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Title: 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:
 [1];  [1]; ORCiD logo [1]
  1. 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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1002/anie.201611796

Citation Metrics:
Cited by: 41 works
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