Cargando…

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...

Descripción completa

Detalles Bibliográficos
Autores principales: Sheppard, Thomas, Daly, Helen, Goguet, Alex, Thompson, Jillian M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2015
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
_version_ 1782416151445241856
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
work_keys_str_mv AT sheppardthomas improvedefficiencyforpartialoxidationofmethanebycontrolledcopperdepositiononsurfacemodifiedzsm5
AT dalyhelen improvedefficiencyforpartialoxidationofmethanebycontrolledcopperdepositiononsurfacemodifiedzsm5
AT goguetalex improvedefficiencyforpartialoxidationofmethanebycontrolledcopperdepositiononsurfacemodifiedzsm5
AT thompsonjillianm improvedefficiencyforpartialoxidationofmethanebycontrolledcopperdepositiononsurfacemodifiedzsm5