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Title: Structure and electronic properties of Ca-doped CeO{sub 2} and implications on catalytic activity: An experimental and theoretical study

Abstract

Doping CeO{sub 2} with for example, Ca gives an enhanced reactivity toward reduction of SO{sub 2} by CO, and total combustion of methane. Theoretical modeling using static minimizations and molecular dynamics (MD) simulations of the doped (110) face in combination with ab initio quantum chemical cluster models shows large effects on the Ce(IV)/Ce(III) balance due to the doping. Computed oxygen-to-cerium charge-transfer energies are strongly reduced as a result of the introduction of defects and oxygen vacancies, but not sufficiently to explain the observed reactivities. The structures resulting from the MD simulations for both the doped and undoped material are in good agreement with recent experimental pulsed neutron scattering results.

Authors:
; ;  [1]; ; ;  [2]; ;  [3]
  1. Stockholm Univ. (Sweden)
  2. Uppsala Univ. (Sweden)
  3. Royal Inst. of Tech., Stockholm (Sweden). Dept. of Materials Chemistry
Publication Date:
OSTI Identifier:
691299
Resource Type:
Journal Article
Journal Name:
Journal of Physical Chemistry B: Materials, Surfaces, Interfaces, amp Biophysical
Additional Journal Information:
Journal Volume: 103; Journal Issue: 36; Other Information: PBD: 9 Sep 1999
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 03 NATURAL GAS; 54 ENVIRONMENTAL SCIENCES; CERIUM OXIDES; CATALYSTS; CALCIUM COMPOUNDS; DOPED MATERIALS; THEORETICAL DATA; EXPERIMENTAL DATA; HETEROGENEOUS CATALYSIS

Citation Formats

Carolis, S. de, Pascual, J.L., Pettersson, L.G.M., Baudin, M., Wojcik, M., Hermansson, K., Palmqvist, A.E.C., and Muhammed, M. Structure and electronic properties of Ca-doped CeO{sub 2} and implications on catalytic activity: An experimental and theoretical study. United States: N. p., 1999. Web. doi:10.1021/jp983323e.
Carolis, S. de, Pascual, J.L., Pettersson, L.G.M., Baudin, M., Wojcik, M., Hermansson, K., Palmqvist, A.E.C., & Muhammed, M. Structure and electronic properties of Ca-doped CeO{sub 2} and implications on catalytic activity: An experimental and theoretical study. United States. doi:10.1021/jp983323e.
Carolis, S. de, Pascual, J.L., Pettersson, L.G.M., Baudin, M., Wojcik, M., Hermansson, K., Palmqvist, A.E.C., and Muhammed, M. Thu . "Structure and electronic properties of Ca-doped CeO{sub 2} and implications on catalytic activity: An experimental and theoretical study". United States. doi:10.1021/jp983323e.
@article{osti_691299,
title = {Structure and electronic properties of Ca-doped CeO{sub 2} and implications on catalytic activity: An experimental and theoretical study},
author = {Carolis, S. de and Pascual, J.L. and Pettersson, L.G.M. and Baudin, M. and Wojcik, M. and Hermansson, K. and Palmqvist, A.E.C. and Muhammed, M.},
abstractNote = {Doping CeO{sub 2} with for example, Ca gives an enhanced reactivity toward reduction of SO{sub 2} by CO, and total combustion of methane. Theoretical modeling using static minimizations and molecular dynamics (MD) simulations of the doped (110) face in combination with ab initio quantum chemical cluster models shows large effects on the Ce(IV)/Ce(III) balance due to the doping. Computed oxygen-to-cerium charge-transfer energies are strongly reduced as a result of the introduction of defects and oxygen vacancies, but not sufficiently to explain the observed reactivities. The structures resulting from the MD simulations for both the doped and undoped material are in good agreement with recent experimental pulsed neutron scattering results.},
doi = {10.1021/jp983323e},
journal = {Journal of Physical Chemistry B: Materials, Surfaces, Interfaces, amp Biophysical},
number = 36,
volume = 103,
place = {United States},
year = {1999},
month = {9}
}