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.

BeDimensional SpA Lungotorrente Secca 30R 16163 Genoa Italy

Center for Advancing Electronics Dresden and Faculty of Chemistry and Food Chemistry Technische Universität Dresden 01062 Dresden Germany

Department of Inorganic Chemistry University of Chemistry and Technology Prague Technicka 5 166 28 Prague 6 Czech Republic

Dipartimento di Chimica e Chimica Industriale Università degli Studi di Genova via Dodecaneso 31 16146 Genoa Italy

Dipartimento di Informatica Bioingegneria Robotica e Ingegneria dei Sistemi Universita Degli Studi di Genova Via All'Opera Pia 13 16145 Genova Italy

Graphene Labs Istituto Italiano di Tecnologia via Morego 30 16163 Genoa Italy

Max Planck Institute of Microstructure Physics Weinberg 2 06120 Halle Germany

Smart Materials Istituto Italiano di Tecnologia Via Morego 30 16163 Genova Italy

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