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Mechanochemical defect engineering of HKUST-1 and impact of the resulting defects on carbon dioxide sorption and catalytic cyclopropanation

Metal–organic frameworks (MOFs) are recognized as ideal candidates for many applications such as gas sorption and catalysis. For a long time the properties of these materials were thought to essentially arise from their well-defined crystal structures. It is only recently that the importance of stru...

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Autores principales: Steenhaut, Timothy, Grégoire, Nicolas, Barozzino-Consiglio, Gabriella, Filinchuk, Yaroslav, Hermans, Sophie
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9054116/
https://www.ncbi.nlm.nih.gov/pubmed/35520409
http://dx.doi.org/10.1039/c9ra10412g
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author Steenhaut, Timothy
Grégoire, Nicolas
Barozzino-Consiglio, Gabriella
Filinchuk, Yaroslav
Hermans, Sophie
author_facet Steenhaut, Timothy
Grégoire, Nicolas
Barozzino-Consiglio, Gabriella
Filinchuk, Yaroslav
Hermans, Sophie
author_sort Steenhaut, Timothy
collection PubMed
description Metal–organic frameworks (MOFs) are recognized as ideal candidates for many applications such as gas sorption and catalysis. For a long time the properties of these materials were thought to essentially arise from their well-defined crystal structures. It is only recently that the importance of structural defects for the properties of MOFs has been evidenced. In this work, salt-assisted and liquid-assisted grinding were used to introduce defects in a copper-based MOF, namely HKUST-1. Different milling times and post-synthetic treatments with alcohols allow introduction of defects in the form of free carboxylic acid groups or reduced copper(i) sites. The nature and the amount of defects were evaluated by spectroscopic methods (FTIR, XPS) as well as TGA and NH(3) temperature-programmed desorption experiments. The negative impact of free –COOH groups on the catalytic cyclopropanation reaction of ethyl diazoacetate with styrene, as well as on the gravimetric CO(2) sorption capacities of the materials, was demonstrated. The improvement of the catalytic activity of carboxylic acid containing materials by the presence of Cu(I) sites was also evidenced.
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spelling pubmed-90541162022-05-04 Mechanochemical defect engineering of HKUST-1 and impact of the resulting defects on carbon dioxide sorption and catalytic cyclopropanation Steenhaut, Timothy Grégoire, Nicolas Barozzino-Consiglio, Gabriella Filinchuk, Yaroslav Hermans, Sophie RSC Adv Chemistry Metal–organic frameworks (MOFs) are recognized as ideal candidates for many applications such as gas sorption and catalysis. For a long time the properties of these materials were thought to essentially arise from their well-defined crystal structures. It is only recently that the importance of structural defects for the properties of MOFs has been evidenced. In this work, salt-assisted and liquid-assisted grinding were used to introduce defects in a copper-based MOF, namely HKUST-1. Different milling times and post-synthetic treatments with alcohols allow introduction of defects in the form of free carboxylic acid groups or reduced copper(i) sites. The nature and the amount of defects were evaluated by spectroscopic methods (FTIR, XPS) as well as TGA and NH(3) temperature-programmed desorption experiments. The negative impact of free –COOH groups on the catalytic cyclopropanation reaction of ethyl diazoacetate with styrene, as well as on the gravimetric CO(2) sorption capacities of the materials, was demonstrated. The improvement of the catalytic activity of carboxylic acid containing materials by the presence of Cu(I) sites was also evidenced. The Royal Society of Chemistry 2020-05-27 /pmc/articles/PMC9054116/ /pubmed/35520409 http://dx.doi.org/10.1039/c9ra10412g Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/
spellingShingle Chemistry
Steenhaut, Timothy
Grégoire, Nicolas
Barozzino-Consiglio, Gabriella
Filinchuk, Yaroslav
Hermans, Sophie
Mechanochemical defect engineering of HKUST-1 and impact of the resulting defects on carbon dioxide sorption and catalytic cyclopropanation
title Mechanochemical defect engineering of HKUST-1 and impact of the resulting defects on carbon dioxide sorption and catalytic cyclopropanation
title_full Mechanochemical defect engineering of HKUST-1 and impact of the resulting defects on carbon dioxide sorption and catalytic cyclopropanation
title_fullStr Mechanochemical defect engineering of HKUST-1 and impact of the resulting defects on carbon dioxide sorption and catalytic cyclopropanation
title_full_unstemmed Mechanochemical defect engineering of HKUST-1 and impact of the resulting defects on carbon dioxide sorption and catalytic cyclopropanation
title_short Mechanochemical defect engineering of HKUST-1 and impact of the resulting defects on carbon dioxide sorption and catalytic cyclopropanation
title_sort mechanochemical defect engineering of hkust-1 and impact of the resulting defects on carbon dioxide sorption and catalytic cyclopropanation
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9054116/
https://www.ncbi.nlm.nih.gov/pubmed/35520409
http://dx.doi.org/10.1039/c9ra10412g
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