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Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol
Exposing a Cu‐based catalyst to a suitable temperature is of great importance to optimize its hydrogenation performance, as copper is sensitive to temperature. Herein, we investigated the effect of the initial oxidation state of copper, tuned by the reduction temperature, on its catalytic performanc...
Autores principales: | , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
John Wiley and Sons Inc.
2018
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6276878/ https://www.ncbi.nlm.nih.gov/pubmed/30524922 http://dx.doi.org/10.1002/open.201800225 |
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author | Sun, Yannan Meng, Fanqiong Ge, Qingjie Sun, Jian |
author_facet | Sun, Yannan Meng, Fanqiong Ge, Qingjie Sun, Jian |
author_sort | Sun, Yannan |
collection | PubMed |
description | Exposing a Cu‐based catalyst to a suitable temperature is of great importance to optimize its hydrogenation performance, as copper is sensitive to temperature. Herein, we investigated the effect of the initial oxidation state of copper, tuned by the reduction temperature, on its catalytic performance in the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG) through designing a series of catalysts with different reduction temperatures (200–350 °C). Among these catalysts, the Cu/SiO(2) catalyst prepared by ammonia evaporation with a hydrogen reduction process at 250 °C showed the best performance in the hydrogenation of DMO with a conversion of 100 % and a selectivity to EG higher than 95 %. The relationship between the initial oxidation state of copper and catalytic performance was well established by characterizing the physicochemical properties of the Cu/SiO(2) catalysts by XRD, TEM, H(2) temperature‐programmed reduction, N(2)O adsorption, and in situ reduction Auger electron spectroscopy. The initial oxidation state of copper determined the conversion of DMO and the distribution of the products, and it could be balanced by reducing the temperature to improve the activity of the catalyst. This work provides a reference for further exploration of the mechanism and guidance for the design of catalysts for the hydrogenation of esters. |
format | Online Article Text |
id | pubmed-6276878 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2018 |
publisher | John Wiley and Sons Inc. |
record_format | MEDLINE/PubMed |
spelling | pubmed-62768782018-12-06 Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol Sun, Yannan Meng, Fanqiong Ge, Qingjie Sun, Jian ChemistryOpen Full Papers Exposing a Cu‐based catalyst to a suitable temperature is of great importance to optimize its hydrogenation performance, as copper is sensitive to temperature. Herein, we investigated the effect of the initial oxidation state of copper, tuned by the reduction temperature, on its catalytic performance in the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG) through designing a series of catalysts with different reduction temperatures (200–350 °C). Among these catalysts, the Cu/SiO(2) catalyst prepared by ammonia evaporation with a hydrogen reduction process at 250 °C showed the best performance in the hydrogenation of DMO with a conversion of 100 % and a selectivity to EG higher than 95 %. The relationship between the initial oxidation state of copper and catalytic performance was well established by characterizing the physicochemical properties of the Cu/SiO(2) catalysts by XRD, TEM, H(2) temperature‐programmed reduction, N(2)O adsorption, and in situ reduction Auger electron spectroscopy. The initial oxidation state of copper determined the conversion of DMO and the distribution of the products, and it could be balanced by reducing the temperature to improve the activity of the catalyst. This work provides a reference for further exploration of the mechanism and guidance for the design of catalysts for the hydrogenation of esters. John Wiley and Sons Inc. 2018-11-20 /pmc/articles/PMC6276878/ /pubmed/30524922 http://dx.doi.org/10.1002/open.201800225 Text en © 2018 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the http://creativecommons.org/licenses/by-nc/4.0/ License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes. |
spellingShingle | Full Papers Sun, Yannan Meng, Fanqiong Ge, Qingjie Sun, Jian Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol |
title | Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol |
title_full | Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol |
title_fullStr | Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol |
title_full_unstemmed | Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol |
title_short | Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol |
title_sort | importance of the initial oxidation state of copper for the catalytic hydrogenation of dimethyl oxalate to ethylene glycol |
topic | Full Papers |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6276878/ https://www.ncbi.nlm.nih.gov/pubmed/30524922 http://dx.doi.org/10.1002/open.201800225 |
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