Computational exploration of Fe55@C240-catalyzed Fischer-Tropsch synthesis

No Thumbnail Available
Access rights
embargoedAccess
Journal Title
Journal ISSN
Volume Title
A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
This publication is imported from Aalto University research portal.
View publication in the Research portal

Other link related to publication
Date
2018
Major/Subject
Mcode
Degree programme
Language
en
Pages
13
2741-2753
Series
Physical Chemistry Chemical Physics, Volume 20, issue 4
Abstract
Single-shell carbon-encapsulated iron nanoparticles (SCEINs), Fe@C, have been shown to be charge-transfer complexes that can act as effective catalysts in the hydrogen and oxygen evolution reactions. A new generation of Fe-based catalysts for Fischer-Tropsch synthesis (FTS) which resembles SCEINs, e.g. single carbide nanoparticles encapsulated in carbon shells, has demonstrated enhanced activity and stability for FTS as compared to other carbon-supported Fe-based FTS. Thus the catalytic ability of SCEINs for the water splitting reactions and the Fe-based FTS catalyst with SCEINs-like features stimulated our exploration of SCEINs-catalyzed FTS. We performed ab initio DFT calculations using a realistic SCEINs model system Fe55@C240 to investigate for the first time the adsorption of the main reactants in FTS (CO and H/H2) and further to evaluate the catalytic ability of Fe55@C240 by reproducing the key steps of the well-known Fe-based FTS mechanisms (carbide, enol and CO insertion). Our calculations revealed: (i) a determinant role of Fe in enhancing CO adsorption (ii) strong cooperative effects with the adsorbates that stabilize the binding (iii) a less favourable two-sites reaction on Fe55@C240 due to preferential positions of the reactants farther to each other which prevent enol and carbide FTS mechanisms. We propose therefore a possible CO insertion path for hydrocarbon growth on Fe55@C240.
Description
Keywords
116 Chemical sciences
Other note
Citation
Cilpa-Karhu , G & Laasonen , K 2018 , ' Computational exploration of Fe55@C240-catalyzed Fischer-Tropsch synthesis ' Physical Chemistry Chemical Physics , vol 20 , no. 4 , pp. 2741-2753 . DOI: 10.1039/C7CP06473J , 10.1039/c7cp06473j