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The Effect of Copper Addition on the Activity and Stability of Iron-Based CO(2) Hydrogenation Catalysts

Iron-based CO(2) catalysts have shown promise as a viable route to the production of olefins from CO(2) and H(2) gas. However, these catalysts can suffer from low conversion and high methane selectivity, as well as being particularly vulnerable to water produced during the reaction. In an effort to...

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Autores principales: Bradley, Matthew J., Ananth, Ramagopal, Willauer, Heather D., Baldwin, Jeffrey W., Hardy, Dennis R., Williams, Frederick W.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6151512/
https://www.ncbi.nlm.nih.gov/pubmed/28930186
http://dx.doi.org/10.3390/molecules22091579
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author Bradley, Matthew J.
Ananth, Ramagopal
Willauer, Heather D.
Baldwin, Jeffrey W.
Hardy, Dennis R.
Williams, Frederick W.
author_facet Bradley, Matthew J.
Ananth, Ramagopal
Willauer, Heather D.
Baldwin, Jeffrey W.
Hardy, Dennis R.
Williams, Frederick W.
author_sort Bradley, Matthew J.
collection PubMed
description Iron-based CO(2) catalysts have shown promise as a viable route to the production of olefins from CO(2) and H(2) gas. However, these catalysts can suffer from low conversion and high methane selectivity, as well as being particularly vulnerable to water produced during the reaction. In an effort to improve both the activity and durability of iron-based catalysts on an alumina support, copper (10–30%) has been added to the catalyst matrix. In this paper, the effects of copper addition on the catalyst activity and morphology are examined. The addition of 10% copper significantly increases the CO(2) conversion, and decreases methane and carbon monoxide selectivity, without significantly altering the crystallinity and structure of the catalyst itself. The FeCu/K catalysts form an inverse spinel crystal phase that is independent of copper content and a metallic phase that increases in abundance with copper loading (>10% Cu). At higher loadings, copper separates from the iron oxide phase and produces metallic copper as shown by SEM-EDS. An addition of copper appears to increase the rate of the Fischer–Tropsch reaction step, as shown by modeling of the chemical kinetics and the inter- and intra-particle transport of mass and energy.
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spelling pubmed-61515122018-11-13 The Effect of Copper Addition on the Activity and Stability of Iron-Based CO(2) Hydrogenation Catalysts Bradley, Matthew J. Ananth, Ramagopal Willauer, Heather D. Baldwin, Jeffrey W. Hardy, Dennis R. Williams, Frederick W. Molecules Article Iron-based CO(2) catalysts have shown promise as a viable route to the production of olefins from CO(2) and H(2) gas. However, these catalysts can suffer from low conversion and high methane selectivity, as well as being particularly vulnerable to water produced during the reaction. In an effort to improve both the activity and durability of iron-based catalysts on an alumina support, copper (10–30%) has been added to the catalyst matrix. In this paper, the effects of copper addition on the catalyst activity and morphology are examined. The addition of 10% copper significantly increases the CO(2) conversion, and decreases methane and carbon monoxide selectivity, without significantly altering the crystallinity and structure of the catalyst itself. The FeCu/K catalysts form an inverse spinel crystal phase that is independent of copper content and a metallic phase that increases in abundance with copper loading (>10% Cu). At higher loadings, copper separates from the iron oxide phase and produces metallic copper as shown by SEM-EDS. An addition of copper appears to increase the rate of the Fischer–Tropsch reaction step, as shown by modeling of the chemical kinetics and the inter- and intra-particle transport of mass and energy. MDPI 2017-09-20 /pmc/articles/PMC6151512/ /pubmed/28930186 http://dx.doi.org/10.3390/molecules22091579 Text en © 2017 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Bradley, Matthew J.
Ananth, Ramagopal
Willauer, Heather D.
Baldwin, Jeffrey W.
Hardy, Dennis R.
Williams, Frederick W.
The Effect of Copper Addition on the Activity and Stability of Iron-Based CO(2) Hydrogenation Catalysts
title The Effect of Copper Addition on the Activity and Stability of Iron-Based CO(2) Hydrogenation Catalysts
title_full The Effect of Copper Addition on the Activity and Stability of Iron-Based CO(2) Hydrogenation Catalysts
title_fullStr The Effect of Copper Addition on the Activity and Stability of Iron-Based CO(2) Hydrogenation Catalysts
title_full_unstemmed The Effect of Copper Addition on the Activity and Stability of Iron-Based CO(2) Hydrogenation Catalysts
title_short The Effect of Copper Addition on the Activity and Stability of Iron-Based CO(2) Hydrogenation Catalysts
title_sort effect of copper addition on the activity and stability of iron-based co(2) hydrogenation catalysts
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6151512/
https://www.ncbi.nlm.nih.gov/pubmed/28930186
http://dx.doi.org/10.3390/molecules22091579
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