Optimizing chemistry at the surface of prodrug-loaded cellulose nanofibrils with MAS-DNP

Studying the surface chemistry of functionalized cellulose nanofibrils at atomic scale is an ongoing challenge, mainly because FT-IR, NMR, XPS and RAMAN spectroscopy are limited in sensitivity or resolution. Herein, we show that dynamic nuclear polarization (DNP) enhanced (13)C and (15)N solid-state...

Descripción completa

Detalles Bibliográficos
Autores principales: Kumar, Akshay, Watbled, Bastien, Baussanne, Isabelle, Hediger, Sabine, Demeunynck, Martine, De Paëpe, Gaël
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Article
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10049993/
https://www.ncbi.nlm.nih.gov/pubmed/36977767
http://dx.doi.org/10.1038/s42004-023-00852-2
_version_ 1785014582684680192
author Kumar, Akshay
Watbled, Bastien
Baussanne, Isabelle
Hediger, Sabine
Demeunynck, Martine
De Paëpe, Gaël
author_facet Kumar, Akshay
Watbled, Bastien
Baussanne, Isabelle
Hediger, Sabine
Demeunynck, Martine
De Paëpe, Gaël
author_sort Kumar, Akshay
collection PubMed
description Studying the surface chemistry of functionalized cellulose nanofibrils at atomic scale is an ongoing challenge, mainly because FT-IR, NMR, XPS and RAMAN spectroscopy are limited in sensitivity or resolution. Herein, we show that dynamic nuclear polarization (DNP) enhanced (13)C and (15)N solid-state NMR is a uniquely suited technique to optimize the drug loading on nanocellulose using aqueous heterogenous chemistry. We compare the efficiency of two conventional coupling agents (DMTMM vs EDC/NHS) to bind a complex prodrug of ciprofloxacin designed for controlled drug release. Besides quantifying the drug grafting, we also evidence the challenge to control the concurrent prodrug adsorption and to optimize washing procedures. We notably highlight the presence of an unexpected prodrug cleavage mechanism triggered by carboxylates at the surface of the cellulose nanofibrils.
format Online
Article
Text
id pubmed-10049993
institution National Center for Biotechnology Information
language English
publishDate 2023
publisher Nature Publishing Group UK
record_format MEDLINE/PubMed
spelling pubmed-100499932023-03-30 Optimizing chemistry at the surface of prodrug-loaded cellulose nanofibrils with MAS-DNP Kumar, Akshay Watbled, Bastien Baussanne, Isabelle Hediger, Sabine Demeunynck, Martine De Paëpe, Gaël Commun Chem Article Studying the surface chemistry of functionalized cellulose nanofibrils at atomic scale is an ongoing challenge, mainly because FT-IR, NMR, XPS and RAMAN spectroscopy are limited in sensitivity or resolution. Herein, we show that dynamic nuclear polarization (DNP) enhanced (13)C and (15)N solid-state NMR is a uniquely suited technique to optimize the drug loading on nanocellulose using aqueous heterogenous chemistry. We compare the efficiency of two conventional coupling agents (DMTMM vs EDC/NHS) to bind a complex prodrug of ciprofloxacin designed for controlled drug release. Besides quantifying the drug grafting, we also evidence the challenge to control the concurrent prodrug adsorption and to optimize washing procedures. We notably highlight the presence of an unexpected prodrug cleavage mechanism triggered by carboxylates at the surface of the cellulose nanofibrils. Nature Publishing Group UK 2023-03-28 /pmc/articles/PMC10049993/ /pubmed/36977767 http://dx.doi.org/10.1038/s42004-023-00852-2 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Kumar, Akshay
Watbled, Bastien
Baussanne, Isabelle
Hediger, Sabine
Demeunynck, Martine
De Paëpe, Gaël
Optimizing chemistry at the surface of prodrug-loaded cellulose nanofibrils with MAS-DNP
title Optimizing chemistry at the surface of prodrug-loaded cellulose nanofibrils with MAS-DNP
title_full Optimizing chemistry at the surface of prodrug-loaded cellulose nanofibrils with MAS-DNP
title_fullStr Optimizing chemistry at the surface of prodrug-loaded cellulose nanofibrils with MAS-DNP
title_full_unstemmed Optimizing chemistry at the surface of prodrug-loaded cellulose nanofibrils with MAS-DNP
title_short Optimizing chemistry at the surface of prodrug-loaded cellulose nanofibrils with MAS-DNP
title_sort optimizing chemistry at the surface of prodrug-loaded cellulose nanofibrils with mas-dnp
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10049993/
https://www.ncbi.nlm.nih.gov/pubmed/36977767
http://dx.doi.org/10.1038/s42004-023-00852-2
work_keys_str_mv AT kumarakshay optimizingchemistryatthesurfaceofprodrugloadedcellulosenanofibrilswithmasdnp
AT watbledbastien optimizingchemistryatthesurfaceofprodrugloadedcellulosenanofibrilswithmasdnp
AT baussanneisabelle optimizingchemistryatthesurfaceofprodrugloadedcellulosenanofibrilswithmasdnp
AT hedigersabine optimizingchemistryatthesurfaceofprodrugloadedcellulosenanofibrilswithmasdnp
AT demeunynckmartine optimizingchemistryatthesurfaceofprodrugloadedcellulosenanofibrilswithmasdnp
AT depaepegael optimizingchemistryatthesurfaceofprodrugloadedcellulosenanofibrilswithmasdnp

Ejemplares similares