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Reactivity of CO2 on the surfaces of magnetite (Fe3O4), greigite (Fe3S4) and mackinawite (FeS).

Authors
  • Santos-Carballal, David1
  • Roldan, Alberto2
  • Dzade, Nelson Y3
  • de Leeuw, Nora H4, 3
  • 1 School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, UK [email protected]
  • 2 School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, UK.
  • 3 Department of Earth Sciences, Utrecht University, Budapestlaan 4, 3584 CD Utrecht, The Netherlands. , (Netherlands)
  • 4 School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, UK [email protected]
Type
Published Article
Journal
Philosophical Transactions of The Royal Society A Mathematical Physical and Engineering Sciences
Publisher
The Royal Society
Publication Date
Jan 13, 2018
Volume
376
Issue
2110
Identifiers
DOI: 10.1098/rsta.2017.0065
PMID: 29175834
Source
Medline
Keywords
License
Unknown

Abstract

The growing environmental, industrial and commercial interests in understanding the processes of carbon dioxide (CO2) capture and conversion have led us to simulate, by means of density functional theory calculations, the application of different iron oxide and sulfide minerals to capture, activate and catalytically dissociate this molecule. We have chosen the {001} and {111} surfaces of the spinel-structured magnetite (Fe3O4) and its isostructural sulfide counterpart greigite (Fe3S4), which are both materials with the Fe cations in the 2+/3+ mixed valence state, as well as mackinawite (tetragonal FeS), in which all iron ions are in the ferrous oxidation state. This selection of iron-bearing compounds provides us with understanding of the effect of the composition, stoichiometry, structure and oxidation state on the catalytic activation of CO2 The largest adsorption energies are released for the interaction with the Fe3O4 surfaces, which also corresponds to the biggest conformational changes of the CO2 molecule. Our results suggest that the Fe3S4 surfaces are unable to activate the CO2 molecule, while a major charge transfer takes place on FeS{111}, effectively activating the CO2 molecule. The thermodynamic and kinetic profiles for the catalytic dissociation of CO2 into CO and O show that this process is feasible only on the FeS{111} surface. The findings reported here show that these minerals show promise for future CO2 capture and conversion technologies, ensuring a sustainable future for society.This article is part of a discussion meeting issue 'Providing sustainable catalytic solutions for a rapidly changing world'.

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