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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...
Autores principales: | , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2020
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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. |
format | Online Article Text |
id | pubmed-7726899 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2020 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
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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