Electrochemical deposition of vertically aligned tellurium nanorods on flexible carbon cloth for wearable supercapacitors
Graphical abstract
Introduction
Supercapacitors or electrochemical capacitors are widely recognised as an alternative energy storage device to battery technology due to their high-power density and long cycle-life [1]. The specific properties of supercapacitors, such as their ability to store and deliver peak power demand, ultra-long life-time, and adaptability for the fabrication of flexible devices, promising applications in electric vehicles, maintenance-free energy storage and delivery systems for wearable/portable electronic devices [2], [3], [4]. Carbon-based materials, mainly activated carbon powders, are widely used as supercapacitor electrodes in commercial products and have an energy density ranging from 5 to 10 Wh kg−1 that is 10 to 20 fold lower than batteries [5]. Therefore, the energy density of supercapacitor electrode needs to be boosted to widen their practical applications [6]. Thus, extensive research has been carried out on various materials, including novel carbon materials such as graphene, graphene oxide, graphdiynes, and carbynes as new electrode materials for supercapacitors that can store energy via electrochemical double-layer capacitance [7], [8], [9]. Transition metal-based oxides, hydroxides-, and chalcogenides have also been explored as supercapacitor electrodes due to their pseudocapacitance, either by intrinsic or extrinsic pathways [10]. Among these, low-dimensional materials such as two-dimensional (2D) graphene, MoS2, Mxenes-, and siloxenes are of particular interest as supercapacitor electrodes for wearable/portable energy systems [11], [12] and self-powered energy storage technologies [13], due to their excellent conductivity, structural integrity as textiles and lightweight [14]. Currently, mono-elemental materials or metallenes are expected to have a major impact on the development of energy harvesting, conversion-, and storage-devices during this decade.
Various low dimensional metallic materials such as boronene, phosphorene, selenene, and antimonene have demonstrated improved capacitance for electrochemical energy storage [15], [16]. For example, Li et al. reported superior capacitive properties of few-layered boron sheets (prepared via liquid-phase exfoliation) with a high energy density (46.1 Wh kg−1) and power density (478.5 W kg−1) in an ionic liquid electrolyte; these properties are superior to those of commercial supercapacitors [17]. Tao et al. reviewed the applications of 2D phosphorene as a novel electrode material for various electrochemical energy storage devices including batteries (Li-ion, Na-ion, K-ion, and Li-S) and supercapacitors (conventional and micro-) [18]. Patil et al. reported that sponge-like selenium thin films prepared by electrodeposition had a specific capacitance of 29.25 F g−1 at 5 mV s−1 in 1 M Na2SO4 electrolyte [19]. We recently reported the energy harvesting and storage properties of antimonene nanodendrites grown on Ni foam via electrochemical deposition; which possess a high specific capacity of about 1618.41 mA h g−1 [20]. Lately, Yang et al. reported liquid-phase exfoliated bismuthene sheets as supercapacitor electrodes having high volumetric capacitance (36.8 F cm−3) [21]. In this context, low-dimensional tellurium (Te) nanostructures are promising metallic materials for diverse applications including thermoelectric energy harvesting, photodetectors, field-effect transistors, piezoelectric energy harvesting, and chemical sensors [22], [23], [24]. In the recent times, nanostructured Te was explored as a potential electrode for next-generation energy storage devices including (i) K-ion, (ii) tellurium–aluminium and (iii) potassium–tellurium batteries [25], [26], [27]. Importantly, Te possesses exceptional environmental stability, which is prime consideration for commercialization [22]. The supercapacitive properties of low- dimensional Te nanostructures have not yet been explored adequately and research concerning the charge-storage properties of such nanostructures is warranted. Herein, we demonstrate a facile electrochemical deposition process (EDP) for the growth of uniform Te nanorods vertically aligned on the surface of carbon cloth (CC) and explored their use in wearable supercapacitors (WSCs). Regarding the methods available for growing Te nanostructures such as hydrothermal, solid-state reaction, chemical vapour deposition, and liquid-phase exfoliation methods [22], [23], the electrochemical deposition possesses many merits including rapid and controlled growth of uniform nanostructures [20], [28], green synthesis methodology [29] and direct integration of nanostructures on the current collector [30]. Herein, the supercapacitive properties of electrochemically deposited Te nanostructures were studied in detail by fabricating and investigating the charge-storage process of a solid-state symmetric supercapacitor based on tetraethylammonium tetrafluoroborate (TEABF4) ionogel.
Section snippets
Materials
Tellurium oxide (TeO2) and polyvinylidene fluoride-co-hexafluoropropylene (PVDF-co-HFP) were purchased from Sigma Aldrich, South Korea. The TEABF4 electrolyte was acquired from Alfa Aesar, South Korea. Ammonium hydroxide and dimethylacetamide (DMAC) were procured from Dae-Jung Chemicals and Metals, South Korea. Chemicals and solvents were all analytical grade and used as received without any further purification. Carbon cloth of 0.33 mm thickness was purchased from Fuel cell store, South Korea.
Growth of tellurium nanorods on flexible carbon cloth substrate
Results and discussion
Fig. 1(A) schematically illustrates the EDP used to grow low-dimensional Te nanorods uniformly on the surface of CC. Here, CC functions as a conductive substrate to grow of Te nanorods and was used instead of metallic foams (Ni and Cu), because CC-based devices can be easily integrated with the wearable devices [31]. The mechanism of Te growth on the CC surface is based on dissolution followed by electrochemical reduction, as previously described [32]. The growth solution consists of TeO2
Conclusion
This research reports a facile electrochemical deposition method for preparing Te-CC and its application in a WSC. The physicochemical characterizations including XRD, Raman spectroscopy, XPS and FE-SEM confirmed the growth of low-dimensional Te nanorods aligned along the CC backbone. The symmetric type WSC fabricated using the Te-CC as electrodes with ionogel electrolyte operated over a wide OVW of 1.5 V, while maintaining excellent performance metrics such as high capacitance (235.6 F g−1),
Declaration of Competing Interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgments
This research work was supported by the Basic Science Research Program through the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (2019R1A2C3009747, 2020R1A2C2007366 and 2021R1A4A2000934).
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These authors contributed equally.