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Redox-Controlled Shunts in a Synthetic Chemical Reaction Cycle
[Image: see text] Shunts, alternative pathways in chemical reaction networks (CRNs), are ubiquitous in nature, enabling adaptability to external and internal stimuli. We introduce a CRN in which the recovery of Michael-accepting species is driven by oxidation chemistry. Using weak oxidants can enabl...
Autores principales: | , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10161229/ https://www.ncbi.nlm.nih.gov/pubmed/37092741 http://dx.doi.org/10.1021/jacs.3c00985 |
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author | Sharko, Anastasiia Spitzbarth, Benjamin Hermans, Thomas M. Eelkema, Rienk |
author_facet | Sharko, Anastasiia Spitzbarth, Benjamin Hermans, Thomas M. Eelkema, Rienk |
author_sort | Sharko, Anastasiia |
collection | PubMed |
description | [Image: see text] Shunts, alternative pathways in chemical reaction networks (CRNs), are ubiquitous in nature, enabling adaptability to external and internal stimuli. We introduce a CRN in which the recovery of Michael-accepting species is driven by oxidation chemistry. Using weak oxidants can enable access to two shunts within this CRN with different kinetics and a reduced number of side reactions compared to the main cycle that is driven by strong oxidants. Furthermore, we introduce a strategy to recycle one of the main products under flow conditions to partially reverse the CRN and control product speciation throughout time. These findings introduce new levels of control over artificial CRNs, driven by redox chemistry, narrowing the gap between synthetic and natural systems. |
format | Online Article Text |
id | pubmed-10161229 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-101612292023-05-06 Redox-Controlled Shunts in a Synthetic Chemical Reaction Cycle Sharko, Anastasiia Spitzbarth, Benjamin Hermans, Thomas M. Eelkema, Rienk J Am Chem Soc [Image: see text] Shunts, alternative pathways in chemical reaction networks (CRNs), are ubiquitous in nature, enabling adaptability to external and internal stimuli. We introduce a CRN in which the recovery of Michael-accepting species is driven by oxidation chemistry. Using weak oxidants can enable access to two shunts within this CRN with different kinetics and a reduced number of side reactions compared to the main cycle that is driven by strong oxidants. Furthermore, we introduce a strategy to recycle one of the main products under flow conditions to partially reverse the CRN and control product speciation throughout time. These findings introduce new levels of control over artificial CRNs, driven by redox chemistry, narrowing the gap between synthetic and natural systems. American Chemical Society 2023-04-24 /pmc/articles/PMC10161229/ /pubmed/37092741 http://dx.doi.org/10.1021/jacs.3c00985 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Sharko, Anastasiia Spitzbarth, Benjamin Hermans, Thomas M. Eelkema, Rienk Redox-Controlled Shunts in a Synthetic Chemical Reaction Cycle |
title | Redox-Controlled Shunts
in a Synthetic Chemical Reaction
Cycle |
title_full | Redox-Controlled Shunts
in a Synthetic Chemical Reaction
Cycle |
title_fullStr | Redox-Controlled Shunts
in a Synthetic Chemical Reaction
Cycle |
title_full_unstemmed | Redox-Controlled Shunts
in a Synthetic Chemical Reaction
Cycle |
title_short | Redox-Controlled Shunts
in a Synthetic Chemical Reaction
Cycle |
title_sort | redox-controlled shunts
in a synthetic chemical reaction
cycle |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10161229/ https://www.ncbi.nlm.nih.gov/pubmed/37092741 http://dx.doi.org/10.1021/jacs.3c00985 |
work_keys_str_mv | AT sharkoanastasiia redoxcontrolledshuntsinasyntheticchemicalreactioncycle AT spitzbarthbenjamin redoxcontrolledshuntsinasyntheticchemicalreactioncycle AT hermansthomasm redoxcontrolledshuntsinasyntheticchemicalreactioncycle AT eelkemarienk redoxcontrolledshuntsinasyntheticchemicalreactioncycle |