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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...
Autores principales: | , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
The Royal Society of Chemistry
2020
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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. |
format | Online Article Text |
id | pubmed-9054116 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2020 |
publisher | The Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
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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