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@ARTICLE{Schneider:186324,
author = {Schneider, Florian and Balaceanu, Andreea and Feoktystov,
Artem and Pipich, Vitaliy and Wu, Yaodong and Allgaier, J.
and Pyckhout-Hintzen, Wim and Pich, Andrij and Schneider,
Gerald J.},
title = {{M}onitoring the {I}nternal {S}tructure of {P}oly( {N}
-vinylcaprolactam) {M}icrogels with {V}ariable
{C}ross-{L}ink {C}oncentration},
journal = {Langmuir},
volume = {30},
number = {50},
issn = {1520-5827},
address = {Washington, DC},
publisher = {ACS Publ.},
reportid = {FZJ-2015-00400},
pages = {15317 - 15326},
year = {2014},
abstract = {The combination of a set of complementary techniques allows
us to construct an unprecedented and comprehensive picture
of the internal structure, temperature dependent swelling
behavior, and the dependence of these properties on the
cross-linker concentration of microgel particles based on
N-vinylcaprolactam (VCL). The microgels were synthesized by
precipitation polymerization using different amounts of
cross-linking agent. Characterization was performed by
small-angle neutron scattering (SANS) using two
complementary neutron instruments to cover a uniquely broad
Q-range with one probe. Additionally we used dynamic light
scattering (DLS), atomic force microscopy (AFM), and
differential scanning calorimetry (DSC). Previously obtained
nuclear magnetic resonance spectroscopy (NMR) results on the
same PVCL particles are utilized to round the picture off.
Our study shows that both the particle radius and the
cross-link density and therefore also the stiffness of the
microgels rises with increasing cross-linker content. Hence,
more cross-linker reduces the swelling capability
distinctly. These findings are supported by SANS and AFM
measurements. Independent DLS experiments also found the
increase in particle size but suggest an unchanged
cross-link density. The reason for the apparent
contradiction is the indirect extraction of the parameters
via a model in the evaluation of DLS measurements. The more
direct approach in AFM by evaluating the cross section
profiles of observed microgel particles gives evidence of
significantly softer and more deformable particles at lower
cross-linker concentrations and therefore verifies the
change in cross-link density. DSC data indicate a minor but
unexpected shift of the volume phase transition temperature
(VPTT) to higher temperatures and exposes a more
heterogeneous internal structure of the microgels with
increasing cross-link density. Moreover, a change in the
total energy transfer during the VPT gives evidence that the
strength of hydrogen bonds is significantly affected by the
cross-link density. A strong and reproducible deviation of
the material density of the cross-linked microgel polymer
chains toward a higher value compared to the respective
linear chains has yet to be explained.},
cin = {ICS-1 / Neutronenstreuung ; JCNS-1 / JCNS (München) ;
Jülich Centre for Neutron Science JCNS (München) ;
JCNS-FRM-II},
ddc = {670},
cid = {I:(DE-Juel1)ICS-1-20110106 / I:(DE-Juel1)JCNS-1-20110106 /
I:(DE-Juel1)JCNS-FRM-II-20110218},
pnm = {451 - Soft Matter Composites (POF2-451) / 54G - JCNS
(POF2-54G24)},
pid = {G:(DE-HGF)POF2-451 / G:(DE-HGF)POF2-54G24},
experiment = {EXP:(DE-MLZ)KWS1-20140101 / EXP:(DE-MLZ)KWS3-20140101},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000347140000033},
doi = {10.1021/la503830w},
url = {https://juser.fz-juelich.de/record/186324},
}