Aqueous
zinc-ion hybrid supercapacitors (ZHSCs) represent one of
the current research subjects because of their flame retardancy, ease
of manufacturing, and exceptional roundtrip efficiency. With the evolution
into real useful energy storage cells, the bottleneck factors of the
corrosion and dendrite growth problems must be properly resolved for
largely boosting their cycling life and energy efficiency. Herein,
a natural polysaccharide strengthened hydrogel electrolyte (denoted
as PAAm/agar/Zn(CF3SO3)2) was engineered
by designing an asymmetric dual network of covalently cross-linked
polyacrylamide (denoted as PAAm) and physically cross-linked loose
polysaccharide (e.g., agar) followed by intense uptake of Zn(CF3SO3)2 aqueous electrolyte. In this polymeric
matrix, the PAAm chains are responsible for constructing the soft
domains to immobilize the water molecules, and the agar component
boosts the mechanical performance (by using its inherent reversible
sacrificial bonds) and favors the electrolyte ion transport. Due to
these reasons, the as-designed hydrogel electrolyte effectively inhibits
the zinc dendrite growth, realizes the uniform Zn deposition, and
affords a satisfactory ionic conductivity of 1.55 S m–1, excellent tensile strength (78.9 kPa at 507.7% stretchable), and
high compression strength (118.0 kPa at 60.0% strain). Additionally,
a biopolymer-derived N-doped carbon microsphere cathode material with
a highly interconnected porous carbonaceous network (denoted as NC)
was also synthesized, which delivers a high capacity of 92.8 mAh g–1, along with superb rate capability and long duration
cycling lifespan (95.4% retention for 10000 cycles) in the aqueous
Zn//NC ZHSC. More notably, with integrated merits of the PAAm/agar/Zn(CF3SO3)2 hydrogel electrolyte and NC, the
as-built quasi-solid-state ZHSC achieves a high specific capacity
of 73.4 mAh g–1 and superior energy density of 61.3
Wh kg–1 together with excellent cycling stability
for 10000 cycles. This work demonstrated favorable practicability
in the structural design of the hydrogel electrolytes and electrode
materials for advanced ZHSC applications.