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  Sites for Methane Activation on Lithium-Doped Magnesium Oxide Surfaces

Kwapien, K., Paier, J., Sauer, J., Geske, M., Zavyalova, U., Horn, R., et al. (2014). Sites for Methane Activation on Lithium-Doped Magnesium Oxide Surfaces. Angewandte Chemie International Edition, 53(33), 8774-8778. doi:10.1002/anie.201310632.

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Sauer-201310632-MS.pdf (Any fulltext), 330KB
 
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Kwapien, Karolina1, Author
Paier, Joachim1, Author
Sauer, Joachim1, Author
Geske, Michael2, Author           
Zavyalova, Ulyana2, Author           
Horn, Raimund2, 3, Author           
Schwach, Pierre2, Author           
Trunschke, Annette2, Author           
Schlögl, Robert2, Author           
Affiliations:
1Institut für Chemie, Humboldt-Universität, Unter den Linden 6, 10099 Berlin (Deutschland), ou_persistent22              
2Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
3Institut für Chemische Reaktionstechnik, Technische Universität Hamburg-Harburg (Deutschland), ou_persistent22              

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Free keywords: active sites; C[BOND]H activation; density functional calculations; Li-doped MgO; magnesium oxide
 Abstract: Density functional calculations yield energy barriers for H abstraction by oxygen radical sites in Li-doped MgO that are much smaller (12±6 kJ mol-1) than the barriers inferred from different experimental studies (80–160 kJ mol-1). This raises further doubts that the Li+O.- site is the active site as postulated by Lunsford. From temperature-programmed oxidative coupling reactions of methane (OCM), we conclude that the same sites are responsible for the activation of CH4 on both Li-doped MgO and pure MgO catalysts. For a MgO catalyst prepared by sol–gel synthesis, the activity proved to be very different in the initial phase of the OCM reaction and in the steady state. This was accompanied by substantial morphological changes and restructuring of the terminations as transmission electron microscopy revealed. Further calculations on cluster models showed that CH4 binds heterolytically on Mg2+O2- sites at steps and corners, and that the homolytic release of methyl radicals into the gas phase will happen only in the presence of O2.

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Language(s): eng - English
 Dates: 2014-02-192013-12-072014-042014-04-232014-08-11
 Publication Status: Published in print
 Pages: 5
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/anie.201310632
 Degree: -

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Title: Angewandte Chemie International Edition
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: - Volume / Issue: 53 (33) Sequence Number: - Start / End Page: 8774 - 8778 Identifier: ISSN: 0570-0833
CoNE: https://pure.mpg.de/cone/journals/resource/110984073528720