Experimental and computational studies of silicon-oxygen bonding structures on metal surfaces

2008 2008

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Abstract (summary)

A different approach to modeling metal-metal oxide chemistry has been attempted. Specifically, the chemistry of Pd, Pt and silica is of concern. The chemistry of Si, O and metal atoms has been studied through the deposition of thin layers of Si and O on the order of one monolayer thick onto Pd(111) and Pt(111). Studies were done through a combination of experimental and computational efforts.

Si chemistry on Pd(111) was studied through the adsorption and reaction of SiH4. Dissociative adsorption to a SiHX surface species was observed through high resolution electron energy loss spectroscopy (HREELS), occurring at 200 K. Complete dissociation occurs above 250 K. Pd-silicide formation is suggested above 500 K.

Si-O bonding on Pd(111) was studied through the adsorption and reaction of SiH4 and O2. The Si-O bonding structure formed on Pd(111) revealed through HREEL spectra indicates a silica-like structure that is thermally stable. The structure measured by HREELS after high temperature treatment appeared to be largely independent of beginning Si and O coverages. Auger electron spectroscopy (AES) results also show evidence of Si-O bonding consistent with a Si suboxide. Temperature programmed desorption (TPD) studies indicate the structure formed by high temperature treatment seemed to act only as a site blocker to H2 and CO. However, structures observed prior to high temperature treatment showed a higher H2 desorption temperature than the clean Pd(111) surface.

Comparisons of SiH4 and O2 adsorption and reaction chemistry on Pt(111) to the same chemistry on Pd(111) revealed a greatly different result. No silica-like layers were indicated, however, Si-O bond vibrations were present in HREEL spectra. Furthermore, no perturbed H2 TPD spectra were observed.

However, density functional theory (DFT) results reveal Si-O species possessing vibration modes similar to those observed on Pt(111). Similarities between the results on Pt(111) and the low coverage structures simulated using DFT suggest higher Si and O coverages were achieved on Pd(111). DFT results also showed a Si-O bonding structure continuous across the simulated metal surfaces. This structure consisted of Si atoms bound to the metal surface with O atoms bridging the Si atoms.

Indexing (details)

Chemical engineering
0542: Chemical engineering
Identifier / keyword
Applied sciences; Density functional theory; Interfacial chemistry model; Metal-metal oxide chemistry; Silicon oxidation; Silicon-oxygen bonding; Surface science; Ultrahigh vacuum
Experimental and computational studies of silicon-oxygen bonding structures on metal surfaces
Kershner, Dylan C.
Number of pages
Publication year
Degree date
School code
DAI-B 69/07, Dissertation Abstracts International
Place of publication
Ann Arbor
Country of publication
United States
Medlin, J. W.
Committee member
Falconer, John L.; George, Steven; Schwartz, Daniel; Stoldt, Conrad
University of Colorado at Boulder
Chemical Engineering
University location
United States -- Colorado
Source type
Dissertations & Theses
Document type
Dissertation/thesis number
ProQuest document ID
Database copyright ProQuest LLC; ProQuest does not claim copyright in the individual underlying works.
Document URL
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