English
 
Help Privacy Policy Disclaimer
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT
  Toward an Understanding of Selective Alkyne Hydrogenation on Ceria: On the Impact of O Vacancies on H2 Interaction with CeO2(111)

Werner, K., Weng, X., Calaza, F., Sterrer, M., Kropp, T., Paier, J., et al. (2017). Toward an Understanding of Selective Alkyne Hydrogenation on Ceria: On the Impact of O Vacancies on H2 Interaction with CeO2(111). Journal of the American Chemical Society, 139(48), 17608-17616. doi:10.1021/jacs.7b10021.

Item is

Files

show Files
hide Files
:
2518052.pdf (Any fulltext), 2MB
 
File Permalink:
-
Name:
2518052.pdf
Description:
-
Visibility:
Private
MIME-Type / Checksum:
application/pdf
Technical Metadata:
Copyright Date:
2017
Copyright Info:
ACS
License:
-

Locators

show

Creators

show
hide
 Creators:
Werner, Kristin1, Author              
Weng, Xuefei1, Author              
Calaza, Florencia1, 2, Author              
Sterrer, Martin3, Author
Kropp, Thomas4, Author
Paier, Joachim4, Author
Sauer, Joachim4, Author
Wilde, Markus5, Author
Fukutani, Katsuyuki5, Author
Shaikhutdinov, Shamil K.1, Author              
Freund, Hans-Joachim1, Author              
Affiliations:
1Chemical Physics, Fritz Haber Institute, Max Planck Society, ou_24022              
2Instituto de Desarrollo Tecnológico para la Industria Química (INTEC), UNL-CONICET, Güemes 3450, 3000 Santa Fe, Argentina, ou_persistent22              
3Institute of Physics, University of Graz, NAWI Graz, Universitätsplatz 5, 8010 Graz, Austria, ou_persistent22              
4Institut für Chemie, Humboldt-Universität, Unter den Linden 6, 10099 Berlin, Germany, ou_persistent22              
5Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro-ku, 153-8505 Tokyo, Japan, ou_persistent22              

Content

show
hide
Free keywords: -
 Abstract: Ceria (CeO2) has recently been found to be a promising catalyst in the selective hydrogenation of alkynes to alkenes. This reaction occurs primarily on highly dispersed metal catalysts, but rarely on oxide surfaces. The origin of the outstanding activity and selectivity observed on CeO2 remains unclear. In this work, we show that one key aspect of the hydrogenation reaction—the interaction of hydrogen with the oxide—depends strongly on the presence of O vacancies within CeO2. Through infrared reflection absorption spectroscopy on well-ordered CeO2(111) thin films and density functional theory (DFT) calculations, we show that the preferred heterolytic dissociation of molecular hydrogen on CeO2(111) requires H2 pressures in the mbar regime. Hydrogen depth profiling with nuclear reaction analysis indicates that H species stay on the surface of stoichiometric CeO2(111) films, whereas H incorporates as a volatile species into the volume of partially reduced CeO2–x(111) thin films (x ∼ 1.8–1.9). Complementary DFT calculations demonstrate that oxygen vacancies facilitate H incorporation below the surface and that they are the key to the stabilization of hydridic H species in the volume of reduced ceria.

Details

show
hide
Language(s): eng - English
 Dates: 2017-09-192017-11-132017-12-06
 Publication Status: Published in print
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/jacs.7b10021
 Degree: -

Event

show

Legal Case

show

Project information

show

Source 1

show
hide
Title: Journal of the American Chemical Society
  Other : J. Am. Chem. Soc.
  Abbreviation : JACS
Source Genre: Journal
 Creator(s):
Affiliations:
Publ. Info: Washington, DC : American Chemical Society
Pages: 9 Volume / Issue: 139 (48) Sequence Number: - Start / End Page: 17608 - 17616 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870