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Title: A new model describing the metal-support interaction in noble metal catalysts

Abstract

The catalytic activity and spectroscopic properties of supported noble metal catalysts are strongly influenced by the acidity/alkalinity of the support but are relatively independent of the metal (Pd or Pt) or the type of support (zeolite LTL or SiO{sub 2}). As the alkalinity of the support increases, the TOF of the metal particles for neopentane hydrogenolysis decreases. At the same time, there is a decrease in the XPS binding energy and a shift from linear to bridge bonded CO in the IR spectra. Analysis of the shape resonance in XANES spectra indicates that in the presence of chemisorbed hydrogen the difference in energy between the Pt-H antibonding orbital and the Fermi level decreases as the alkalinity of the support increases. Based on the results from the IR, XPS, and shape resonance data a new model is proposed in which the interaction between the metal and support leads to a shift in the energy of the metal valence orbitals. The EXAFS structural analysis indicates that the small metal particles are in contact only with the oxide ions of the support. Finally, a new spectroscopic characterization, Atomic XAFS, is presented which provides new insights into the origin of the electronic changes inmore » the metal. As the alkalinity of the support increases, there is decrease in the metal ionization potential. The primary interaction is a Coulomb attraction between metal particle and support oxygen ions, which affects the metal interatomic potential. This model for the metal-support interaction explicitly excludes the need for electron transfer, and it can account for all observed changes in the catalytic, electronic, and structural properties of the supported metal particles induced by support acidity ranging from acidic to neutral to alkaline.« less

Authors:
;  [1];  [2];  [3]
  1. Utrecht Univ. (Netherlands). Dept. of Inorganic Chemistry and Catalysis
  2. Amoco Research Center, Naperville, IL (United States)
  3. George Washington Univ., DC (United States). Chemistry Dept.
Publication Date:
OSTI Identifier:
687746
Resource Type:
Journal Article
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 186; Journal Issue: 2; Other Information: PBD: 10 Sep 1999
Country of Publication:
United States
Language:
English
Subject:
33 ADVANCED PROPULSION SYSTEMS; 02 PETROLEUM; CATALYSTS; CATALYST SUPPORTS; CONFIGURATION INTERACTION; MATHEMATICAL MODELS; PALLADIUM; PLATINUM; ZEOLITES; CATALYTIC CONVERTERS; NAPHTHA; CATALYTIC REFORMING

Citation Formats

Mojet, B.L., Koningsberger, D.C., Miller, J.T., and Ramaker, D.E. A new model describing the metal-support interaction in noble metal catalysts. United States: N. p., 1999. Web. doi:10.1006/jcat.1999.2568.
Mojet, B.L., Koningsberger, D.C., Miller, J.T., & Ramaker, D.E. A new model describing the metal-support interaction in noble metal catalysts. United States. doi:10.1006/jcat.1999.2568.
Mojet, B.L., Koningsberger, D.C., Miller, J.T., and Ramaker, D.E. Fri . "A new model describing the metal-support interaction in noble metal catalysts". United States. doi:10.1006/jcat.1999.2568.
@article{osti_687746,
title = {A new model describing the metal-support interaction in noble metal catalysts},
author = {Mojet, B.L. and Koningsberger, D.C. and Miller, J.T. and Ramaker, D.E.},
abstractNote = {The catalytic activity and spectroscopic properties of supported noble metal catalysts are strongly influenced by the acidity/alkalinity of the support but are relatively independent of the metal (Pd or Pt) or the type of support (zeolite LTL or SiO{sub 2}). As the alkalinity of the support increases, the TOF of the metal particles for neopentane hydrogenolysis decreases. At the same time, there is a decrease in the XPS binding energy and a shift from linear to bridge bonded CO in the IR spectra. Analysis of the shape resonance in XANES spectra indicates that in the presence of chemisorbed hydrogen the difference in energy between the Pt-H antibonding orbital and the Fermi level decreases as the alkalinity of the support increases. Based on the results from the IR, XPS, and shape resonance data a new model is proposed in which the interaction between the metal and support leads to a shift in the energy of the metal valence orbitals. The EXAFS structural analysis indicates that the small metal particles are in contact only with the oxide ions of the support. Finally, a new spectroscopic characterization, Atomic XAFS, is presented which provides new insights into the origin of the electronic changes in the metal. As the alkalinity of the support increases, there is decrease in the metal ionization potential. The primary interaction is a Coulomb attraction between metal particle and support oxygen ions, which affects the metal interatomic potential. This model for the metal-support interaction explicitly excludes the need for electron transfer, and it can account for all observed changes in the catalytic, electronic, and structural properties of the supported metal particles induced by support acidity ranging from acidic to neutral to alkaline.},
doi = {10.1006/jcat.1999.2568},
journal = {Journal of Catalysis},
number = 2,
volume = 186,
place = {United States},
year = {1999},
month = {9}
}