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Binding Mechanism of the Model Charged Dye Carboxyfluorescein to Hyaluronan/Polylysine Multilayers

[Image: see text] Biopolymer-based multilayers become more and more attractive due to the vast span of biological application they can be used for, e.g., implant coatings, cell culture supports, scaffolds. Multilayers have demonstrated superior capability to store enormous amounts of small charged m...

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Autores principales: Prokopovic, Vladimir Z., Vikulina, Anna S., Sustr, David, Shchukina, Elena M., Shchukin, Dmitry G., Volodkin, Dmitry V.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2017
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5682609/
https://www.ncbi.nlm.nih.gov/pubmed/29035502
http://dx.doi.org/10.1021/acsami.7b12449
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author Prokopovic, Vladimir Z.
Vikulina, Anna S.
Sustr, David
Shchukina, Elena M.
Shchukin, Dmitry G.
Volodkin, Dmitry V.
author_facet Prokopovic, Vladimir Z.
Vikulina, Anna S.
Sustr, David
Shchukina, Elena M.
Shchukin, Dmitry G.
Volodkin, Dmitry V.
author_sort Prokopovic, Vladimir Z.
collection PubMed
description [Image: see text] Biopolymer-based multilayers become more and more attractive due to the vast span of biological application they can be used for, e.g., implant coatings, cell culture supports, scaffolds. Multilayers have demonstrated superior capability to store enormous amounts of small charged molecules, such as drugs, and release them in a controlled manner; however, the binding mechanism for drug loading into the multilayers is still poorly understood. Here we focus on this mechanism using model hyaluronan/polylysine (HA/PLL) multilayers and a model charged dye, carboxyfluorescein (CF). We found that CF reaches a concentration of 13 mM in the multilayers that by far exceeds its solubility in water. The high loading is not related to the aggregation of CF in the multilayers. In the multilayers, CF molecules bind to free amino groups of PLL; however, intermolecular CF–CF interactions also play a role and (i) endow the binding with a cooperative nature and (ii) result in polyadsorption of CF molecules, as proven by fitting of the adsorption isotherm using the BET model. Analysis of CF mobility in the multilayers by fluorescence recovery after photobleaching has revealed that CF diffusion in the multilayers is likely a result of both jumping of CF molecules from one amino group to another and movement, together with a PLL chain being bound to it. We believe that this study may help in the design of tailor-made multilayers that act as advanced drug delivery platforms for a variety of bioapplications where high loading and controlled release are strongly desired.
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spelling pubmed-56826092017-11-15 Binding Mechanism of the Model Charged Dye Carboxyfluorescein to Hyaluronan/Polylysine Multilayers Prokopovic, Vladimir Z. Vikulina, Anna S. Sustr, David Shchukina, Elena M. Shchukin, Dmitry G. Volodkin, Dmitry V. ACS Appl Mater Interfaces [Image: see text] Biopolymer-based multilayers become more and more attractive due to the vast span of biological application they can be used for, e.g., implant coatings, cell culture supports, scaffolds. Multilayers have demonstrated superior capability to store enormous amounts of small charged molecules, such as drugs, and release them in a controlled manner; however, the binding mechanism for drug loading into the multilayers is still poorly understood. Here we focus on this mechanism using model hyaluronan/polylysine (HA/PLL) multilayers and a model charged dye, carboxyfluorescein (CF). We found that CF reaches a concentration of 13 mM in the multilayers that by far exceeds its solubility in water. The high loading is not related to the aggregation of CF in the multilayers. In the multilayers, CF molecules bind to free amino groups of PLL; however, intermolecular CF–CF interactions also play a role and (i) endow the binding with a cooperative nature and (ii) result in polyadsorption of CF molecules, as proven by fitting of the adsorption isotherm using the BET model. Analysis of CF mobility in the multilayers by fluorescence recovery after photobleaching has revealed that CF diffusion in the multilayers is likely a result of both jumping of CF molecules from one amino group to another and movement, together with a PLL chain being bound to it. We believe that this study may help in the design of tailor-made multilayers that act as advanced drug delivery platforms for a variety of bioapplications where high loading and controlled release are strongly desired. American Chemical Society 2017-10-16 2017-11-08 /pmc/articles/PMC5682609/ /pubmed/29035502 http://dx.doi.org/10.1021/acsami.7b12449 Text en Copyright © 2017 American Chemical Society This is an open access article published under a Creative Commons Attribution (CC-BY) License (http://pubs.acs.org/page/policy/authorchoice_ccby_termsofuse.html) , which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.
spellingShingle Prokopovic, Vladimir Z.
Vikulina, Anna S.
Sustr, David
Shchukina, Elena M.
Shchukin, Dmitry G.
Volodkin, Dmitry V.
Binding Mechanism of the Model Charged Dye Carboxyfluorescein to Hyaluronan/Polylysine Multilayers
title Binding Mechanism of the Model Charged Dye Carboxyfluorescein to Hyaluronan/Polylysine Multilayers
title_full Binding Mechanism of the Model Charged Dye Carboxyfluorescein to Hyaluronan/Polylysine Multilayers
title_fullStr Binding Mechanism of the Model Charged Dye Carboxyfluorescein to Hyaluronan/Polylysine Multilayers
title_full_unstemmed Binding Mechanism of the Model Charged Dye Carboxyfluorescein to Hyaluronan/Polylysine Multilayers
title_short Binding Mechanism of the Model Charged Dye Carboxyfluorescein to Hyaluronan/Polylysine Multilayers
title_sort binding mechanism of the model charged dye carboxyfluorescein to hyaluronan/polylysine multilayers
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5682609/
https://www.ncbi.nlm.nih.gov/pubmed/29035502
http://dx.doi.org/10.1021/acsami.7b12449
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