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High resolution spectroscopic and microscopic signatures of ordered growth of ferrous sulfate in SO2 assisted corrosion of Fe3O4(100)
KTH, School of Information and Communication Technology (ICT), Material Physics, Material Physics, MF.
KTH, School of Information and Communication Technology (ICT), Material Physics, Material Physics, MF.
KTH, School of Information and Communication Technology (ICT), Material Physics, Material Physics, MF.ORCID iD: 0000-0001-7409-575X
KTH, School of Information and Communication Technology (ICT), Material Physics, Material Physics, MF.
2007 (English)In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 91, no 9Article in journal (Refereed) Published
Abstract [en]

The authors present a high-resolution core-level photoemission study of a Fe3O4(100) surface exposed to 50 L (1 L=10(-6) mbar s) of H2O and 50 L of SO2. S 2p core-level spectra reveal the presence of SO3 and SO4 species. An additional peak in the Fe 3p core-level spectrum shows that they bond with iron from the substrate. Complementary scanning tunneling microscopy of the same surface demonstrates formation of a long-range ordered sulfate locked in the (root 2x root 2)R45 degrees-surface potential.

Place, publisher, year, edition, pages
2007. Vol. 91, no 9
Keyword [en]
scanning-tunneling-microscopy, sulfuric-acid-solution, in-situ, adsorbed sulfate, zno powders, adlayer, photoemission, electrodes, fe3o4(001), adsorption
National Category
Physical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-16921DOI: 10.1063/1.2776854ISI: 000249156100099Scopus ID: 2-s2.0-34548439418OAI: oai:DiVA.org:kth-16921DiVA: diva2:334964
Note

QC 20100525

Available from: 2010-08-05 Created: 2010-08-05 Last updated: 2013-01-16Bibliographically approved
In thesis
1. Surface Reactivity and Electronic Structure of Metal Oxides
Open this publication in new window or tab >>Surface Reactivity and Electronic Structure of Metal Oxides
2011 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The foci of this thesis are the metal oxides Cu2O, ZnO and Fe3O4 and their interaction with water and sulfur dioxide (SO2). The intention is to study SO2-induced atmospheric corrosion on a molecular level. All studies are based on photoelectron spectroscopy (PES) and scanning tunneling microscopy (STM) measurements. The band structure of Cu2O in the Γ-M direction has been probed by angle-resolved PES (ARPES). It reveals a more detailed picture of the bulk band structure than earlier data and gives the first experimental evidence of a dispersive hybridized Cu 3d-Cu 4s state. The experimental data is compared to band structure calculations. The structure of clean metal oxide surfaces and impact of sample preparation have been studied. Oxygen vacancies can form a (√3x√3)R30° reconstruction on Cu2O(111). Oxygen atoms adjacent to copper vacancies, steps or kinks are shown to be adsorption sites for both water and SO2. Annealing temperature influences the defect density and hydrogen content in ZnO, which can have large impact on the surface properties of ZnO(0001). Water is shown to adsorb dissociatively on ZnO(0001) and partly dissociatively on Cu2O(111). The dissociation occurs at undercoordinated oxygen sites on both surfaces. Water stays adsorbed on ZnO(0001) at room temperature but on Cu2O(111), all water has desorbed at 210 K. SO2 interacts with one or two undercoordinated O-sites on all studied oxide surfaces forming SO3 or SO4 species respectively. SO4 on Fe3O4(100) follows the (√2x√2)R45° reconstruction. On Cu2O(111) and ZnO(0001), SO2 adsorbs on defect sites. An SO3 to SO4 transition is observed on Cu2O(111) when heating an SO3 adsorbate layer from 150 K to 280K. Coadsorption of water and SO2 on ZnO(0001) and Fe3O4(100) has been studied briefly. Water blocks SO2 adsorption sites on ZnO(0001). On Fe3O4(100) and on one type of reduced ZnO(0001) sample, SO2 dissociation to atomic sulfur or sulfide occurs to a higher extent on water exposed surfaces than on clean surfaces. Water thus appears to increase the charge density on some surfaces. Further studies are needed to reveal the cause of this unexpected effect.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2011. xiv, 58 p.
Series
Trita-ICT/MAP AVH, ISSN 1653-7610 ; 2011:07
Keyword
oxides, surfaces, defects, cuprous oxide, zinc oxide, magnetite, water, OH, sulfur dioxide, photoelectron spectroscopy, scanning tunneling microscopy
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-33667 (URN)978-91-7415-995-0 (ISBN)
Public defence
2011-05-30, Electrum, C2, Isafjordsgatan 26, Kista, 10:00 (English)
Opponent
Supervisors
Note

QC 20110516

Available from: 2011-05-16 Created: 2011-05-13 Last updated: 2012-10-30Bibliographically approved

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Karlsson, Ulf O.

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