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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...

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Autores principales: Sun, Yannan, Meng, Fanqiong, Ge, Qingjie, Sun, Jian
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2018
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.
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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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