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Selective catalytic two-step process for ethylene glycol from carbon monoxide

Upgrading C1 chemicals (for example, CO, CO/H(2), MeOH and CO(2)) with C–C bond formation is essential for the synthesis of bulk chemicals. In general, these industrially important processes (for example, Fischer Tropsch) proceed at drastic reaction conditions (>250 °C; high pressure) and suffer...

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Autores principales: Dong, Kaiwu, Elangovan, Saravanakumar, Sang, Rui, Spannenberg, Anke, Jackstell, Ralf, Junge, Kathrin, Li, Yuehui, Beller, Matthias
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group 2016
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4935967/
https://www.ncbi.nlm.nih.gov/pubmed/27377550
http://dx.doi.org/10.1038/ncomms12075
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author Dong, Kaiwu
Elangovan, Saravanakumar
Sang, Rui
Spannenberg, Anke
Jackstell, Ralf
Junge, Kathrin
Li, Yuehui
Beller, Matthias
author_facet Dong, Kaiwu
Elangovan, Saravanakumar
Sang, Rui
Spannenberg, Anke
Jackstell, Ralf
Junge, Kathrin
Li, Yuehui
Beller, Matthias
author_sort Dong, Kaiwu
collection PubMed
description Upgrading C1 chemicals (for example, CO, CO/H(2), MeOH and CO(2)) with C–C bond formation is essential for the synthesis of bulk chemicals. In general, these industrially important processes (for example, Fischer Tropsch) proceed at drastic reaction conditions (>250 °C; high pressure) and suffer from low selectivity, which makes high capital investment necessary and requires additional purifications. Here, a different strategy for the preparation of ethylene glycol (EG) via initial oxidative coupling and subsequent reduction is presented. Separating coupling and reduction steps allows for a completely selective formation of EG (99%) from CO. This two-step catalytic procedure makes use of a Pd-catalysed oxycarbonylation of amines to oxamides at room temperature (RT) and subsequent Ru- or Fe-catalysed hydrogenation to EG. Notably, in the first step the required amines can be efficiently reused. The presented stepwise oxamide-mediated coupling provides the basis for a new strategy for selective upgrading of C1 chemicals.
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spelling pubmed-49359672016-07-14 Selective catalytic two-step process for ethylene glycol from carbon monoxide Dong, Kaiwu Elangovan, Saravanakumar Sang, Rui Spannenberg, Anke Jackstell, Ralf Junge, Kathrin Li, Yuehui Beller, Matthias Nat Commun Article Upgrading C1 chemicals (for example, CO, CO/H(2), MeOH and CO(2)) with C–C bond formation is essential for the synthesis of bulk chemicals. In general, these industrially important processes (for example, Fischer Tropsch) proceed at drastic reaction conditions (>250 °C; high pressure) and suffer from low selectivity, which makes high capital investment necessary and requires additional purifications. Here, a different strategy for the preparation of ethylene glycol (EG) via initial oxidative coupling and subsequent reduction is presented. Separating coupling and reduction steps allows for a completely selective formation of EG (99%) from CO. This two-step catalytic procedure makes use of a Pd-catalysed oxycarbonylation of amines to oxamides at room temperature (RT) and subsequent Ru- or Fe-catalysed hydrogenation to EG. Notably, in the first step the required amines can be efficiently reused. The presented stepwise oxamide-mediated coupling provides the basis for a new strategy for selective upgrading of C1 chemicals. Nature Publishing Group 2016-07-05 /pmc/articles/PMC4935967/ /pubmed/27377550 http://dx.doi.org/10.1038/ncomms12075 Text en Copyright © 2016, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved. http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
spellingShingle Article
Dong, Kaiwu
Elangovan, Saravanakumar
Sang, Rui
Spannenberg, Anke
Jackstell, Ralf
Junge, Kathrin
Li, Yuehui
Beller, Matthias
Selective catalytic two-step process for ethylene glycol from carbon monoxide
title Selective catalytic two-step process for ethylene glycol from carbon monoxide
title_full Selective catalytic two-step process for ethylene glycol from carbon monoxide
title_fullStr Selective catalytic two-step process for ethylene glycol from carbon monoxide
title_full_unstemmed Selective catalytic two-step process for ethylene glycol from carbon monoxide
title_short Selective catalytic two-step process for ethylene glycol from carbon monoxide
title_sort selective catalytic two-step process for ethylene glycol from carbon monoxide
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4935967/
https://www.ncbi.nlm.nih.gov/pubmed/27377550
http://dx.doi.org/10.1038/ncomms12075
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