X-ray Photoelectron Spectroscopy and Kinetic Study: Pt-Group Metals and Bimetallic Surfaces

Abstract

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 Ptgroup 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.