Conductive
hydrogels, exhibiting wide applications in electronic
skins and soft wearable sensors, often require maturely regulating
of the hydrogel mechanical properties to meet specific demands and
work for a long-term or under extreme environment. However, in situ regulation of the mechanical properties of hydrogels
is still a challenge, and regular conductive hydrogels will inevitably
freeze at subzero temperature and easily dehydrate, which leads to
a short service life. Herein, a novel adhesive hydrogel (PAA-Dopa-Zr4+) capable of strain sensing is proposed with antifreezing,
nondrying, strong surface adhesion, and tunable mechanical properties.
3,4-Dihydroxyphenyl-l-alanine (l-Dopa)-grafted
poly(acrylic acid) (PAA) and Zr4+ ion are introduced into
the hydrogel, which broadly alters the mechanical properties via tuning
the in situ aggregation state of polymer chains by
ions based on the complexation effect. The catechol groups of l-Dopa and viscous glucose endow the hydrogel with high adhesiveness
for skin and device interface (including humid and dry environments)
and exhibit an outstanding temperature tolerance under extreme wide
temperature spectrum (−35 to 65 °C) or long-lasting moisture
retention (60 days). Furthermore, this PAA-Dopa-Zr4+ can
be assembled as a flexible strain-sensitive sensor to detect human
motions based on specific mechanical properties requirements. This
work, enabling superior adhesive and temperature tolerance performance
and broad mechanical tenability, presents a new paradigm for numerous
applications to wearable sensing and personalized healthcare monitoring.