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@ARTICLE{Lund:18197,
author = {Lund, R. and Willner, L. and Pipich, V. and Grillo, I. and
Lindner, P. and Colmenero, J. and Richter, D.},
title = {{E}quilibrium {C}hain {E}xchange {K}inetics of {D}iblock
{C}opolymer {M}icelles: {E}ffect of {M}orphology
{M}acromolecules},
journal = {Macromolecules},
volume = {44},
issn = {0024-9297},
address = {Washington, DC},
publisher = {Soc.},
reportid = {PreJuSER-18197},
pages = {6145 - 6154},
year = {2011},
note = {The authors acknowledge support of the European Community
within the Soft Comp Network of Excellence (NoE) program.
R.L. and J.C. also acknowledge support from the following
grants: GIC07/35-IT-463-07, MAT2007-63681, and
CSD2006-00053.},
abstract = {In this work, we present the chain exchange kinetics in
block copolymer micelles of spherical and cylindrical
geometry. The aim of this work was to understand the
mechanisms controlling the molecular exchange with a
particular focus to delineate any potential effect of the
micellar morphology. As model system symmetric short-chain
amphiphilic poly(ethylene-alt-propylene)-poly(ethylene
oxide) diblock copolymer (PEP1-PEO1, numbers denote
approximate molecular weight in l(D) in aqueous solutions
has been used. This system undergoes a irreversible cylinder
to sphere transition upon addition of N,N-dimethylformamide
(DMF) as cosolvent or upon heating. This feature allowed to
quantitatively compare chain exchange kinetics in both
morphologies. The kinetics were accessed by using
hydrogen/deuterium labeling and time-resolved small-angle
neutron scattering experiments employing a stopped flow
apparatus by which the kinetics could be followed from about
some hundreds of milliseconds up to hours. The results show
that, independent of morphology, all data can be
satisfactorily described by a scaling model that takes into
account the polydispersity of the core forming PEP block in
order to describe the broad logarithmic time decay at longer
times. A small but significant effect of the morphology
could be seen which was reflected in a slightly accelerated
kinetics for spherical micelles. A detailed comparison shows
that for both morphologies, the activation energy follows a
scaling law proportional to the product of the interfacial
tension, gamma, and the number of repeat units of the,
insoluble block, N-B, i.e., E-a similar to gamma N-B rather
than the gamma N-B(2/3) predicted by Halperin and Alexander.
This implies a stretched conformation of the insoluble block
during the expulsion process compared to the more globular
shape considered in the original scaling theory. This can be
related to insufficient chain length/statistics for these
rather small chains to form a globule during the expulsion
process; or to an higher polymer density within the corona
of these "crew cut" type micelles. Through the analysis, the
faster kinetics could be summarized in a slightly smaller
activation energy for the spherical micelles which is
probably related to small changes in the internal corona
structure.},
keywords = {J (WoSType)},
cin = {ICS-1 / JCNS (München) ; Jülich Centre for Neutron
Science JCNS (München) ; JCNS-FRM-II / JCNS-1 / JCNS-2},
ddc = {540},
cid = {I:(DE-Juel1)ICS-1-20110106 /
I:(DE-Juel1)JCNS-FRM-II-20110218 /
I:(DE-Juel1)JCNS-1-20110106 / I:(DE-Juel1)JCNS-2-20110106},
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)KWS2-20140101},
shelfmark = {Polymer Science},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000293353800041},
doi = {10.1021/ma200532r},
url = {https://juser.fz-juelich.de/record/18197},
}