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High Catalytic Efficiency of a Nanosized Copper-Based Catalyst for Automotives: A Physicochemical Characterization

The global trend in restrictions on pollutant emissions requires the use of catalytic converters in the automotive industry. Noble metals belonging to the platinum group metals (PGMs, platinum, palladium, and rhodium) are currently used for autocatalysts. However, recent efforts focus on the develop...

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Autores principales: Soto Beobide, Amaia, Moschovi, Anastasia M., Mathioudakis, Georgios N., Kourtelesis, Marios, Lada, Zoi G., Andrikopoulos, Konstantinos S., Sygellou, Labrini, Dracopoulos, Vassilios, Yakoumis, Iakovos, Voyiatzis, George A.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9657973/
https://www.ncbi.nlm.nih.gov/pubmed/36364229
http://dx.doi.org/10.3390/molecules27217402
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author Soto Beobide, Amaia
Moschovi, Anastasia M.
Mathioudakis, Georgios N.
Kourtelesis, Marios
Lada, Zoi G.
Andrikopoulos, Konstantinos S.
Sygellou, Labrini
Dracopoulos, Vassilios
Yakoumis, Iakovos
Voyiatzis, George A.
author_facet Soto Beobide, Amaia
Moschovi, Anastasia M.
Mathioudakis, Georgios N.
Kourtelesis, Marios
Lada, Zoi G.
Andrikopoulos, Konstantinos S.
Sygellou, Labrini
Dracopoulos, Vassilios
Yakoumis, Iakovos
Voyiatzis, George A.
author_sort Soto Beobide, Amaia
collection PubMed
description The global trend in restrictions on pollutant emissions requires the use of catalytic converters in the automotive industry. Noble metals belonging to the platinum group metals (PGMs, platinum, palladium, and rhodium) are currently used for autocatalysts. However, recent efforts focus on the development of new catalytic converters that combine high activity and reduced cost, attracting the interest of the automotive industry. Among them, the partial substitution of PGMs by abundant non-PGMs (transition metals such as copper) seems to be a promising alternative. The PROMETHEUS catalyst (PROM100) is a polymetallic nanosized copper-based catalyst for automotives prepared by a wet impregnation method, using as a carrier an inorganic mixed oxide (CeO(2)-ZrO(2)) exhibiting elevated oxygen storage capacity. On the other hand, catalyst deactivation or ageing is defined as the process in which the structure and state of the catalyst change, leading to the loss of the catalyst’s active sites with a subsequent decrease in the catalyst’s performance, significantly affecting the emissions of the catalyst. The main scope of this research is to investigate in detail the effect of ageing on this low-cost, effective catalyst. To that end, a detailed characterization has been performed with a train of methods, such as SEM, Raman, XRD, XRF, BET and XPS, to both ceria–zirconia mixed inorganic oxide support (CZ-fresh and -aged) and to the copper-based catalyst (PROM100-fresh and -aged), revealing the impact of ageing on catalytic efficiency. It was found that ageing affects the Ce–Zr mixed oxide structure by initiating the formation of distinct ZrO(2) and CeO(2) structures monitored by Raman and XRD. In addition, it crucially affects the morphology of the sample by reducing the surface area by a factor of nearly two orders of magnitude and increasing particle size as indicated by BET and SEM due to sintering. Finally, the Pd concentration was found to be considerably reduced from the material’s surface as suggested by XPS data. The above-mentioned alterations observed after ageing increased the light-off temperatures by more than 175 °C, compared to the fresh sample, without affecting the overall efficiency of the catalyst for CO and CH(4) oxidation reactions. Metal particle and CeZr carrier sintering, washcoat loss as well as partial metal encapsulation by Cu and/or CeZrO(4) are identified as the main causes for the deactivation after hydrothermal ageing.
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spelling pubmed-96579732022-11-15 High Catalytic Efficiency of a Nanosized Copper-Based Catalyst for Automotives: A Physicochemical Characterization Soto Beobide, Amaia Moschovi, Anastasia M. Mathioudakis, Georgios N. Kourtelesis, Marios Lada, Zoi G. Andrikopoulos, Konstantinos S. Sygellou, Labrini Dracopoulos, Vassilios Yakoumis, Iakovos Voyiatzis, George A. Molecules Article The global trend in restrictions on pollutant emissions requires the use of catalytic converters in the automotive industry. Noble metals belonging to the platinum group metals (PGMs, platinum, palladium, and rhodium) are currently used for autocatalysts. However, recent efforts focus on the development of new catalytic converters that combine high activity and reduced cost, attracting the interest of the automotive industry. Among them, the partial substitution of PGMs by abundant non-PGMs (transition metals such as copper) seems to be a promising alternative. The PROMETHEUS catalyst (PROM100) is a polymetallic nanosized copper-based catalyst for automotives prepared by a wet impregnation method, using as a carrier an inorganic mixed oxide (CeO(2)-ZrO(2)) exhibiting elevated oxygen storage capacity. On the other hand, catalyst deactivation or ageing is defined as the process in which the structure and state of the catalyst change, leading to the loss of the catalyst’s active sites with a subsequent decrease in the catalyst’s performance, significantly affecting the emissions of the catalyst. The main scope of this research is to investigate in detail the effect of ageing on this low-cost, effective catalyst. To that end, a detailed characterization has been performed with a train of methods, such as SEM, Raman, XRD, XRF, BET and XPS, to both ceria–zirconia mixed inorganic oxide support (CZ-fresh and -aged) and to the copper-based catalyst (PROM100-fresh and -aged), revealing the impact of ageing on catalytic efficiency. It was found that ageing affects the Ce–Zr mixed oxide structure by initiating the formation of distinct ZrO(2) and CeO(2) structures monitored by Raman and XRD. In addition, it crucially affects the morphology of the sample by reducing the surface area by a factor of nearly two orders of magnitude and increasing particle size as indicated by BET and SEM due to sintering. Finally, the Pd concentration was found to be considerably reduced from the material’s surface as suggested by XPS data. The above-mentioned alterations observed after ageing increased the light-off temperatures by more than 175 °C, compared to the fresh sample, without affecting the overall efficiency of the catalyst for CO and CH(4) oxidation reactions. Metal particle and CeZr carrier sintering, washcoat loss as well as partial metal encapsulation by Cu and/or CeZrO(4) are identified as the main causes for the deactivation after hydrothermal ageing. MDPI 2022-10-31 /pmc/articles/PMC9657973/ /pubmed/36364229 http://dx.doi.org/10.3390/molecules27217402 Text en © 2022 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
Soto Beobide, Amaia
Moschovi, Anastasia M.
Mathioudakis, Georgios N.
Kourtelesis, Marios
Lada, Zoi G.
Andrikopoulos, Konstantinos S.
Sygellou, Labrini
Dracopoulos, Vassilios
Yakoumis, Iakovos
Voyiatzis, George A.
High Catalytic Efficiency of a Nanosized Copper-Based Catalyst for Automotives: A Physicochemical Characterization
title High Catalytic Efficiency of a Nanosized Copper-Based Catalyst for Automotives: A Physicochemical Characterization
title_full High Catalytic Efficiency of a Nanosized Copper-Based Catalyst for Automotives: A Physicochemical Characterization
title_fullStr High Catalytic Efficiency of a Nanosized Copper-Based Catalyst for Automotives: A Physicochemical Characterization
title_full_unstemmed High Catalytic Efficiency of a Nanosized Copper-Based Catalyst for Automotives: A Physicochemical Characterization
title_short High Catalytic Efficiency of a Nanosized Copper-Based Catalyst for Automotives: A Physicochemical Characterization
title_sort high catalytic efficiency of a nanosized copper-based catalyst for automotives: a physicochemical characterization
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9657973/
https://www.ncbi.nlm.nih.gov/pubmed/36364229
http://dx.doi.org/10.3390/molecules27217402
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