The
design of three-dimensional crosslinked units with a spatial
structure is of great significance for improving the mechanical properties
of hydrogels. However, almost all the nanocomposites incorporated
in hydrogels were defined as rigid nanofillers without further discussion
on the potential contribution from the spatial structure change. In
this work, the 3D nano chemical crosslinker multilayer graphene oxide
acrylate (mGOa) was developed as a pressure-responsive crosslinker
to achieve both low elastic modulus and high compression stress by
synergizing more polymer chains against the loading force through
interlayer sliding. Results showed that the hydrogel crosslinked by
only 2 mg/mL mGOa nano chemical crosslinker in the poly(2-hydroxyethyl
methacrylate-co-acrylamide) hydrogel (molar ratio:
1:1) can effectively enhance the mechanical strength up to 14.1 ±
2.1 MPa at a high compressive strain (90.6%) with an elastic modulus
of less than 0.03 MPa at the initial 5% compression, whereas the hydrogel
crosslinked by methacrylated single-layer graphene oxide (sGOa) or
a small-molecule chemical crosslinker, N,N′-methylene bisacrylamide, can only reach 2.3 ±
0.8 MPa and 1.4 ± 0.4 MPa, respectively. In addition, the instantaneous
modulus of the mGOa crosslinked hydrogel rapidly increased to the
peak value with the increase of strain. The repeated compression test
of HcA-mGOa hydrogels showed the responsive increase of the modulus,
which was promoted by the synergism of polymer chains under compression.
This indicated that the interlayer sliding of mGOa is the key contributor
to mechanical strength enhancement, which provides a new rationale
to design tough hydrogels.