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Design of Pd-based pseudo-binary alloy catalysts for highly active and selective NO reduction

The development of Pd-based alloy catalysts for highly active and selective reduction of NO by CO was investigated. A survey of Pd-based bimetallic catalysts (PdM/Al(2)O(3): M = Cu, In, Pb, Sn, and Zn) revealed that the PdIn/Al(2)O(3) catalyst displayed excellent N(2) selectivity even at low tempera...

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Autores principales: Jeon, Jaewan, Kon, Ken-ichi, Toyao, Takashi, Shimizu, Ken-ichi, Furukawa, Shinya
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Royal Society of Chemistry 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6471737/
https://www.ncbi.nlm.nih.gov/pubmed/31057743
http://dx.doi.org/10.1039/c8sc05496g
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author Jeon, Jaewan
Kon, Ken-ichi
Toyao, Takashi
Shimizu, Ken-ichi
Furukawa, Shinya
author_facet Jeon, Jaewan
Kon, Ken-ichi
Toyao, Takashi
Shimizu, Ken-ichi
Furukawa, Shinya
author_sort Jeon, Jaewan
collection PubMed
description The development of Pd-based alloy catalysts for highly active and selective reduction of NO by CO was investigated. A survey of Pd-based bimetallic catalysts (PdM/Al(2)O(3): M = Cu, In, Pb, Sn, and Zn) revealed that the PdIn/Al(2)O(3) catalyst displayed excellent N(2) selectivity even at low temperatures (100% at 200 °C). The catalytic activity of PdIn was further improved by substituting a part of In with Cu, where a Pd(In(1–x)Cu(x)) pseudo-binary alloy structure was formed. The optimized catalyst, namely, Pd(In(0.33)Cu(0.67))/Al(2)O(3), facilitated the complete conversion of NO to N(2) (100% yield) even at 200 °C and higher, which has never been achieved using metallic catalysts. The formation of the pseudo-binary alloy structure was confirmed by the combination of HAADF-STEM-EDS, EXAFS, and CO-FT-IR analyses. A detailed mechanistic study based on kinetic analysis, operando XAFS, and DFT calculations revealed the roles of In and Cu in the significant enhancement of catalytic performance: (1) N(2)O adsorption and decomposition (N(2)O → N(2) + O) were drastically enhanced by In, thus resulting in high N(2) selectivity; (2) CO oxidation was promoted by In, thus leading to enhanced low-temperature activity; and (3) Cu substitution improved NO adsorption and dissociation (NO → N + O), thus resulting in the promotion of high-temperature activity.
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spelling pubmed-64717372019-05-03 Design of Pd-based pseudo-binary alloy catalysts for highly active and selective NO reduction Jeon, Jaewan Kon, Ken-ichi Toyao, Takashi Shimizu, Ken-ichi Furukawa, Shinya Chem Sci Chemistry The development of Pd-based alloy catalysts for highly active and selective reduction of NO by CO was investigated. A survey of Pd-based bimetallic catalysts (PdM/Al(2)O(3): M = Cu, In, Pb, Sn, and Zn) revealed that the PdIn/Al(2)O(3) catalyst displayed excellent N(2) selectivity even at low temperatures (100% at 200 °C). The catalytic activity of PdIn was further improved by substituting a part of In with Cu, where a Pd(In(1–x)Cu(x)) pseudo-binary alloy structure was formed. The optimized catalyst, namely, Pd(In(0.33)Cu(0.67))/Al(2)O(3), facilitated the complete conversion of NO to N(2) (100% yield) even at 200 °C and higher, which has never been achieved using metallic catalysts. The formation of the pseudo-binary alloy structure was confirmed by the combination of HAADF-STEM-EDS, EXAFS, and CO-FT-IR analyses. A detailed mechanistic study based on kinetic analysis, operando XAFS, and DFT calculations revealed the roles of In and Cu in the significant enhancement of catalytic performance: (1) N(2)O adsorption and decomposition (N(2)O → N(2) + O) were drastically enhanced by In, thus resulting in high N(2) selectivity; (2) CO oxidation was promoted by In, thus leading to enhanced low-temperature activity; and (3) Cu substitution improved NO adsorption and dissociation (NO → N + O), thus resulting in the promotion of high-temperature activity. Royal Society of Chemistry 2019-03-04 /pmc/articles/PMC6471737/ /pubmed/31057743 http://dx.doi.org/10.1039/c8sc05496g Text en This journal is © The Royal Society of Chemistry 2019 http://creativecommons.org/licenses/by/3.0/ This article is freely available. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence (CC BY 3.0)
spellingShingle Chemistry
Jeon, Jaewan
Kon, Ken-ichi
Toyao, Takashi
Shimizu, Ken-ichi
Furukawa, Shinya
Design of Pd-based pseudo-binary alloy catalysts for highly active and selective NO reduction
title Design of Pd-based pseudo-binary alloy catalysts for highly active and selective NO reduction
title_full Design of Pd-based pseudo-binary alloy catalysts for highly active and selective NO reduction
title_fullStr Design of Pd-based pseudo-binary alloy catalysts for highly active and selective NO reduction
title_full_unstemmed Design of Pd-based pseudo-binary alloy catalysts for highly active and selective NO reduction
title_short Design of Pd-based pseudo-binary alloy catalysts for highly active and selective NO reduction
title_sort design of pd-based pseudo-binary alloy catalysts for highly active and selective no reduction
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6471737/
https://www.ncbi.nlm.nih.gov/pubmed/31057743
http://dx.doi.org/10.1039/c8sc05496g
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