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Improved Efficiency for Partial Oxidation of Methane by Controlled Copper Deposition on Surface‐Modified ZSM‐5
The mono(μ‐oxo) dicopper cores present in the pores of Cu‐ZSM‐5 are active for the partial oxidation of methane to methanol. However, copper on the external surface reduces the ratio of active, selective sites to unselective sites. More efficient catalysts are obtained by controlling the copper depo...
Autores principales: | , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
John Wiley and Sons Inc.
2015
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4755137/ https://www.ncbi.nlm.nih.gov/pubmed/26925172 http://dx.doi.org/10.1002/cctc.201500980 |
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author | Sheppard, Thomas Daly, Helen Goguet, Alex Thompson, Jillian M. |
author_facet | Sheppard, Thomas Daly, Helen Goguet, Alex Thompson, Jillian M. |
author_sort | Sheppard, Thomas |
collection | PubMed |
description | The mono(μ‐oxo) dicopper cores present in the pores of Cu‐ZSM‐5 are active for the partial oxidation of methane to methanol. However, copper on the external surface reduces the ratio of active, selective sites to unselective sites. More efficient catalysts are obtained by controlling the copper deposition during synthesis. Herein, the external exchange sites of ZSM‐5 samples were passivated by bis(trimethylsilyl) trifluoroacetamide (BSTFA) followed by calcination, promoting selective deposition of intraporous copper during aqueous copper ion exchange. At an optimum level of 1–2 wt % SiO(2), IR studies showed a 64 % relative reduction in external copper species and temperature‐programmed oxidation analysis showed an associated increase in the formation of methanol compared with unmodified Cu‐ZSM‐5 samples. It is, therefore, reported that the modified zeolites contained a significantly higher proportion of active, selective copper species than their unmodified counterparts with activity for partial methane oxidation to methanol. |
format | Online Article Text |
id | pubmed-4755137 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2015 |
publisher | John Wiley and Sons Inc. |
record_format | MEDLINE/PubMed |
spelling | pubmed-47551372016-02-25 Improved Efficiency for Partial Oxidation of Methane by Controlled Copper Deposition on Surface‐Modified ZSM‐5 Sheppard, Thomas Daly, Helen Goguet, Alex Thompson, Jillian M. ChemCatChem Full Papers The mono(μ‐oxo) dicopper cores present in the pores of Cu‐ZSM‐5 are active for the partial oxidation of methane to methanol. However, copper on the external surface reduces the ratio of active, selective sites to unselective sites. More efficient catalysts are obtained by controlling the copper deposition during synthesis. Herein, the external exchange sites of ZSM‐5 samples were passivated by bis(trimethylsilyl) trifluoroacetamide (BSTFA) followed by calcination, promoting selective deposition of intraporous copper during aqueous copper ion exchange. At an optimum level of 1–2 wt % SiO(2), IR studies showed a 64 % relative reduction in external copper species and temperature‐programmed oxidation analysis showed an associated increase in the formation of methanol compared with unmodified Cu‐ZSM‐5 samples. It is, therefore, reported that the modified zeolites contained a significantly higher proportion of active, selective copper species than their unmodified counterparts with activity for partial methane oxidation to methanol. John Wiley and Sons Inc. 2015-12-04 2016-02 /pmc/articles/PMC4755137/ /pubmed/26925172 http://dx.doi.org/10.1002/cctc.201500980 Text en © 2015 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution (http://creativecommons.org/licenses/by/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited. |
spellingShingle | Full Papers Sheppard, Thomas Daly, Helen Goguet, Alex Thompson, Jillian M. Improved Efficiency for Partial Oxidation of Methane by Controlled Copper Deposition on Surface‐Modified ZSM‐5 |
title | Improved Efficiency for Partial Oxidation of Methane by Controlled Copper Deposition on Surface‐Modified ZSM‐5 |
title_full | Improved Efficiency for Partial Oxidation of Methane by Controlled Copper Deposition on Surface‐Modified ZSM‐5 |
title_fullStr | Improved Efficiency for Partial Oxidation of Methane by Controlled Copper Deposition on Surface‐Modified ZSM‐5 |
title_full_unstemmed | Improved Efficiency for Partial Oxidation of Methane by Controlled Copper Deposition on Surface‐Modified ZSM‐5 |
title_short | Improved Efficiency for Partial Oxidation of Methane by Controlled Copper Deposition on Surface‐Modified ZSM‐5 |
title_sort | improved efficiency for partial oxidation of methane by controlled copper deposition on surface‐modified zsm‐5 |
topic | Full Papers |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4755137/ https://www.ncbi.nlm.nih.gov/pubmed/26925172 http://dx.doi.org/10.1002/cctc.201500980 |
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