modified: 26 Mar 2019 23:14
URI: http://orca-mwe.cf.ac.uk/id/eprint/97308

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