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Multivalency Enables Dynamic Supramolecular Host–Guest Hydrogel Formation

[Image: see text] Supramolecular and dynamic biomaterials hold promise to recapitulate the time-dependent properties and stimuli-responsiveness of the native extracellular matrix (ECM). Host–guest chemistry is one of the most widely studied supramolecular bonds, yet the binding characteristics of ho...

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Autores principales: Ooi, Huey Wen, Kocken, Jordy M. M., Morgan, Francis L. C., Malheiro, Afonso, Zoetebier, Bram, Karperien, Marcel, Wieringa, Paul A., Dijkstra, Pieter J., Moroni, Lorenzo, Baker, Matthew B.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2020
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7284802/
https://www.ncbi.nlm.nih.gov/pubmed/32243138
http://dx.doi.org/10.1021/acs.biomac.0c00148
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author Ooi, Huey Wen
Kocken, Jordy M. M.
Morgan, Francis L. C.
Malheiro, Afonso
Zoetebier, Bram
Karperien, Marcel
Wieringa, Paul A.
Dijkstra, Pieter J.
Moroni, Lorenzo
Baker, Matthew B.
author_facet Ooi, Huey Wen
Kocken, Jordy M. M.
Morgan, Francis L. C.
Malheiro, Afonso
Zoetebier, Bram
Karperien, Marcel
Wieringa, Paul A.
Dijkstra, Pieter J.
Moroni, Lorenzo
Baker, Matthew B.
author_sort Ooi, Huey Wen
collection PubMed
description [Image: see text] Supramolecular and dynamic biomaterials hold promise to recapitulate the time-dependent properties and stimuli-responsiveness of the native extracellular matrix (ECM). Host–guest chemistry is one of the most widely studied supramolecular bonds, yet the binding characteristics of host–guest complexes (β-CD/adamantane) in relevant biomaterials have mostly focused on singular host–guest interactions or nondiscrete multivalent pendent polymers. The stepwise synergistic effect of multivalent host–guest interactions for the formation of dynamic biomaterials remains relatively unreported. In this work, we study how a series of multivalent adamantane (guest) cross-linkers affect the overall binding affinity and ability to form supramolecular networks with alginate-CD (Alg-CD). These binding constants of the multivalent cross-linkers were determined via NMR titrations and showed increases in binding constants occurring with multivalent constructs. The higher multivalent cross-linkers enabled hydrogel formation; furthermore, an increase in binding and gelation was observed with the inclusion of a phenyl spacer to the cross-linker. A preliminary screen shows that only cross-linking Alg-CD with an 8-arm-multivalent guest results in robust gel formation. These cytocompatible hydrogels highlight the importance of multivalent design for dynamically cross-linked hydrogels. These materials hold promise for development toward cell- and small molecule-delivery platforms and allow discrete and fine-tuning of network properties.
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spelling pubmed-72848022020-06-15 Multivalency Enables Dynamic Supramolecular Host–Guest Hydrogel Formation Ooi, Huey Wen Kocken, Jordy M. M. Morgan, Francis L. C. Malheiro, Afonso Zoetebier, Bram Karperien, Marcel Wieringa, Paul A. Dijkstra, Pieter J. Moroni, Lorenzo Baker, Matthew B. Biomacromolecules [Image: see text] Supramolecular and dynamic biomaterials hold promise to recapitulate the time-dependent properties and stimuli-responsiveness of the native extracellular matrix (ECM). Host–guest chemistry is one of the most widely studied supramolecular bonds, yet the binding characteristics of host–guest complexes (β-CD/adamantane) in relevant biomaterials have mostly focused on singular host–guest interactions or nondiscrete multivalent pendent polymers. The stepwise synergistic effect of multivalent host–guest interactions for the formation of dynamic biomaterials remains relatively unreported. In this work, we study how a series of multivalent adamantane (guest) cross-linkers affect the overall binding affinity and ability to form supramolecular networks with alginate-CD (Alg-CD). These binding constants of the multivalent cross-linkers were determined via NMR titrations and showed increases in binding constants occurring with multivalent constructs. The higher multivalent cross-linkers enabled hydrogel formation; furthermore, an increase in binding and gelation was observed with the inclusion of a phenyl spacer to the cross-linker. A preliminary screen shows that only cross-linking Alg-CD with an 8-arm-multivalent guest results in robust gel formation. These cytocompatible hydrogels highlight the importance of multivalent design for dynamically cross-linked hydrogels. These materials hold promise for development toward cell- and small molecule-delivery platforms and allow discrete and fine-tuning of network properties. American Chemical Society 2020-04-03 2020-06-08 /pmc/articles/PMC7284802/ /pubmed/32243138 http://dx.doi.org/10.1021/acs.biomac.0c00148 Text en Copyright © 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 Ooi, Huey Wen
Kocken, Jordy M. M.
Morgan, Francis L. C.
Malheiro, Afonso
Zoetebier, Bram
Karperien, Marcel
Wieringa, Paul A.
Dijkstra, Pieter J.
Moroni, Lorenzo
Baker, Matthew B.
Multivalency Enables Dynamic Supramolecular Host–Guest Hydrogel Formation
title Multivalency Enables Dynamic Supramolecular Host–Guest Hydrogel Formation
title_full Multivalency Enables Dynamic Supramolecular Host–Guest Hydrogel Formation
title_fullStr Multivalency Enables Dynamic Supramolecular Host–Guest Hydrogel Formation
title_full_unstemmed Multivalency Enables Dynamic Supramolecular Host–Guest Hydrogel Formation
title_short Multivalency Enables Dynamic Supramolecular Host–Guest Hydrogel Formation
title_sort multivalency enables dynamic supramolecular host–guest hydrogel formation
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7284802/
https://www.ncbi.nlm.nih.gov/pubmed/32243138
http://dx.doi.org/10.1021/acs.biomac.0c00148
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