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Structure of copper sites in zeolites examined by Fourier and wavelet transform analysis of EXAFS

Copper-exchanged zeolites are a class of redox-active materials that find application in the selective catalytic reduction of exhaust gases of diesel vehicles and, more recently, the selective oxidation of methane to methanol. However, the structure of the active copper-oxo species present in zeolit...

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Autores principales: Sushkevich, Vitaly L., Safonova, Olga V., Palagin, Dennis, Newton, Mark A., van Bokhoven, Jeroen A.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8159279/
https://www.ncbi.nlm.nih.gov/pubmed/34122988
http://dx.doi.org/10.1039/d0sc01472a
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author Sushkevich, Vitaly L.
Safonova, Olga V.
Palagin, Dennis
Newton, Mark A.
van Bokhoven, Jeroen A.
author_facet Sushkevich, Vitaly L.
Safonova, Olga V.
Palagin, Dennis
Newton, Mark A.
van Bokhoven, Jeroen A.
author_sort Sushkevich, Vitaly L.
collection PubMed
description Copper-exchanged zeolites are a class of redox-active materials that find application in the selective catalytic reduction of exhaust gases of diesel vehicles and, more recently, the selective oxidation of methane to methanol. However, the structure of the active copper-oxo species present in zeolites under oxidative environments is still a subject of debate. Herein, we make a comprehensive study of copper species in copper-exchanged zeolites with MOR, MFI, BEA, and FAU frameworks and for different Si/Al ratios and copper loadings using X-ray absorption spectroscopy. Only obtaining high quality EXAFS data, collected at large k-values and measured under cryogenic conditions, in combination with wavelet transform analysis enables the discrimination between the copper-oxo species having different structures. The zeolite topology strongly affects the copper speciation, ranging from monomeric copper species to copper-oxo clusters, hosted in zeolites of different topologies. In contrast, the variation of the Si/Al ratio or copper loading in mordenite does not lead to significant differences in XAS spectra, suggesting that a change, if any, in the structure of copper species in these materials is not distinguishable by EXAFS.
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spelling pubmed-81592792021-06-11 Structure of copper sites in zeolites examined by Fourier and wavelet transform analysis of EXAFS Sushkevich, Vitaly L. Safonova, Olga V. Palagin, Dennis Newton, Mark A. van Bokhoven, Jeroen A. Chem Sci Chemistry Copper-exchanged zeolites are a class of redox-active materials that find application in the selective catalytic reduction of exhaust gases of diesel vehicles and, more recently, the selective oxidation of methane to methanol. However, the structure of the active copper-oxo species present in zeolites under oxidative environments is still a subject of debate. Herein, we make a comprehensive study of copper species in copper-exchanged zeolites with MOR, MFI, BEA, and FAU frameworks and for different Si/Al ratios and copper loadings using X-ray absorption spectroscopy. Only obtaining high quality EXAFS data, collected at large k-values and measured under cryogenic conditions, in combination with wavelet transform analysis enables the discrimination between the copper-oxo species having different structures. The zeolite topology strongly affects the copper speciation, ranging from monomeric copper species to copper-oxo clusters, hosted in zeolites of different topologies. In contrast, the variation of the Si/Al ratio or copper loading in mordenite does not lead to significant differences in XAS spectra, suggesting that a change, if any, in the structure of copper species in these materials is not distinguishable by EXAFS. The Royal Society of Chemistry 2020-05-01 /pmc/articles/PMC8159279/ /pubmed/34122988 http://dx.doi.org/10.1039/d0sc01472a Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by/3.0/
spellingShingle Chemistry
Sushkevich, Vitaly L.
Safonova, Olga V.
Palagin, Dennis
Newton, Mark A.
van Bokhoven, Jeroen A.
Structure of copper sites in zeolites examined by Fourier and wavelet transform analysis of EXAFS
title Structure of copper sites in zeolites examined by Fourier and wavelet transform analysis of EXAFS
title_full Structure of copper sites in zeolites examined by Fourier and wavelet transform analysis of EXAFS
title_fullStr Structure of copper sites in zeolites examined by Fourier and wavelet transform analysis of EXAFS
title_full_unstemmed Structure of copper sites in zeolites examined by Fourier and wavelet transform analysis of EXAFS
title_short Structure of copper sites in zeolites examined by Fourier and wavelet transform analysis of EXAFS
title_sort structure of copper sites in zeolites examined by fourier and wavelet transform analysis of exafs
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8159279/
https://www.ncbi.nlm.nih.gov/pubmed/34122988
http://dx.doi.org/10.1039/d0sc01472a
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