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Structure, Bonding and Chemistry of Water and Hydroxyl on Transition Metal Surfaces
Stockholms universitet, Naturvetenskapliga fakulteten, Fysikum.
2006 (engelsk)Doktoravhandling, med artikler (Annet vitenskapelig)
Abstract [en]

The structure, bonding and chemistry of water and hydroxyl on metal surfaces are presented. Synchrotron based x-ray photoelectron- and x-ray absorption spectroscopy along with density functional theory calculations mainly form the basis of the results. Conditions span the temperature range 35 - 520 K and pressures from ultra-high vacuum (~10 fAtm) to near ambient pressures (~1 mAtm). The results provide, e.g, new insights on the importance of hydrogen bonding for surface chemical kinetics.

Water adsorbs intact on the Pt(111), Ru(001) and Cu(110) surfaces at low temperatures forming 2-dimensional wetting layers where bonding to the metal (M) mainly occurs via H2O-M and M-HOH bonds. Observed isotope differences in structure and kinetics for H2O and D2O adsorption on Ru(001) are due to qualitatively different surface chemistries. D2O desorbs intact but H2O dissociates in kinetic competition with desorption similar to the D2O/Cu(110) system. The intact water layers are very sensitive to x-ray and electron induced damage.

The mixed H2O:OH phase on Ru(001) consists of stripe-like structures 4 to 6 Ru lattice parameters wide where OH decorates the edges of the stripes. On Pt(111), two different long-range ordered mixed H2O:OH structures are found to be inter-related by geometric distortions originating from the asymmetric H-bond donor-acceptor properties of OH towards H2O.

Water adsorption on Cu(110) was studied at near ambient conditions and compared to Cu(111). Whereas Cu(111) remains clean, Cu(110) holds significant amounts of water in a mixed H2O:OH layer. The difference is explained by the differing activation barriers for water dissociation, leading to the presence of OH groups on Cu(110) which lowers the desorption kinetics of water by orders of magnitude due to the formation of strong H2O-OH bonds. By lowering the activation barrier for water dissociation on Cu(111) by pre-adsorbing atomic O, generating adsorbed OH, similar results to those on Cu(110) are obtained.

sted, utgiver, år, opplag, sider
Stockholm: Fysikum , 2006. , s. 62
Emneord [en]
core-level spectroscopy, surface chemistry, water, hydroxyl, metal surfaces, adsorption, structure, hydrogen bonding
HSV kategori
Identifikatorer
URN: urn:nbn:se:su:diva-1246ISBN: 91-7155-318-5 (tryckt)OAI: oai:DiVA.org:su-1246DiVA, id: diva2:189691
Disputas
2006-09-26, sal FR4, AlbaNova universitetscentrum, Roslagstullsbacken 21, Stockholm, 10:00
Opponent
Veileder
Tilgjengelig fra: 2006-08-31 Laget: 2006-08-31 Sist oppdatert: 2010-12-21bibliografisk kontrollert
Delarbeid
1. Water dissociation on Ru(001): an activated process
Åpne denne publikasjonen i ny fane eller vindu >>Water dissociation on Ru(001): an activated process
Vise andre…
2004 Inngår i: Phys. Rev. Lett, Vol. 93, nr 196101Artikkel i tidsskrift (Fagfellevurdert) Published
Identifikatorer
urn:nbn:se:su:diva-22885 (URN)
Merknad
Part of urn:nbn:se:su:diva-1246Tilgjengelig fra: 2006-08-31 Laget: 2006-08-31bibliografisk kontrollert
2. Molecularly intact and dissociative adsorption of water on clean Cu(110): a comparison with the water/Ru(001) system
Åpne denne publikasjonen i ny fane eller vindu >>Molecularly intact and dissociative adsorption of water on clean Cu(110): a comparison with the water/Ru(001) system
Vise andre…
2005 Inngår i: Surf. Sci., Vol. 585, nr L183Artikkel i tidsskrift (Fagfellevurdert) Published
Identifikatorer
urn:nbn:se:su:diva-22886 (URN)
Merknad
Part of urn:nbn:se:su:diva-1246Tilgjengelig fra: 2006-08-31 Laget: 2006-08-31bibliografisk kontrollert
3. Structure of water adsorbed on the open Cu(110) surface: H-up, H-down, or both?
Åpne denne publikasjonen i ny fane eller vindu >>Structure of water adsorbed on the open Cu(110) surface: H-up, H-down, or both?
Vise andre…
2006 (engelsk)Inngår i: Chemical Physics Letters, ISSN 0009-2614, E-ISSN 1873-4448, Vol. 429, nr 4-6, s. 415-419Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

We investigated the structure of the water monolayer on an open surface, Cu(1 1 0), at low temperature. We found that water adsorbs molecularly, adopting a 2:1 ratio of H-down and H-up configurations. This behavior of water on an open surface is quite different to the behavior on close-packed surfaces, such as Pt(1 1 1) and Ru(0 0 0 1), where water adsorbs primarily H-down, but can be understood on the basis of a range of different water adsorption sites across the observed (7 × 8) unit cell.

HSV kategori
Identifikatorer
urn:nbn:se:su:diva-24765 (URN)10.1016/j.cplett.2006.08.048 (DOI)
Merknad
Part of urn:nbn:se:su:diva-7435Tilgjengelig fra: 2008-03-18 Laget: 2008-03-18 Sist oppdatert: 2017-12-13bibliografisk kontrollert
4. Structure and bonding of mixed water-hydroxyl phases on Pt(111)
Åpne denne publikasjonen i ny fane eller vindu >>Structure and bonding of mixed water-hydroxyl phases on Pt(111)
Vise andre…
Manuskript (Annet vitenskapelig)
Identifikatorer
urn:nbn:se:su:diva-22888 (URN)
Merknad
Part of urn:nbn:se:su:diva-1246Tilgjengelig fra: 2006-08-31 Laget: 2006-08-31 Sist oppdatert: 2010-01-13bibliografisk kontrollert
5. Structure and properties of mixed H2O:OH stripes on Ru(001)
Åpne denne publikasjonen i ny fane eller vindu >>Structure and properties of mixed H2O:OH stripes on Ru(001)
Vise andre…
Manuskript (Annet vitenskapelig)
Identifikatorer
urn:nbn:se:su:diva-22889 (URN)
Merknad
Part of urn:nbn:se:su:diva-1246Tilgjengelig fra: 2006-08-31 Laget: 2006-08-31 Sist oppdatert: 2010-01-13bibliografisk kontrollert
6. Water and hydroxyl surface chemistry on Cu(110) at near ambient pressures from in situ photoelectron spectroscopy studies
Åpne denne publikasjonen i ny fane eller vindu >>Water and hydroxyl surface chemistry on Cu(110) at near ambient pressures from in situ photoelectron spectroscopy studies
Vise andre…
Manuskript (Annet vitenskapelig)
Identifikatorer
urn:nbn:se:su:diva-22890 (URN)
Merknad
Part of urn:nbn:se:su:diva-1246Tilgjengelig fra: 2006-08-31 Laget: 2006-08-31 Sist oppdatert: 2010-01-13bibliografisk kontrollert
7. Different water chemistry on Cu(110) and Cu(111) at near ambient conditions
Åpne denne publikasjonen i ny fane eller vindu >>Different water chemistry on Cu(110) and Cu(111) at near ambient conditions
Vise andre…
Manuskript (Annet vitenskapelig)
Identifikatorer
urn:nbn:se:su:diva-22891 (URN)
Merknad
Part of urn:nbn:se:su:diva-1246Tilgjengelig fra: 2006-08-31 Laget: 2006-08-31 Sist oppdatert: 2010-01-13bibliografisk kontrollert

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