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X-ray photoelectron spectroscopy and kinetic study: Platinum-group metals and bimetallic surfaces

Posted on:2009-06-04Degree:Ph.DType:Dissertation
University:Texas A&M UniversityCandidate:Gath, Kerrie KFull Text:PDF
GTID:1441390005459143Subject:Chemistry
Abstract/Summary:
Pt-group metals were some of the first metals to be studied as catalysts for industrial use. The goal of these studies was to ascertain a fundamental understanding of CO oxidation and acetylene cyclotrimerization reactions on Pt-group metals. A further goal was to determine the optimal conditions for each reaction.;CO oxidation on Rh(111), Pt(100), and Pd(100) was scrutinized on various oxide surfaces from chemisorbed to bulk metal oxides. Low pressure reactions on Rh(111) reveal the highest activity was a CO uninhibited surface with <1ML of chemisorbed oxygen. Pt(100) high pressure oxidation revealed that only <1ML oxygen is formed during high pressures reactions. High pressure CO oxidation reactions on Pd(100) show oxygen penetration after CO has been consumed; however, during the highest activity XPS found only chemisorbed species.;The cyclotrimerization of acetylene to benzene is another reaction found in industry typically carried out on Pd. The active site is considered to be a 7 atom configuration with 6 atoms surrounding a central atom. By adding relatively catalytically inert Au atoms to the active Pd(111) surface the acetylene coupling activity is enhanced. Cyclization activity is a function of the surface composition and the surface structure. A single Pd atom surrounded by six Au atoms is found to have the highest activity at 300K for acetylene cyclotrimerization.
Keywords/Search Tags:Metals, CO oxidation, Highest activity, Surface, Acetylene
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