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Recovery of homogeneous photocatalysts by covalent organic framework membranes
Transition metal-based homogeneous photocatalysts offer a wealth of opportunities for organic synthesis. The most versatile ruthenium(II) and iridium(III) polypyridyl complexes, however, are among the rarest metal complexes. Moreover, immobilizing these precious catalysts for recycling is challengin...
Autores principales: | , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2023
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10175538/ https://www.ncbi.nlm.nih.gov/pubmed/37169759 http://dx.doi.org/10.1038/s41467-023-38424-6 |
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author | Yang, Hao Xu, Jinhui Cao, Hui Wu, Jie Zhao, Dan |
author_facet | Yang, Hao Xu, Jinhui Cao, Hui Wu, Jie Zhao, Dan |
author_sort | Yang, Hao |
collection | PubMed |
description | Transition metal-based homogeneous photocatalysts offer a wealth of opportunities for organic synthesis. The most versatile ruthenium(II) and iridium(III) polypyridyl complexes, however, are among the rarest metal complexes. Moreover, immobilizing these precious catalysts for recycling is challenging as their opacity may obstruct light transmission. Recovery of homogeneous catalysts by conventional polymeric membranes is promising but limited, as the modulation of their pore structure and tolerance of polar organic solvents are challenging. Here, we report the effective recovery of homogeneous photocatalysts using covalent organic framework (COF) membranes. An array of COF membranes with tunable pore sizes and superior organic solvent resistance were prepared. Ruthenium and iridium photoredox catalysts were recycled for 10 cycles in various types of photochemical reactions, constantly achieving high catalytical performance, high recovery rates, and high permeance. We successfully recovered the photocatalysts at gram-scale. Furthermore, we demonstrated a cascade isolation of an iridium photocatalyst and purification of a small organic molecule product with COF membranes possessing different pore sizes. Our results indicate an intriguing potential to shift the paradigm of the pharmaceutical and fine chemical synthesis campaign. |
format | Online Article Text |
id | pubmed-10175538 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-101755382023-05-13 Recovery of homogeneous photocatalysts by covalent organic framework membranes Yang, Hao Xu, Jinhui Cao, Hui Wu, Jie Zhao, Dan Nat Commun Article Transition metal-based homogeneous photocatalysts offer a wealth of opportunities for organic synthesis. The most versatile ruthenium(II) and iridium(III) polypyridyl complexes, however, are among the rarest metal complexes. Moreover, immobilizing these precious catalysts for recycling is challenging as their opacity may obstruct light transmission. Recovery of homogeneous catalysts by conventional polymeric membranes is promising but limited, as the modulation of their pore structure and tolerance of polar organic solvents are challenging. Here, we report the effective recovery of homogeneous photocatalysts using covalent organic framework (COF) membranes. An array of COF membranes with tunable pore sizes and superior organic solvent resistance were prepared. Ruthenium and iridium photoredox catalysts were recycled for 10 cycles in various types of photochemical reactions, constantly achieving high catalytical performance, high recovery rates, and high permeance. We successfully recovered the photocatalysts at gram-scale. Furthermore, we demonstrated a cascade isolation of an iridium photocatalyst and purification of a small organic molecule product with COF membranes possessing different pore sizes. Our results indicate an intriguing potential to shift the paradigm of the pharmaceutical and fine chemical synthesis campaign. Nature Publishing Group UK 2023-05-11 /pmc/articles/PMC10175538/ /pubmed/37169759 http://dx.doi.org/10.1038/s41467-023-38424-6 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/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/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Yang, Hao Xu, Jinhui Cao, Hui Wu, Jie Zhao, Dan Recovery of homogeneous photocatalysts by covalent organic framework membranes |
title | Recovery of homogeneous photocatalysts by covalent organic framework membranes |
title_full | Recovery of homogeneous photocatalysts by covalent organic framework membranes |
title_fullStr | Recovery of homogeneous photocatalysts by covalent organic framework membranes |
title_full_unstemmed | Recovery of homogeneous photocatalysts by covalent organic framework membranes |
title_short | Recovery of homogeneous photocatalysts by covalent organic framework membranes |
title_sort | recovery of homogeneous photocatalysts by covalent organic framework membranes |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10175538/ https://www.ncbi.nlm.nih.gov/pubmed/37169759 http://dx.doi.org/10.1038/s41467-023-38424-6 |
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