The
development of hydrogel-based electronic sensors integrated
with excellent mechanical performance, conductivity, high sensitivity,
and stability is still a great challenge. In this work, a highly strong,
tough, and stretchable conductive hydrogel was proposed using silk
sericin (SS), polyvinyl alcohol (PVA), and sodium citrate (Na3Cit) via combining freeze–thaw with the salting-out
route. SS with rich-binding sites (−COO–,
−NH2, and −OH) was exploited to construct
an ionic conductive hydrogel with multiple physical interactions containing
hydrogen bonds, ionic coordinations, and hydrophobic interactions.
The obtained composite hydrogels (PVA/SS/Na3Cit) displayed
a prominent tensile strength of 4.42 ± 0.32 MPa, an elastic modulus
of 3.14 ± 0.26 MPa, a toughness of 13.73 ± 1.05 MJ/m3, and an excellent stretchability (>500% of strain) and
self-recovery.
In addition, the introduction of SS not only mediated the noncovalent
cross-link network but also enabled excellent ionic conductivity of
the hydrogels due to the coordination effect of Na+ and
Cit3– ions. Moreover, the PVA/SS/Na3Cit
conductive hydrogels can be used as a strain sensor to monitor human
activities, and they exhibit a wide work range, good sensitivity,
and stability, suggesting promising applications in flexible and stretchable
wearable electronics.