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Statements

Subject Item
n2:RIV%2F61389013%3A_____%2F14%3A00432036%21RIV15-GA0-61389013
rdf:type
skos:Concept n18:Vysledek
dcterms:description
Thermoresponsive polymeric surfactant CAE85 is a telechelic carboxyl group derivative of Pluronic P85 and its carboxyl end-groups undergo deprotonation into carboxylate groups upon micellization. Micelle formation and disintegration were studied here by means of small angle X-ray scattering, FTIR and Raman spectroscopy, quantum mechanical calculations and dynamical mechanical analysis. The deprotonation was observed in aqueous solutions of CAE85 for concentrations from 5 wt% to 30 wt% at temperatures above the corresponding critical micellization temperature (CMT). The most likely cause is a difference between the proton dissociation constant of the micelle (pKm) and the proton dissociation constant of the unimers in solution (pKa); our observations indicate that pKm < pKa. For concentrations up to 15 wt%, the presence of carboxylate groups in CAE85 lowered the CMT in comparison with P85. In addition, the behavior of CAE85 was generally not thermo-reversible and reproducible upon cooling. Quantum chemical calculations showed that, in the dense micelle corona, the deprotonated states were more stable than hydrogen-bonded states of neutral molecules, which is likely to affect the equilibrium processes in the micelle. In contrast to the unmodified P85, no gelation was observed in the case of CAE85. By studying the processes at all the levels of organization from nanoscale charge formation through micellization to the macroscale process of gelation, our understanding of polymeric micelle formation may be advanced. Thermoresponsive polymeric surfactant CAE85 is a telechelic carboxyl group derivative of Pluronic P85 and its carboxyl end-groups undergo deprotonation into carboxylate groups upon micellization. Micelle formation and disintegration were studied here by means of small angle X-ray scattering, FTIR and Raman spectroscopy, quantum mechanical calculations and dynamical mechanical analysis. The deprotonation was observed in aqueous solutions of CAE85 for concentrations from 5 wt% to 30 wt% at temperatures above the corresponding critical micellization temperature (CMT). The most likely cause is a difference between the proton dissociation constant of the micelle (pKm) and the proton dissociation constant of the unimers in solution (pKa); our observations indicate that pKm < pKa. For concentrations up to 15 wt%, the presence of carboxylate groups in CAE85 lowered the CMT in comparison with P85. In addition, the behavior of CAE85 was generally not thermo-reversible and reproducible upon cooling. Quantum chemical calculations showed that, in the dense micelle corona, the deprotonated states were more stable than hydrogen-bonded states of neutral molecules, which is likely to affect the equilibrium processes in the micelle. In contrast to the unmodified P85, no gelation was observed in the case of CAE85. By studying the processes at all the levels of organization from nanoscale charge formation through micellization to the macroscale process of gelation, our understanding of polymeric micelle formation may be advanced.
dcterms:title
The effect of micellization-induced deprotonation on the associative behavior of a carboxyl modified Pluronic P85 The effect of micellization-induced deprotonation on the associative behavior of a carboxyl modified Pluronic P85
skos:prefLabel
The effect of micellization-induced deprotonation on the associative behavior of a carboxyl modified Pluronic P85 The effect of micellization-induced deprotonation on the associative behavior of a carboxyl modified Pluronic P85
skos:notation
RIV/61389013:_____/14:00432036!RIV15-GA0-61389013
n3:aktivita
n4:P n4:I
n3:aktivity
I, P(GAP108/12/0703)
n3:cisloPeriodika
40
n3:dodaniDat
n12:2015
n3:domaciTvurceVysledku
Kotov, Nikolay n10:1518755 n10:5536898 n10:1926284 Zhigunov, Alexander
n3:druhVysledku
n17:J
n3:duvernostUdaju
n15:S
n3:entitaPredkladatele
n13:predkladatel
n3:idSjednocenehoVysledku
13398
n3:idVysledku
RIV/61389013:_____/14:00432036
n3:jazykVysledku
n7:eng
n3:klicovaSlova
Pluronic; deprotonation; SAXS
n3:klicoveSlovo
n6:SAXS n6:deprotonation n6:Pluronic
n3:kodStatuVydavatele
GB - Spojené království Velké Británie a Severního Irska
n3:kontrolniKodProRIV
[E1A0CD27A5A4]
n3:nazevZdroje
Soft Matter
n3:obor
n9:CD
n3:pocetDomacichTvurcuVysledku
5
n3:pocetTvurcuVysledku
5
n3:projekt
n11:GAP108%2F12%2F0703
n3:rokUplatneniVysledku
n12:2014
n3:svazekPeriodika
10
n3:tvurceVysledku
Dybal, Jiří Braunová, Alena Šturcová, Adriana Kotov, Nikolay Zhigunov, Alexander
n3:wos
000344998600013
s:issn
1744-683X
s:numberOfPages
12
n8:doi
10.1039/C4SM01337A