Highly efficient
and durable flexible solid-state supercapacitors
(FSSSCs) are emerging as low-cost devices for portable and wearable
electronics due to the elimination of leakage of toxic/corrosive liquid
electrolytes and their capability to withstand elevated mechanical
stresses. Nevertheless, the spread of FSSSCs requires the development
of durable and highly conductive solid-state electrolytes, whose electrochemical
characteristics must be competitive with those of traditional liquid
electrolytes. Here, we propose an innovative composite solid-state
electrolyte prepared by incorporating metallic two-dimensional group-5
transition metal dichalcogenides, namely, liquid-phase exfoliated
functionalized niobium disulfide (f-NbS2) nanoflakes, into
a sulfonated poly(ether ether ketone) (SPEEK) polymeric matrix. The
terminal sulfonate groups in f-NbS2 nanoflakes interact
with the sulfonic acid groups of SPEEK by forming a robust hydrogen
bonding network. Consequently, the composite solid-state electrolyte
is mechanically/dimensionally stable even at a degree of sulfonation
of SPEEK as high as 70.2%. At this degree of sulfonation, the mechanical
strength is 38.3 MPa, and thanks to an efficient proton transport
through the Grotthuss mechanism, the proton conductivity is as high
as 94.4 mS cm–1 at room temperature. To elucidate
the importance of the interaction between the electrode materials
(including active materials and binders) and the solid-state electrolyte,
solid-state supercapacitors were produced using SPEEK and poly(vinylidene
fluoride) as proton conducting and nonconducting binders, respectively.
The use of our solid-state electrolyte in combination with proton-conducting
SPEEK binder and carbonaceous electrode materials (mixture of activated
carbon, single/few-layer graphene, and carbon black) results in a
solid-state supercapacitor with a specific capacitance of 116 F g–1 at 0.02 A g–1, optimal rate capability
(76 F g–1 at 10 A g–1), and electrochemical
stability during galvanostatic charge/discharge cycling and folding/bending
stresses.