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Gas reactions under intrapore condensation regime within tailored metal–organic framework catalysts
Production of 1-butene, a major monomer in polymer industry, is dominated by homogeneous protocols via ethylene dimerization. Homogeneous catalysts can achieve high selectivity but require large amounts of activators and solvents, and exhibit poor recyclability; in turn, heterogeneous systems are ro...
Autores principales: | , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2019
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6502813/ https://www.ncbi.nlm.nih.gov/pubmed/31061386 http://dx.doi.org/10.1038/s41467-019-10013-6 |
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author | Agirrezabal-Telleria, Iker Luz, Ignacio Ortuño, Manuel A. Oregui-Bengoechea, Mikel Gandarias, Iñaki López, Núria Lail, Marty A. Soukri, Mustapha |
author_facet | Agirrezabal-Telleria, Iker Luz, Ignacio Ortuño, Manuel A. Oregui-Bengoechea, Mikel Gandarias, Iñaki López, Núria Lail, Marty A. Soukri, Mustapha |
author_sort | Agirrezabal-Telleria, Iker |
collection | PubMed |
description | Production of 1-butene, a major monomer in polymer industry, is dominated by homogeneous protocols via ethylene dimerization. Homogeneous catalysts can achieve high selectivity but require large amounts of activators and solvents, and exhibit poor recyclability; in turn, heterogeneous systems are robust but lack selectivity. Here we show how the precise engineering of metal–organic frameworks (MOFs) holds promise for a sustainable process. The key to the (Ru)HKUST-1 MOF activity is the intrapore reactant condensation that enhances ethylene dimerization with high selectivity (> 99% 1-butene) and high stability (> 120 h) in the absence of activators and solvents. According to spectroscopy, kinetics, and modeling, the engineering of defective nodes via controlled thermal approaches rules the activity, while intrapore ethylene condensation accounts for selectivity and stability. The combination of well-defined actives sites with the concentration effect arising from condensation regimes paves the way toward the development of robust MOF catalysts for diverse gas-phase reactions. |
format | Online Article Text |
id | pubmed-6502813 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2019 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-65028132019-05-08 Gas reactions under intrapore condensation regime within tailored metal–organic framework catalysts Agirrezabal-Telleria, Iker Luz, Ignacio Ortuño, Manuel A. Oregui-Bengoechea, Mikel Gandarias, Iñaki López, Núria Lail, Marty A. Soukri, Mustapha Nat Commun Article Production of 1-butene, a major monomer in polymer industry, is dominated by homogeneous protocols via ethylene dimerization. Homogeneous catalysts can achieve high selectivity but require large amounts of activators and solvents, and exhibit poor recyclability; in turn, heterogeneous systems are robust but lack selectivity. Here we show how the precise engineering of metal–organic frameworks (MOFs) holds promise for a sustainable process. The key to the (Ru)HKUST-1 MOF activity is the intrapore reactant condensation that enhances ethylene dimerization with high selectivity (> 99% 1-butene) and high stability (> 120 h) in the absence of activators and solvents. According to spectroscopy, kinetics, and modeling, the engineering of defective nodes via controlled thermal approaches rules the activity, while intrapore ethylene condensation accounts for selectivity and stability. The combination of well-defined actives sites with the concentration effect arising from condensation regimes paves the way toward the development of robust MOF catalysts for diverse gas-phase reactions. Nature Publishing Group UK 2019-05-06 /pmc/articles/PMC6502813/ /pubmed/31061386 http://dx.doi.org/10.1038/s41467-019-10013-6 Text en © The Author(s) 2019 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. |
spellingShingle | Article Agirrezabal-Telleria, Iker Luz, Ignacio Ortuño, Manuel A. Oregui-Bengoechea, Mikel Gandarias, Iñaki López, Núria Lail, Marty A. Soukri, Mustapha Gas reactions under intrapore condensation regime within tailored metal–organic framework catalysts |
title | Gas reactions under intrapore condensation regime within tailored metal–organic framework catalysts |
title_full | Gas reactions under intrapore condensation regime within tailored metal–organic framework catalysts |
title_fullStr | Gas reactions under intrapore condensation regime within tailored metal–organic framework catalysts |
title_full_unstemmed | Gas reactions under intrapore condensation regime within tailored metal–organic framework catalysts |
title_short | Gas reactions under intrapore condensation regime within tailored metal–organic framework catalysts |
title_sort | gas reactions under intrapore condensation regime within tailored metal–organic framework catalysts |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6502813/ https://www.ncbi.nlm.nih.gov/pubmed/31061386 http://dx.doi.org/10.1038/s41467-019-10013-6 |
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