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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...

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Autores principales: Yang, Hao, Xu, Jinhui, Cao, Hui, Wu, Jie, Zhao, Dan
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
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.
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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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