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      Functionalized Metallic 2D Transition Metal Dichalcogenide-Based Solid-State Electrolyte for Flexible All-Solid-State Supercapacitors

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          Abstract

          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-NbS 2) nanoflakes, into a sulfonated poly(ether ether ketone) (SPEEK) polymeric matrix. The terminal sulfonate groups in f-NbS 2 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.

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          Most cited references162

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          A comprehensive review on PEM water electrolysis

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            A review of electrolyte materials and compositions for electrochemical supercapacitors.

            Electrolytes have been identified as some of the most influential components in the performance of electrochemical supercapacitors (ESs), which include: electrical double-layer capacitors, pseudocapacitors and hybrid supercapacitors. This paper reviews recent progress in the research and development of ES electrolytes. The electrolytes are classified into several categories, including: aqueous, organic, ionic liquids, solid-state or quasi-solid-state, as well as redox-active electrolytes. Effects of electrolyte properties on ES performance are discussed in detail. The principles and methods of designing and optimizing electrolytes for ES performance and application are highlighted through a comprehensive analysis of the literature. Interaction among the electrolytes, electro-active materials and inactive components (current collectors, binders, and separators) is discussed. The challenges in producing high-performing electrolytes are analyzed. Several possible research directions to overcome these challenges are proposed for future efforts, with the main aim of improving ESs' energy density without sacrificing existing advantages (e.g., a high power density and a long cycle-life) (507 references).
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              A review on recent advances in hybrid supercapacitors: Design, fabrication and applications

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                Author and article information

                Journal
                ACS Nano
                ACS Nano
                nn
                ancac3
                ACS Nano
                American Chemical Society
                1936-0851
                1936-086X
                04 October 2022
                25 October 2022
                : 16
                : 10
                : 16426-16442
                Affiliations
                []Graphene Labs, Istituto Italiano di Tecnologia , via Morego 30, 16163 Genoa, Italy
                []Center for Advancing Electronics Dresden (CFAED) & Faculty of Chemistry and Food Chemistry, Technische Universität Dresden , 01062 Dresden, Germany
                [§ ]BeDimensional SpA , Lungotorrente Secca 30R, 16163 Genoa, Italy
                []Dipartimento di Chimica e Chimica Industriale, Università degli Studi di Genova , via Dodecaneso 31, 16146 Genoa, Italy
                []Smart Materials, Istituto Italiano di Tecnologia , Via Morego 30, 16163 Genova, Italy
                [# ]Dipartimento di Informatica Bioingegneria, Robotica e Ingegneria dei Sistemi (DIBRIS), Universita Degli Studi di Genova , Via All’Opera Pia 13, 16145 Genova, Italy
                []Department of Inorganic Chemistry, University of Chemistry and Technology Prague , Technicka 5, 166 28 Prague 6, Czech Republic
                []Max Planck Institute of Microstructure Physics , Weinberg 2, 06120 Halle, Germany
                Author notes
                Author information
                https://orcid.org/0000-0002-1391-4448
                https://orcid.org/0000-0001-7238-9420
                Article
                10.1021/acsnano.2c05640
                9620411
                36194759
                f31d71e0-c0be-4c6a-a374-6f425858a221
                © 2022 The Authors. Published by American Chemical Society

                Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained ( https://creativecommons.org/licenses/by/4.0/).

                History
                : 08 June 2022
                : 23 September 2022
                Funding
                Funded by: H2020 Future and Emerging Technologies, doi 10.13039/100010664;
                Award ID: 881603
                Funded by: Grantová Agentura Ceské Republiky, doi 10.13039/501100001824;
                Award ID: 20-16124J
                Funded by: H2020 Marie Sklodowska-Curie Actions, doi 10.13039/100010665;
                Award ID: 813036
                Funded by: H2020 Future and Emerging Technologies, doi 10.13039/100010664;
                Award ID: 957273
                Categories
                Article
                Custom metadata
                nn2c05640
                nn2c05640

                Nanotechnology
                solid-state supercapacitors,transition metal dichalcogenides,niobium disulfide,functionalization,flexibility

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