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Chemical Feedback in Templated Reaction-Assembly Networks

[Image: see text] Chemical feedback between building block synthesis and their subsequent supramolecular self-assembly into nanostructures has profound effects on assembly pathways. Nature harnesses feedback in reaction-assembly networks in a variety of scenarios including virion formation and prote...

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Autores principales: Bos, Inge, Terenzi, Camilla, Sprakel, Joris
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2020
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7726899/
https://www.ncbi.nlm.nih.gov/pubmed/33328693
http://dx.doi.org/10.1021/acs.macromol.0c01915
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author Bos, Inge
Terenzi, Camilla
Sprakel, Joris
author_facet Bos, Inge
Terenzi, Camilla
Sprakel, Joris
author_sort Bos, Inge
collection PubMed
description [Image: see text] Chemical feedback between building block synthesis and their subsequent supramolecular self-assembly into nanostructures has profound effects on assembly pathways. Nature harnesses feedback in reaction-assembly networks in a variety of scenarios including virion formation and protein folding. Also in nanomaterial synthesis, reaction-assembly networks have emerged as a promising control strategy to regulate assembly processes. Yet, how chemical feedback affects the fundamental pathways of structure formation remains unclear. Here, we unravel the pathways of a templated reaction-assembly network that couples a covalent polymerization to an electrostatic coassembly process. We show how the supramolecular staging of building blocks at a macromolecular template can accelerate the polymerization reaction and prevent the formation of kinetically trapped structures inherent to the process in the absence of feedback. Finally, we establish a predictive kinetic reaction model that quantitatively describes the pathways underlying these reaction-assembly networks. Our results shed light on the fundamental mechanisms by which chemical feedback can steer self-assembly reactions and can be used to rationally design new nanostructures.
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spelling pubmed-77268992020-12-14 Chemical Feedback in Templated Reaction-Assembly Networks Bos, Inge Terenzi, Camilla Sprakel, Joris Macromolecules [Image: see text] Chemical feedback between building block synthesis and their subsequent supramolecular self-assembly into nanostructures has profound effects on assembly pathways. Nature harnesses feedback in reaction-assembly networks in a variety of scenarios including virion formation and protein folding. Also in nanomaterial synthesis, reaction-assembly networks have emerged as a promising control strategy to regulate assembly processes. Yet, how chemical feedback affects the fundamental pathways of structure formation remains unclear. Here, we unravel the pathways of a templated reaction-assembly network that couples a covalent polymerization to an electrostatic coassembly process. We show how the supramolecular staging of building blocks at a macromolecular template can accelerate the polymerization reaction and prevent the formation of kinetically trapped structures inherent to the process in the absence of feedback. Finally, we establish a predictive kinetic reaction model that quantitatively describes the pathways underlying these reaction-assembly networks. Our results shed light on the fundamental mechanisms by which chemical feedback can steer self-assembly reactions and can be used to rationally design new nanostructures. American Chemical Society 2020-11-23 2020-12-08 /pmc/articles/PMC7726899/ /pubmed/33328693 http://dx.doi.org/10.1021/acs.macromol.0c01915 Text en © 2020 American Chemical Society This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
spellingShingle Bos, Inge
Terenzi, Camilla
Sprakel, Joris
Chemical Feedback in Templated Reaction-Assembly Networks
title Chemical Feedback in Templated Reaction-Assembly Networks
title_full Chemical Feedback in Templated Reaction-Assembly Networks
title_fullStr Chemical Feedback in Templated Reaction-Assembly Networks
title_full_unstemmed Chemical Feedback in Templated Reaction-Assembly Networks
title_short Chemical Feedback in Templated Reaction-Assembly Networks
title_sort chemical feedback in templated reaction-assembly networks
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7726899/
https://www.ncbi.nlm.nih.gov/pubmed/33328693
http://dx.doi.org/10.1021/acs.macromol.0c01915
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