TY - JOUR
T1 - Supramolecular nucleoside-based gel
T2 - molecular dynamics simulation and characterization of its nanoarchitecture and self-assembly mechanism
AU - Angelerou, Maria G. F.
AU - Frederix, Pim W. J. M.
AU - Wallace, Matthew
AU - Yang, Bin
AU - Rodger, Alison
AU - Adams, Dave J.
AU - Marlow, Maria
AU - Zelzer, Mischa
N1 - Copyright the Publisher 2018. Version archived for private and non-commercial use with the permission of the author/s and according to publisher conditions. For further rights please contact the publisher.
Correction to this article published in Langmuir 2019, 35, 7, 2885.
PY - 2018/6/12
Y1 - 2018/6/12
N2 - Amongst the diversity of existing supramolecular hydrogels, nucleic acid-based hydrogels are of particular interest for potential drug delivery and tissue engineering applications because of their inherent biocompatibility. Hydrogel performance is directly related to nanostructure and the self-assembly mechanism of the material, an aspect that is not well understood for nucleic acid-based hydrogels in general and has not yet been explored for cytosine based hydrogels in particular. Herein, we use a broad range of experimental characterization techniques along with molecular dynamics simulations to demonstrate the complementarity and applicability of both approaches for nucleic acid-based gelators in general and propose the self-assembly mechanism for a novel supramolecular gelator, N4-octanoyl-2'-deoxycytidine. The experimental data and the MD simulations are in complete agreement with each other and demonstrate the formation of a hydrophobic core within the fibrillar structures of these mainly water-containing materials. The characterization of the distinct duality of environments in this cytidine based gel will form the basis for further encapsulation of both small hydrophobic drugs and biopharmaceuticals (proteins and nucleic acids) for drug delivery and tissue engineering applications.
AB - Amongst the diversity of existing supramolecular hydrogels, nucleic acid-based hydrogels are of particular interest for potential drug delivery and tissue engineering applications because of their inherent biocompatibility. Hydrogel performance is directly related to nanostructure and the self-assembly mechanism of the material, an aspect that is not well understood for nucleic acid-based hydrogels in general and has not yet been explored for cytosine based hydrogels in particular. Herein, we use a broad range of experimental characterization techniques along with molecular dynamics simulations to demonstrate the complementarity and applicability of both approaches for nucleic acid-based gelators in general and propose the self-assembly mechanism for a novel supramolecular gelator, N4-octanoyl-2'-deoxycytidine. The experimental data and the MD simulations are in complete agreement with each other and demonstrate the formation of a hydrophobic core within the fibrillar structures of these mainly water-containing materials. The characterization of the distinct duality of environments in this cytidine based gel will form the basis for further encapsulation of both small hydrophobic drugs and biopharmaceuticals (proteins and nucleic acids) for drug delivery and tissue engineering applications.
UR - http://www.scopus.com/inward/record.url?scp=85047096205&partnerID=8YFLogxK
UR - https://doi.org/10.1021/acs.langmuir.9b00009
U2 - 10.1021/acs.langmuir.8b00646
DO - 10.1021/acs.langmuir.8b00646
M3 - Article
C2 - 29757652
AN - SCOPUS:85047096205
SN - 0743-7463
VL - 34
SP - 6912
EP - 6921
JO - Langmuir
JF - Langmuir
IS - 23
ER -