Electronic band contraction induced low temperature methane activation on metal alloys
Abstract
The catalytic conversion of methane under mild conditions is an appealing approach to selectively produce value-added products from natural gas. Catalysts which can chemisorb methane can potentially overcome challenges associated with its high stability and achieve facile activation. Although transition metals can activate C–H bonds, chemisorption and low-temperature conversion remain elusive on these surfaces. The broad electronic bands of metals can only weakly interact with the methane orbitals, in contrast to specific transition metal oxide and supported metal cluster surfaces which are now recognized to form methane σ-complexes. Here, we report methane chemisorption can, remarkably, occur on metal surfaces via electronic band contraction and localization from metal alloying. From a broad screening including single atom and intermetallic alloys in various substrates, we find early transition metals as promising metal solutes for methane chemisorption and low-temperature activation. These findings demonstrate a combinatorial diversity of possible candidates in earth abundant metal alloys with this attractive catalytic behavior.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1615207
- Alternate Identifier(s):
- OSTI ID: 1604482
- Grant/Contract Number:
- AC05-00OR22725; SC0012577; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Materials Chemistry. A
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 12; Journal ID: ISSN 2050-7488
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Fung, Victor, Hu, Guoxiang, and Sumpter, Bobby. Electronic band contraction induced low temperature methane activation on metal alloys. United States: N. p., 2020.
Web. doi:10.1039/D0TA00375A.
Fung, Victor, Hu, Guoxiang, & Sumpter, Bobby. Electronic band contraction induced low temperature methane activation on metal alloys. United States. https://doi.org/10.1039/D0TA00375A
Fung, Victor, Hu, Guoxiang, and Sumpter, Bobby. Mon .
"Electronic band contraction induced low temperature methane activation on metal alloys". United States. https://doi.org/10.1039/D0TA00375A. https://www.osti.gov/servlets/purl/1615207.
@article{osti_1615207,
title = {Electronic band contraction induced low temperature methane activation on metal alloys},
author = {Fung, Victor and Hu, Guoxiang and Sumpter, Bobby},
abstractNote = {The catalytic conversion of methane under mild conditions is an appealing approach to selectively produce value-added products from natural gas. Catalysts which can chemisorb methane can potentially overcome challenges associated with its high stability and achieve facile activation. Although transition metals can activate C–H bonds, chemisorption and low-temperature conversion remain elusive on these surfaces. The broad electronic bands of metals can only weakly interact with the methane orbitals, in contrast to specific transition metal oxide and supported metal cluster surfaces which are now recognized to form methane σ-complexes. Here, we report methane chemisorption can, remarkably, occur on metal surfaces via electronic band contraction and localization from metal alloying. From a broad screening including single atom and intermetallic alloys in various substrates, we find early transition metals as promising metal solutes for methane chemisorption and low-temperature activation. These findings demonstrate a combinatorial diversity of possible candidates in earth abundant metal alloys with this attractive catalytic behavior.},
doi = {10.1039/D0TA00375A},
journal = {Journal of Materials Chemistry. A},
number = 12,
volume = 8,
place = {United States},
year = {Mon Feb 24 00:00:00 EST 2020},
month = {Mon Feb 24 00:00:00 EST 2020}
}
Web of Science
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