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Pd-C Catalytic Thin Films Prepared by Magnetron Sputtering for the Decomposition of Formic Acid

Formic acid is an advantageous liquid organic hydrogen carrier. It is relatively nontoxic and can be synthesized by the reaction of CO(2) with sustainable hydrogen or by biomass decomposition. As an alternative to more widely studied powdery catalysts, supported Pd-C catalytic thin films with contro...

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Autores principales: Arzac, Gisela Mariana, Fernández, Asunción, Godinho, Vanda, Hufschmidt, Dirk, Jiménez de Haro, Maria Carmen, Medrán, Beatriz, Montes, Olga
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8466502/
https://www.ncbi.nlm.nih.gov/pubmed/34578642
http://dx.doi.org/10.3390/nano11092326
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author Arzac, Gisela Mariana
Fernández, Asunción
Godinho, Vanda
Hufschmidt, Dirk
Jiménez de Haro, Maria Carmen
Medrán, Beatriz
Montes, Olga
author_facet Arzac, Gisela Mariana
Fernández, Asunción
Godinho, Vanda
Hufschmidt, Dirk
Jiménez de Haro, Maria Carmen
Medrán, Beatriz
Montes, Olga
author_sort Arzac, Gisela Mariana
collection PubMed
description Formic acid is an advantageous liquid organic hydrogen carrier. It is relatively nontoxic and can be synthesized by the reaction of CO(2) with sustainable hydrogen or by biomass decomposition. As an alternative to more widely studied powdery catalysts, supported Pd-C catalytic thin films with controlled nanostructure and compositions were newly prepared in this work by magnetron sputtering on structured supports and tested for the formic acid decomposition reaction. A two-magnetron configuration (carbon and tailored Pd-C targets) was used to achieve a reduction in Pd consumption and high catalyst surface roughness and dispersion by increasing the carbon content. Activity and durability tests were carried out for the gas phase formic acid decomposition reaction on SiC foam monoliths coated with the Pd-C films and the effects of column width, surface roughness and thermal pre-reduction time were investigated. Activity of 5.04 mol(H2)·g(Pd)(−1)·h(−1) and 92% selectivity to the dehydrogenation reaction were achieved at 300 °C for the catalyst with a lower column width and higher carbon content and surface roughness. It was also found that deactivation occurs when Pd is sintered due to the elimination of carbon and/or the segregation and agglomeration of Pd upon cycling. Magnetron sputtering deposition appears as a promising and scalable route for the one-step preparation of Pd-C catalytic films by overcoming the different deposition characteristics of Pd and C with an appropriate experimental design.
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spelling pubmed-84665022021-09-27 Pd-C Catalytic Thin Films Prepared by Magnetron Sputtering for the Decomposition of Formic Acid Arzac, Gisela Mariana Fernández, Asunción Godinho, Vanda Hufschmidt, Dirk Jiménez de Haro, Maria Carmen Medrán, Beatriz Montes, Olga Nanomaterials (Basel) Article Formic acid is an advantageous liquid organic hydrogen carrier. It is relatively nontoxic and can be synthesized by the reaction of CO(2) with sustainable hydrogen or by biomass decomposition. As an alternative to more widely studied powdery catalysts, supported Pd-C catalytic thin films with controlled nanostructure and compositions were newly prepared in this work by magnetron sputtering on structured supports and tested for the formic acid decomposition reaction. A two-magnetron configuration (carbon and tailored Pd-C targets) was used to achieve a reduction in Pd consumption and high catalyst surface roughness and dispersion by increasing the carbon content. Activity and durability tests were carried out for the gas phase formic acid decomposition reaction on SiC foam monoliths coated with the Pd-C films and the effects of column width, surface roughness and thermal pre-reduction time were investigated. Activity of 5.04 mol(H2)·g(Pd)(−1)·h(−1) and 92% selectivity to the dehydrogenation reaction were achieved at 300 °C for the catalyst with a lower column width and higher carbon content and surface roughness. It was also found that deactivation occurs when Pd is sintered due to the elimination of carbon and/or the segregation and agglomeration of Pd upon cycling. Magnetron sputtering deposition appears as a promising and scalable route for the one-step preparation of Pd-C catalytic films by overcoming the different deposition characteristics of Pd and C with an appropriate experimental design. MDPI 2021-09-07 /pmc/articles/PMC8466502/ /pubmed/34578642 http://dx.doi.org/10.3390/nano11092326 Text en © 2021 by the authors. https://creativecommons.org/licenses/by/4.0/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 (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Arzac, Gisela Mariana
Fernández, Asunción
Godinho, Vanda
Hufschmidt, Dirk
Jiménez de Haro, Maria Carmen
Medrán, Beatriz
Montes, Olga
Pd-C Catalytic Thin Films Prepared by Magnetron Sputtering for the Decomposition of Formic Acid
title Pd-C Catalytic Thin Films Prepared by Magnetron Sputtering for the Decomposition of Formic Acid
title_full Pd-C Catalytic Thin Films Prepared by Magnetron Sputtering for the Decomposition of Formic Acid
title_fullStr Pd-C Catalytic Thin Films Prepared by Magnetron Sputtering for the Decomposition of Formic Acid
title_full_unstemmed Pd-C Catalytic Thin Films Prepared by Magnetron Sputtering for the Decomposition of Formic Acid
title_short Pd-C Catalytic Thin Films Prepared by Magnetron Sputtering for the Decomposition of Formic Acid
title_sort pd-c catalytic thin films prepared by magnetron sputtering for the decomposition of formic acid
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8466502/
https://www.ncbi.nlm.nih.gov/pubmed/34578642
http://dx.doi.org/10.3390/nano11092326
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