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@ARTICLE{Ghugare:11790,
author = {Ghugare, S.V. and Chiessi, E. and Telling, M.T.F. and
Deriu, A. and Gerelli, Y. and Wuttke, J. and Paradossi, G.},
title = {{S}tructure and {D}ynamics of a {T}hermoresponsive
{M}icrogel around {I}ts {V}olume {P}hase {T}ransition
{T}emperature},
journal = {The journal of physical chemistry / B},
volume = {114},
issn = {1520-6106},
address = {Washington, DC},
publisher = {Soc.},
reportid = {PreJuSER-11790},
pages = {10285 - 10293},
year = {2010},
note = {This work was partially funded by MIUR-PRIN project
20077LCNTW. S.G. gratefully acknowledges the international
Ph.D. student program of the University of Rome Tor Vergata.
The SPHERES experiment has been supported by the European
Commission under the Seventh Framework Programme through the
Key Action: Strengthening the European Research Area,
Research Infrastructures, Contract no.: 226507 (NMI3). The
IRIS experiment was performed within Agreement No. 01/901
between CCLRC and CNR.},
abstract = {Sustained drug delivery requires the use of multifunctional
devices with enhanced properties. These properties include
responsiveness to external stimuli (such as temperature, pH,
ionic strength), ability to deliver suitably designed
ligands to specific receptors, enhanced bioadhesion to
cells, and cytocompatibility. Microgels represent one of
such multifunctional drug delivery devices. Recently, we
described the fabrication of a stable colloidal aqueous
suspension of cytocompatible microgel spheres based on a
poly(vinyl
alcohol)/poly(methacrylate-co-N-isopropylacrylamide) network
( Ghugare, S. Mozetic, P. Paradossi, G. Biomacromolecules
2009 , 10 , 1589 ). These microgel spheres undergo an
entropy-driven volume phase transition around the
physiological temperature, this phase transition being
driven by the incorporation of NiPAAm residues in the
network. In that study, the microgel was loaded with the
anticancer drug doxorubicin. As the microgel shrank, a
marked increase in the amount of doxorubicin released was
noted. Indeed, dynamic light scattering measurements showed
the diameter reduction to be about $50\%.$ In the present
paper, we focus on some fundamental issues regarding
modifications of the hydrogel architecture at a nanoscopic
level as well as of the diffusive behavior of water
associated with the polymer network around the volume phase
transition temperature (VPTT). Sieving and size exclusion
effects were studied by laser scanning confocal microscopy
with the microgel exposed to fluorescent probes with
different molecular weights. Confocal microscopy
observations at room temperature and at 40 degrees C (i.e.,
below and above the VPTT) provided an evaluation of the
variation of the average pore size (from 5 nm to less than 3
nm). Using quasielastic neutron scattering (QENS) with the
IRIS spectrometer at ISIS, UK, the diffusive behavior of
water molecules closely associated to the polymer network
around the VPTT was investigated. A clear change in the
values of diffusion coefficient of bound water was observed
at the transition temperature. In addition, the local
dynamics of the polymer itself was probed using the QENS
spectrometer SPHERES at FRM II, Germany. For this study, the
microgel was swollen in D(2)O. An average characteristic
distance of about 5 A for the localized chain motions was
evaluated from the elastic incoherent structure factor
(EISF) and from the Q-dependence of the Lorentzian width.},
keywords = {Acrylamides: chemistry / Antibiotics, Antineoplastic:
chemistry / Doxorubicin: chemistry / Drug Delivery Systems /
Hydrogels: chemistry / Materials Testing / Molecular
Structure / Particle Size / Phase Transition /
Polymethacrylic Acids: chemistry / Polyvinyl Alcohol:
chemistry / Transition Temperature / Acrylamides (NLM
Chemicals) / Antibiotics, Antineoplastic (NLM Chemicals) /
Hydrogels (NLM Chemicals) / Polymethacrylic Acids (NLM
Chemicals) / N-isopropylacrylamide (NLM Chemicals) /
Doxorubicin (NLM Chemicals) / Polyvinyl Alcohol (NLM
Chemicals) / J (WoSType)},
cin = {IFF-4 / IFF-5 / Jülich Centre for Neutron Science JCNS
(JCNS) ; JCNS},
ddc = {530},
cid = {I:(DE-Juel1)VDB784 / I:(DE-Juel1)VDB785 /
I:(DE-Juel1)JCNS-20121112},
pnm = {BioSoft: Makromolekulare Systeme und biologische
Informationsverarbeitung / Großgeräte für die Forschung
mit Photonen, Neutronen und Ionen (PNI)},
pid = {G:(DE-Juel1)FUEK505 / G:(DE-Juel1)FUEK415},
experiment = {EXP:(DE-MLZ)SPHERES-20140101},
shelfmark = {Chemistry, Physical},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:20701364},
UT = {WOS:000280727700005},
doi = {10.1021/jp100962p},
url = {https://juser.fz-juelich.de/record/11790},
}