Electride support boosts nitrogen dissociation over ruthenium catalyst and shifts the bottleneck in ammonia synthesis.
Author(s)
Type
Journal Article
Abstract
Novel approaches to efficient ammonia synthesis at an ambient pressure are actively sought out so as to reduce the cost of ammonia production and to allow for compact production facilities. It is accepted that the key is the development of a high-performance catalyst that significantly enhances dissociation of the nitrogen-nitrogen triple bond, which is generally considered a rate-determining step. Here we examine kinetics of nitrogen and hydrogen isotope exchange and hydrogen adsorption/desorption reactions for a recently discovered efficient catalyst for ammonia synthesis--ruthenium-loaded 12CaO·7Al2O3 electride (Ru/C12A7:e(-))--and find that the rate controlling step of ammonia synthesis over Ru/C12A7:e(-) is not dissociation of the nitrogen-nitrogen triple bond but the subsequent formation of N-Hn species. A mechanism of ammonia synthesis involving reversible storage and release of hydrogen atoms on the Ru/C12A7:e(-) surface is proposed on the basis of observed hydrogen absorption/desorption kinetics.
Date Issued
2015-03-30
Date Acceptance
2015-02-24
Citation
Nature Communications, 2015, 6
ISSN
2041-1723
Publisher
Nature Publishing Group: Nature Communications
Journal / Book Title
Nature Communications
Volume
6
Copyright Statement
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users will need to obtain permission from the license holder to reproduce the material.
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International License. The images or other third party material in this
article are included in the article’s Creative Commons license, unless indicated otherwise
in the credit line; if the material is not included under the Creative Commons license,
users will need to obtain permission from the license holder to reproduce the material.
To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
License URL
Identifier
PII: ncomms7731
Publication Status
Published