Traditional synthetic hydrogels for flexible electronic
devices
are mostly derived from nonsustainable polymers, resulting in environmental
pollution. Herein, scalable, moldable, and stretchable ionic hydrogels
are synthesized utilizing two model biopolymers, κ-carrageenan
(κ-CG) and amylopectin (Amy). In such hydrogels, physically
cross-linked κ-CG networks work as a relatively rigid component
to maintain the shape of hydrogels, Amy networks cross-linked by borate/cis-diol
dynamic covalent bonds help to improve the stretchability, and ZnSO4 is introduced as an ionic conductive component. The hydrogels,
denoted as κ-CG/Amy/Zn2+ hydrogels, exhibit acceptable
stretchability (>100%) because of the special cross-linking structure
and ionic conductivity (2.9 S·m–1) due to the
existence of various ions. Flexible mechanosensors (resistive strain
sensors and capacitive pressure sensors) are demonstrated utilizing
κ-CG/Amy/Zn2+ hydrogels, and high gauge factors (0.76
for strain sensors and 0.77 kPa–1 for pressure sensors)
are achieved. Interestingly, κ-CG/Amy/Zn2+ hydrogels
also work as quasi-solid-state electrolytes in zinc-ion hybrid supercapacitors,
which exhibit an initial specific capacity of 47.4 mAh·g–1 at a current density of 3 A·g–1 and stable charge/discharge ability in more than 42,000 cycles.
The sustainable biopolymer hydrogels may provide promising eco-friendly
materials for future wearable devices and energy storage systems.