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@ARTICLE{Bras:894130,
author = {Bras, Ana and Arizaga, Ana and Agirre, Uxue and Dorau,
Marie and Houston, Judith and Radulescu, Aurel and Kruteva,
Margarita and Pyckhout-Hintzen, Wim and Schmidt, Annette M.},
title = {{C}hain-{E}nd {E}ffects on {S}upramolecular {P}oly(ethylene
glycol) {P}olymers},
journal = {Polymers},
volume = {13},
number = {14},
issn = {2073-4360},
address = {Basel},
publisher = {MDPI},
reportid = {FZJ-2021-03057},
pages = {2235},
year = {2021},
abstract = {In this work we present a fundamental analysis based on
small-angle scattering, linear rheology and differential
scanning calorimetry (DSC) experiments of the role of
different hydrogen bonding (H-bonding) types on the
structure and dynamics of chain-end modified poly(ethylene
glycol) (PEG) in bulk. As such bifunctional PEG with a molar
mass below the entanglement mass Me is symmetrically
end-functionalized with three different hydrogen bonding
(H-bonding) groups: thymine-1-acetic acid (thy),
diamino-triazine (dat) and 2-ureido-4[1H]-pyrimidinone
(upy). A linear block copolymer structure and a
Newtonian-like dynamics is observed for PEG-thy/dat while
results for PEG-upy structure and dynamics reveal a sphere
and a network-like behavior, respectively. These
observations are concomitant with an increase of the
Flory–Huggins interaction parameter from PEG-thy/dat to
PEG-upy that is used to quantify the difference between the
H-bonding types. The upy association into spherical clusters
is established by the Percus–Yevick approximation that
models the inter-particle structure factor for PEG-upy.
Moreover, the viscosity study reveals for PEG-upy a shear
thickening behavior interpreted in terms of the free path
model and related to the time for PEG-upy to dissociate from
the upy clusters, seen as virtual crosslinks of the formed
network. Moreover, a second relaxation time of different
nature is also obtained from the complex shear modulus
measurements of PEG-upy by the inverse of the angular
frequency where G’ and G’’ crosses from the
network-like to glass-like transition relaxation time, which
is related to the segmental friction of PEG-upy polymeric
network strands. In fact, not only do PEG-thy/dat and
PEG-upy have different viscoelastic properties, but the
relaxation times found for PEG-upy are much slower than the
ones for PEG-thy/dat. However, the activation energy related
to the association dynamics is very similar for both
PEG-thy/dat and PEG-upy. Concerning the segmental dynamics,
the glass transition temperature obtained from both
rheological and calorimetric analysis is similar and
increases for PEG-upy while for PEG-thy/dat is almost
independent of association behavior. Our results show how
supramolecular PEG properties vary by modifying the
H-bonding association type and changing the molecular
Flory–Huggins interaction parameter, which can be further
explored for possible applications},
cin = {JCNS-FRM-II / MLZ / JCNS-1 / JCNS-4},
ddc = {540},
cid = {I:(DE-Juel1)JCNS-FRM-II-20110218 / I:(DE-588b)4597118-3 /
I:(DE-Juel1)JCNS-1-20110106 / I:(DE-Juel1)JCNS-4-20201012},
pnm = {6G4 - Jülich Centre for Neutron Research (JCNS) (FZJ)
(POF4-6G4) / 632 - Materials – Quantum, Complex and
Functional Materials (POF4-632)},
pid = {G:(DE-HGF)POF4-6G4 / G:(DE-HGF)POF4-632},
experiment = {EXP:(DE-MLZ)KWS2-20140101},
typ = {PUB:(DE-HGF)16},
pubmed = {34300992},
UT = {WOS:000677180200001},
doi = {10.3390/polym13142235},
url = {https://juser.fz-juelich.de/record/894130},
}