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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...

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Autores principales: Sharko, Anastasiia, Spitzbarth, Benjamin, Hermans, Thomas M., Eelkema, Rienk
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
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.
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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
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