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  Electron stimulated hydroxylation of a metal supported silicate film

Yu, X., Emmez, E., Pan, Q., Yang, B., Pomp, S., Kaden, W., et al. (2016). Electron stimulated hydroxylation of a metal supported silicate film. Physical Chemistry Chemical Physics, 18(5), 3755-3764. doi: 10.1039/C5CP06852E.

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 Creators:
Yu, Xin1, Author           
Emmez, Emre1, Author           
Pan, Qiushi1, Author           
Yang, Bing1, Author           
Pomp, Sascha1, 2, Author           
Kaden, William1, Author           
Sterrer, Martin1, 2, Author           
Shaikhutdinov, Shamil K.1, Author           
Freund, Hans-Joachim1, Author           
Goikoetxea, Itziar3, Author
Wlodarczyk, Radoslaw3, Author
Sauer, Joachim3, Author
Affiliations:
1Chemical Physics, Fritz Haber Institute, Max Planck Society, ou_24022              
2Institut für Physik, Universität Graz, Universitätsplatz 5, 8010 Graz, Austria , ou_persistent22              
3Institut für Chemie, Humboldt-Universität zu Berlin, Unter den Linden 6, 10099 Berlin, Germany , ou_persistent22              

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 Abstract: Water adsorption on a double-layer silicate film was studied by using infrared reflection–absorption spectroscopy, thermal desorption spectroscopy and scanning tunneling microscopy. Under vacuum conditions, small amounts of silanols (Si–OH) could only be formed upon deposition of an ice-like (amorphous solid water, ASW) film and subsequent heating to room temperature. Silanol coverage is considerably enhanced by low-energy electron irradiation of an ASW pre-covered silicate film. The degree of hydroxylation can be tuned by the irradiation parameters (beam energy, exposure) and the ASW film thickness. The results are consistent with a generally accepted picture that hydroxylation occurs through hydrolysis of siloxane (Si–O–Si) bonds in the silica network. Calculations using density functional theory show that this may happen on Si–O–Si bonds, which are either parallel (i.e., in the topmost silicate layer) or vertical to the film surface (i.e., connecting two silicate layers). In the latter case, the mechanism may additionally involve the reaction with a metal support underneath. The observed vibrational spectra are dominated by terminal silanol groups (ν(OD) band at 2763 cm−1) formed by hydrolysis of vertical Si–O–Si linkages. Film dehydroxylation fully occurs only upon heating to very high temperatures (∼1200 K) and is accompanied by substantial film restructuring, and even film dewetting upon cycling hydroxylation/dehydroxylation treatment.

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Language(s): eng - English
 Dates: 2015-11-092016-01-062016-01-062016-02-07
 Publication Status: Published in print
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1039/C5CP06852E
 Degree: -

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Project name : STRUBOLI - Structure and Bonding at Oxide-Liquid Interfaces
Grant ID : 280070
Funding program : Funding Programme 7 (FP7)
Funding organization : European Commission (EC)

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Title: Physical Chemistry Chemical Physics
  Abbreviation : Phys. Chem. Chem. Phys.
Source Genre: Journal
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Publ. Info: Cambridge, England : Royal Society of Chemistry
Pages: 10 Volume / Issue: 18 (5) Sequence Number: - Start / End Page: 3755 - 3764 Identifier: ISSN: 1463-9076
CoNE: https://pure.mpg.de/cone/journals/resource/954925272413_1