Catalytic Reaction Rates Controlled by Metal Oxidation State: C−H Bond Cleavage in Methane over Nickel‐Based Catalysts
Abstract
Abstract The role of low concentrations of carbon complexes in hydrocarbon decomposition over transition metal surfaces has been a topic of much debate over the past decades. It is also a mystery as to whether or not electric fields can enhance hydrocarbon conversion in an electrochemical device at lower than normal reforming temperatures. To provide a “bottom‐up” fundamental insight, C−H bond cleavage in methane over Ni‐based catalysts was investigated. Our theoretical results show that the presence of carbon or carbide‐like species at the interface between the Ni cluster and its metal‐oxide support, as well as the application of an external positive electric field, can significantly increase the Ni oxidation state. Furthermore, the first C−H bond cleavage in methane is favored as the local oxidation state of Ni increases. Thus, the presence of a low concentration of carbon species, or the addition of a positive electric field will improve the hydrocarbon activation process.
- Authors:
-
- The Gene and Linda Voiland School of Chemical Engineering and Bioengineering Washington State University Pullman WA 99164 USA
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1401761
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition) Journal Volume: 56 Journal Issue: 13; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Che, Fanglin, Ha, Su, and McEwen, Jean‐Sabin. Catalytic Reaction Rates Controlled by Metal Oxidation State: C−H Bond Cleavage in Methane over Nickel‐Based Catalysts. Germany: N. p., 2017.
Web. doi:10.1002/anie.201611796.
Che, Fanglin, Ha, Su, & McEwen, Jean‐Sabin. Catalytic Reaction Rates Controlled by Metal Oxidation State: C−H Bond Cleavage in Methane over Nickel‐Based Catalysts. Germany. https://doi.org/10.1002/anie.201611796
Che, Fanglin, Ha, Su, and McEwen, Jean‐Sabin. Mon .
"Catalytic Reaction Rates Controlled by Metal Oxidation State: C−H Bond Cleavage in Methane over Nickel‐Based Catalysts". Germany. https://doi.org/10.1002/anie.201611796.
@article{osti_1401761,
title = {Catalytic Reaction Rates Controlled by Metal Oxidation State: C−H Bond Cleavage in Methane over Nickel‐Based Catalysts},
author = {Che, Fanglin and Ha, Su and McEwen, Jean‐Sabin},
abstractNote = {Abstract The role of low concentrations of carbon complexes in hydrocarbon decomposition over transition metal surfaces has been a topic of much debate over the past decades. It is also a mystery as to whether or not electric fields can enhance hydrocarbon conversion in an electrochemical device at lower than normal reforming temperatures. To provide a “bottom‐up” fundamental insight, C−H bond cleavage in methane over Ni‐based catalysts was investigated. Our theoretical results show that the presence of carbon or carbide‐like species at the interface between the Ni cluster and its metal‐oxide support, as well as the application of an external positive electric field, can significantly increase the Ni oxidation state. Furthermore, the first C−H bond cleavage in methane is favored as the local oxidation state of Ni increases. Thus, the presence of a low concentration of carbon species, or the addition of a positive electric field will improve the hydrocarbon activation process.},
doi = {10.1002/anie.201611796},
journal = {Angewandte Chemie (International Edition)},
number = 13,
volume = 56,
place = {Germany},
year = {Mon Feb 27 00:00:00 EST 2017},
month = {Mon Feb 27 00:00:00 EST 2017}
}
https://doi.org/10.1002/anie.201611796
Web of Science
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