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Pnictogen-Bonding Catalysis and Transport Combined: Polyether Transporters Made In Situ
[Image: see text] The combination of catalysis and transport across lipid bilayer membranes promises directional access to a solvent-free and structured nanospace that could accelerate, modulate, and, at best, enable new chemical reactions. To elaborate on these expectations, anion transport and cat...
Autores principales: | , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2021
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8549043/ https://www.ncbi.nlm.nih.gov/pubmed/34723261 http://dx.doi.org/10.1021/jacsau.1c00345 |
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author | Humeniuk, Heorhii V. Gini, Andrea Hao, Xiaoyu Coelho, Filipe Sakai, Naomi Matile, Stefan |
author_facet | Humeniuk, Heorhii V. Gini, Andrea Hao, Xiaoyu Coelho, Filipe Sakai, Naomi Matile, Stefan |
author_sort | Humeniuk, Heorhii V. |
collection | PubMed |
description | [Image: see text] The combination of catalysis and transport across lipid bilayer membranes promises directional access to a solvent-free and structured nanospace that could accelerate, modulate, and, at best, enable new chemical reactions. To elaborate on these expectations, anion transport and catalysis with pnictogen and tetrel bonds are combined with polyether cascade cyclizations into bioinspired cation transporters. Characterized separately, synergistic anion and cation transporters of very high activity are identified. Combined for catalysis in membranes, cascade cyclizations are found to occur with a formal rate enhancement beyond one million compared to bulk solution and product formation is detected in situ as an increase in transport activity. With this operational system in place, intriguing perspectives open up to exploit all aspects of this unique nanospace for important chemical transformations. |
format | Online Article Text |
id | pubmed-8549043 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-85490432021-10-28 Pnictogen-Bonding Catalysis and Transport Combined: Polyether Transporters Made In Situ Humeniuk, Heorhii V. Gini, Andrea Hao, Xiaoyu Coelho, Filipe Sakai, Naomi Matile, Stefan JACS Au [Image: see text] The combination of catalysis and transport across lipid bilayer membranes promises directional access to a solvent-free and structured nanospace that could accelerate, modulate, and, at best, enable new chemical reactions. To elaborate on these expectations, anion transport and catalysis with pnictogen and tetrel bonds are combined with polyether cascade cyclizations into bioinspired cation transporters. Characterized separately, synergistic anion and cation transporters of very high activity are identified. Combined for catalysis in membranes, cascade cyclizations are found to occur with a formal rate enhancement beyond one million compared to bulk solution and product formation is detected in situ as an increase in transport activity. With this operational system in place, intriguing perspectives open up to exploit all aspects of this unique nanospace for important chemical transformations. American Chemical Society 2021-09-28 /pmc/articles/PMC8549043/ /pubmed/34723261 http://dx.doi.org/10.1021/jacsau.1c00345 Text en © 2021 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by-nc-nd/4.0/Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/). |
spellingShingle | Humeniuk, Heorhii V. Gini, Andrea Hao, Xiaoyu Coelho, Filipe Sakai, Naomi Matile, Stefan Pnictogen-Bonding Catalysis and Transport Combined: Polyether Transporters Made In Situ |
title | Pnictogen-Bonding Catalysis and Transport Combined:
Polyether Transporters Made In Situ |
title_full | Pnictogen-Bonding Catalysis and Transport Combined:
Polyether Transporters Made In Situ |
title_fullStr | Pnictogen-Bonding Catalysis and Transport Combined:
Polyether Transporters Made In Situ |
title_full_unstemmed | Pnictogen-Bonding Catalysis and Transport Combined:
Polyether Transporters Made In Situ |
title_short | Pnictogen-Bonding Catalysis and Transport Combined:
Polyether Transporters Made In Situ |
title_sort | pnictogen-bonding catalysis and transport combined:
polyether transporters made in situ |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8549043/ https://www.ncbi.nlm.nih.gov/pubmed/34723261 http://dx.doi.org/10.1021/jacsau.1c00345 |
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