A multi-technique study of CO2 adsorption on Fe3O4 magnetite

The adsorption of CO2 on the Fe3O4(001)-( 2 × 2 )R45° surface was studied experimentally using temperature programmed desorption (TPD), photoelectron spectroscopies (UPS and XPS), and scanning tunneling microscopy. CO2 binds most strongly at defects related to Fe2+, including antiphase domain bounda...

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Published inThe Journal of chemical physics Vol. 146; no. 1
Main Authors Pavelec, Jiri, Hulva, Jan, Halwidl, Daniel, Bliem, Roland, Gamba, Oscar, Jakub, Zdenek, Brunbauer, Florian, Schmid, Michael, Diebold, Ulrike, Parkinson, Gareth S.
Format Journal Article
Published 07.01.2017
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Abstract The adsorption of CO2 on the Fe3O4(001)-( 2 × 2 )R45° surface was studied experimentally using temperature programmed desorption (TPD), photoelectron spectroscopies (UPS and XPS), and scanning tunneling microscopy. CO2 binds most strongly at defects related to Fe2+, including antiphase domain boundaries in the surface reconstruction and above incorporated Fe interstitials. At higher coverages,CO2 adsorbs at fivefold-coordinated Fe3+ sites with a binding energy of 0.4 eV. Above a coverage of 4 molecules per ( 2 × 2 )R45° unit cell, further adsorption results in a compression of the first monolayer up to a density approaching that of a CO2 ice layer. Surprisingly, desorption of the second monolayer occurs at a lower temperature (≈84 K) than CO2 multilayers (≈88 K), suggestive of a metastable phase or diffusion-limited island growth. The paper also discusses design considerations for a vacuum system optimized to study the surface chemistry of metal oxide single crystals, including the calibration and characterisation of a molecular beam source for quantitative TPD measurements.
AbstractList The adsorption of CO2 on the Fe3O4(001)-( 2 × 2 )R45° surface was studied experimentally using temperature programmed desorption (TPD), photoelectron spectroscopies (UPS and XPS), and scanning tunneling microscopy. CO2 binds most strongly at defects related to Fe2+, including antiphase domain boundaries in the surface reconstruction and above incorporated Fe interstitials. At higher coverages,CO2 adsorbs at fivefold-coordinated Fe3+ sites with a binding energy of 0.4 eV. Above a coverage of 4 molecules per ( 2 × 2 )R45° unit cell, further adsorption results in a compression of the first monolayer up to a density approaching that of a CO2 ice layer. Surprisingly, desorption of the second monolayer occurs at a lower temperature (≈84 K) than CO2 multilayers (≈88 K), suggestive of a metastable phase or diffusion-limited island growth. The paper also discusses design considerations for a vacuum system optimized to study the surface chemistry of metal oxide single crystals, including the calibration and characterisation of a molecular beam source for quantitative TPD measurements.
Author Diebold, Ulrike
Halwidl, Daniel
Parkinson, Gareth S.
Brunbauer, Florian
Hulva, Jan
Jakub, Zdenek
Gamba, Oscar
Bliem, Roland
Pavelec, Jiri
Schmid, Michael
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  organization: Institute of Applied Physics, TU Wien, Wiedner Hauptstrasse 8-10, 1050 Wien, Austria
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Snippet The adsorption of CO2 on the Fe3O4(001)-( 2 × 2 )R45° surface was studied experimentally using temperature programmed desorption (TPD), photoelectron...
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Title A multi-technique study of CO2 adsorption on Fe3O4 magnetite
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