Intramicrogel Complexation of Oppositely Charged Compartments
As a Route to Quasi-Hollow Structures
Posted on 2017-05-22 - 18:51
We
have predicted using computer simulations and have detected
with SAXS measurements that pH-sensitive core–shell polyampholyte
microgels can form a dense layer (“skin”) at the core–shell
interface. The microgels have cationic core and neutral shell at low
pH, whereas the core becomes neutral and the shell becomes anionic
at high pH. The core and shell are oppositely charged at intermediate
pH values. The layer formation is a result of the electrostatic complexation
between oppositely charged subchains. We have studied microgels with
different core–shell ratios and fractions of ionizable groups
and analyzed radial distribution of polymer volume fraction and volume
fractions of cationic and anionic groups. We have demonstrated that
in many cases complexation of oppositely charged subchains (intermediate
pH values) or swelling of charged core with neutral shell (low pH)
are responsible for the formation of quasi-hollow structures with
a loose core of strongly swollen subchains and dense shell of interpenetrating
core- and shell-forming subchains. The most pronounced quasi-hollow
structures are predicted in computer simulations for highly charged
microgels. On the contrary, practically homogeneous swelling of the
microgels is observed at high pH, when electrostatics-driven swelling
of the anionic shell promotes swelling of the neutral core. All structures
are colloidally stable due to the spatial segregation of the opposite
charges. Therefore, the microgels can be useful as carriers for pH-controlled
uptake, storage, and release of neutral guest molecules, which can
be trapped within the microgel at low and intermediate pH and released
at high pH.
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Rudov, Andrey
A.; P. H. Gelissen, Arjan; Lotze, Gudrun; Schmid, Andreas; Eckert, Thomas; Pich, Andrij; et al. (2017). Intramicrogel Complexation of Oppositely Charged Compartments
As a Route to Quasi-Hollow Structures. ACS Publications. Collection. https://doi.org/10.1021/acs.macromol.7b00553
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AUTHORS (8)
AR
Andrey
A. Rudov
AP
Arjan P. H. Gelissen
GL
Gudrun Lotze
AS
Andreas Schmid
TE
Thomas Eckert
AP
Andrij Pich
WR
Walter Richtering
IP
Igor I. Potemkin