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Water-Metal Surfaces: Insights from core-level spectroscopy and density functional theory
Stockholm University, Faculty of Science, Department of Physics.
2008 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Computational methods are combined with synchrotron-based techniques to analyze the structure and bonding of water and water plus hydroxyl at metal surfaces under UHV and at near-ambient conditions. Water-metal interaction plays a crucial role in a multitude of cosmic, atmospheric and biological phenomena as well as heterogeneous catalysis, electrochemistry and corrosion. A spotlight of renewed interest has recently been cast on water-metal systems due to their relevance for surface chemical reactions related to the production and utilization of hydrogen as a clean energy carrier. In particular, H2O and OH are essential reaction intermediates in the renewable production of hydrogen from sunlight and water and in fuel cell electrocatalysis.

Fuel cells are considered one of the most promising power generation technologies for a sustainable energy future. A mechanistic understanding of the oxygen reduction reaction (ORR) pathway, including the role of electronic and geometric structure of the catalyst, is essential to the design of more efficient fuel cell catalysts. This is intimately connected to fundamental factors that affect the ability to form water-metal bonds as well as the site occupation and orientation of the adsorbed H2O and OH at active metal surfaces.

Key relationships related to critical issues in the fuel cell reaction are illuminated by the synergy of theory and experiment in this thesis. We emerge with a detailed understanding of the structure of the water-metal interface and the factors that rule the wettability of a metal surface, including geometric and electronic structure effects and the influence of coadsorbed species. We show that the preferred microscopic orientation of the water monolayer has consequences for macroscopic properties, and reveal the origin of the hydrophobic water layer. Finally, we identify a cooperativity effect that drives the stability of the mixed water/hydroxyl layer at metal surfaces, an important ORR intermediate.

Place, publisher, year, edition, pages
Stockholm: Fysikum , 2008. , 74 p.
Keyword [en]
water, hydroxyl, metal, surfaces, x-ray spectroscopy, density functional theory, bonding, fuel cell
Research subject
Chemical Physics
Identifiers
URN: urn:nbn:se:su:diva-7435ISBN: 978-91-7155-607-3 (print)OAI: oai:DiVA.org:su-7435DiVA: diva2:198277
Public defence
2008-04-17, sal FB42, AlbaNova universitetscentrum, Roslagstullsbacken 21, Stockholm, 10:00
Opponent
Supervisors
Available from: 2008-03-18 Created: 2008-03-18Bibliographically approved
List of papers
1. The Role of Electronic and Geometric Structure in Bonding of Water to Metals
Open this publication in new window or tab >>The Role of Electronic and Geometric Structure in Bonding of Water to Metals
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Manuscript (Other academic)
Identifiers
urn:nbn:se:su:diva-24763 (URN)
Note
Part of urn:nbn:se:su:diva-7435Available from: 2008-03-18 Created: 2008-03-18 Last updated: 2010-01-13Bibliographically approved
2. Unique Water-Water Coordination Tailored by a Metal Surface
Open this publication in new window or tab >>Unique Water-Water Coordination Tailored by a Metal Surface
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Manuscript (Other academic)
Identifiers
urn:nbn:se:su:diva-24764 (URN)
Note
Part of urn:nbn:se:su:diva-7435Available from: 2008-03-18 Created: 2008-03-18 Last updated: 2010-01-13Bibliographically approved
3. Structure of water adsorbed on the open Cu(110) surface: H-up, H-down, or both?
Open this publication in new window or tab >>Structure of water adsorbed on the open Cu(110) surface: H-up, H-down, or both?
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2006 (English)In: Chemical Physics Letters, ISSN 0009-2614, E-ISSN 1873-4448, Vol. 429, no 4-6, 415-419 p.Article in journal (Refereed) 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.

National Category
Physical Sciences
Identifiers
urn:nbn:se:su:diva-24765 (URN)10.1016/j.cplett.2006.08.048 (DOI)
Note
Part of urn:nbn:se:su:diva-7435Available from: 2008-03-18 Created: 2008-03-18 Last updated: 2010-12-21Bibliographically approved
4. When Water Isn't Wet: Origin of the Hydrophobic Monolayer
Open this publication in new window or tab >>When Water Isn't Wet: Origin of the Hydrophobic Monolayer
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Manuscript (Other academic)
Identifiers
urn:nbn:se:su:diva-24766 (URN)
Note
Part of urn:nbn:se:su:diva-7435Available from: 2008-03-18 Created: 2008-03-18 Last updated: 2010-01-13Bibliographically approved
5. Hydroxyl-Induced Wetting of Metals by Water at Near-Ambient Conditions
Open this publication in new window or tab >>Hydroxyl-Induced Wetting of Metals by Water at Near-Ambient Conditions
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2007 In: The Journal of Physical Chemistry C, ISSN 1932-7447, Vol. 111, 7848-7850 p.Article in journal (Refereed) Published
Identifiers
urn:nbn:se:su:diva-24767 (URN)
Note
Part of urn:nbn:se:su:diva-7435Available from: 2008-03-18 Created: 2008-03-18Bibliographically approved
6. Structure and Bonding of the Water-Hydroxyl Mixed Phase on Pt(111)
Open this publication in new window or tab >>Structure and Bonding of the Water-Hydroxyl Mixed Phase on Pt(111)
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2007 In: Journal of Physical Chemistry C, ISSN 1932-7447, Vol. 111, no 41, 15003-15012 p.Article in journal (Refereed) Published
Identifiers
urn:nbn:se:su:diva-24768 (URN)000250142300013 ()
Note
Part of urn:nbn:se:su:diva-7435Available from: 2008-03-18 Created: 2008-03-18Bibliographically approved
7. Cooperativity effect in surface and hydrogen bonding for the OH+H2O mixed layer at metal surfaces
Open this publication in new window or tab >>Cooperativity effect in surface and hydrogen bonding for the OH+H2O mixed layer at metal surfaces
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Manuscript (Other academic)
Identifiers
urn:nbn:se:su:diva-24769 (URN)
Note
Part of urn:nbn:se:su:diva-7435Available from: 2008-03-18 Created: 2008-03-18 Last updated: 2010-01-13Bibliographically approved

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