In
this article, we report the supramolecular assemblies of a semirigid
polyelectrolyte, poly(2,2′-disulfonyl-4,4′-benzidine
terephthalamide) (PBDT) in water. Cryo-TEM observation and SAXS measurement
reveal that PBDT forms bundle-like structure even in very dilute concentration, C
P, of 0.02 wt %. These bundle-like assemblies
serve as new primary building blocks and self-assemble further as C
P increases, to form large associations with
or without long-range orientation. When 2 wt % < C
P < 6 wt %, liquid–liquid phase separation occurs.
Some of the supramolecular associations form bipolar liquid crystalline
(LC) droplets via a typical nucleation and growth process. The droplets
grow up by the coalescence of small ones and sediment under the gravity
and coalesce to form a bottom nematic phase. When C
P ≥ 6 wt %, the solutions are in a uniform nematic
phase. The existence of these preliminary supramolecular assemblies
of PBDT in aqueous solutions should be crucial for the formation of
nematic LC phase at a significantly low C
P, as well as the formation of macroscopic ordered structures in hydrogels
via electrostatic interaction between PBDT and oppositely charge multivalent
metallic ion or polycation.
In this paper, we developed several
kinds of ordered structures in hydrogels with different geometries
and sizes by harnessing heterogeneous swelling induced mechanical
instability, i.e., surface creasing, which leads to molecular orientations
along the tensile direction. These hydrogels were synthesized by polymerization
of a cationic monomer, N-[3-(
N,N
-dimethylamino)propyl] acrylamide methyl chloride quaternary
(DMAPAA-Q) and a chemical cross-linker, in the presence of a small
amount of the semirigid polyanion, poly(2,2′-disulfonyl-4,4′-benzidine
terephthalamide) (PBDT), as dopant. During the swelling process of
as-prepared gels, surface creasing occurs and induces formation of
a lattice-like periodic ordered structure, which is maintained in
the swollen gels due to the formation of strong polyion complex. Besides
this structure formed at the central part of gel sheets, PBDTs align
parallel to the gel boundary at the edge of gels with a cuboid, disk,
or ring shape. The size of the two regions with different structures
and the size of each unit of lattice-like pattern are related to the
geometry and size of the gels. The formation of different ordered
structures was found due to the different mechanical instabilities
at different parts of the gel during the heterogeneous swelling. This
work presenting the creation of ordered structures in hydrogels by
tuning the mechanical instability will pave the way to develop other
functional structured materials and merit revealing the formation
mechanism of ordered structures in soft biotissues during the nonequilibrium
growth.
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