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Carbon‐Supported Bimetallic Ruthenium‐Iridium Catalysts for Selective and Stable Hydrodebromination of Dibromomethane

Catalysts based on individual precious metals on carbon‐ and oxide‐based carriers have shown remarkably selective behavior in the hydrodebromination of CH(2)Br(2) to CH(3)Br, an important transformation within halogen‐mediated methane upgrading processes. However, the high susceptibility of the acti...

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Autores principales: Saadun, Ali J., Mitchell, Sharon, Bonchev, Hristo, Pérez‐Ramírez, Javier
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9300165/
https://www.ncbi.nlm.nih.gov/pubmed/35874462
http://dx.doi.org/10.1002/cctc.202101494
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author Saadun, Ali J.
Mitchell, Sharon
Bonchev, Hristo
Pérez‐Ramírez, Javier
author_facet Saadun, Ali J.
Mitchell, Sharon
Bonchev, Hristo
Pérez‐Ramírez, Javier
author_sort Saadun, Ali J.
collection PubMed
description Catalysts based on individual precious metals on carbon‐ and oxide‐based carriers have shown remarkably selective behavior in the hydrodebromination of CH(2)Br(2) to CH(3)Br, an important transformation within halogen‐mediated methane upgrading processes. However, the high susceptibility of the active phase to coking and to sintering, which cannot be overcome by controlling the nuclearity of the metal species, hinders their practical implementation. Herein, a platform of carbon‐supported Ir−Ru catalysts with distinct metal ratios at comparable metal nanoparticle size (ca. 1.0 nm) was adopted to systematically study the effects of a second metal on reactivity and stability. Catalytic tests reveal ruthenium‐doped iridium nanoparticles as the first system that combines high CH(3)Br selectivity (up to 93 %) with unprecedented stability, outperforming any of the previously reported catalysts. This superior performance was rationalized by the intimate interaction between the two metals, forming ruthenium‐poor surface alloys, which enable suppressing deactivation mechanisms as well as over hydrogenation/coking pathways.
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spelling pubmed-93001652022-07-21 Carbon‐Supported Bimetallic Ruthenium‐Iridium Catalysts for Selective and Stable Hydrodebromination of Dibromomethane Saadun, Ali J. Mitchell, Sharon Bonchev, Hristo Pérez‐Ramírez, Javier ChemCatChem Communications Catalysts based on individual precious metals on carbon‐ and oxide‐based carriers have shown remarkably selective behavior in the hydrodebromination of CH(2)Br(2) to CH(3)Br, an important transformation within halogen‐mediated methane upgrading processes. However, the high susceptibility of the active phase to coking and to sintering, which cannot be overcome by controlling the nuclearity of the metal species, hinders their practical implementation. Herein, a platform of carbon‐supported Ir−Ru catalysts with distinct metal ratios at comparable metal nanoparticle size (ca. 1.0 nm) was adopted to systematically study the effects of a second metal on reactivity and stability. Catalytic tests reveal ruthenium‐doped iridium nanoparticles as the first system that combines high CH(3)Br selectivity (up to 93 %) with unprecedented stability, outperforming any of the previously reported catalysts. This superior performance was rationalized by the intimate interaction between the two metals, forming ruthenium‐poor surface alloys, which enable suppressing deactivation mechanisms as well as over hydrogenation/coking pathways. John Wiley and Sons Inc. 2021-11-29 2022-01-21 /pmc/articles/PMC9300165/ /pubmed/35874462 http://dx.doi.org/10.1002/cctc.202101494 Text en © 2021 The Authors. ChemCatChem published by Wiley-VCH GmbH https://creativecommons.org/licenses/by-nc/4.0/This is an open access article under the terms of the http://creativecommons.org/licenses/by-nc/4.0/ (https://creativecommons.org/licenses/by-nc/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes.
spellingShingle Communications
Saadun, Ali J.
Mitchell, Sharon
Bonchev, Hristo
Pérez‐Ramírez, Javier
Carbon‐Supported Bimetallic Ruthenium‐Iridium Catalysts for Selective and Stable Hydrodebromination of Dibromomethane
title Carbon‐Supported Bimetallic Ruthenium‐Iridium Catalysts for Selective and Stable Hydrodebromination of Dibromomethane
title_full Carbon‐Supported Bimetallic Ruthenium‐Iridium Catalysts for Selective and Stable Hydrodebromination of Dibromomethane
title_fullStr Carbon‐Supported Bimetallic Ruthenium‐Iridium Catalysts for Selective and Stable Hydrodebromination of Dibromomethane
title_full_unstemmed Carbon‐Supported Bimetallic Ruthenium‐Iridium Catalysts for Selective and Stable Hydrodebromination of Dibromomethane
title_short Carbon‐Supported Bimetallic Ruthenium‐Iridium Catalysts for Selective and Stable Hydrodebromination of Dibromomethane
title_sort carbon‐supported bimetallic ruthenium‐iridium catalysts for selective and stable hydrodebromination of dibromomethane
topic Communications
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9300165/
https://www.ncbi.nlm.nih.gov/pubmed/35874462
http://dx.doi.org/10.1002/cctc.202101494
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