Binder free and high performance of sputtered tungsten nitride thin film electrode for supercapacitor device

Here, we demonstrates the fabrication of binder free and very efficient supercapacitor electrode based on tungsten nitride (W₂N) thin film on stainless steel (SS) substrate using reactive sputtering technique. W₂N thin film as a working electrode exhibits high specific capacitance (163 F g⁻¹ at 0.5 mA cm⁻² in 1 M H₂SO₄) along with excellent cycling stability. The binder free symmetric supercapacitor (W₂N||W₂N) device delivers a high specific capacitance (80 Fg^-1) and long life span (90.46% capacitance retention after 10,000 cycles) along with high energy (12.92 Whkg⁻¹) and power (∼674 kWkg⁻¹ at 9.36 Whkg⁻¹) densities. These observed excellent electrochemical performances of the present W₂N thin film based supercapacitor device, recommend it as a potential candidate for energy storage applications.     

Sol-gel synthesis of ternary conducting polymer hydrogel for application in all-solid-state flexible supercapacitor

In this contribution, we reported the preparation of a novel conducting polymer hydrogel (CPH) by a sol-gel method, which was subsequently employed to fabricate a flexible all-solid-state supercapacitor device. Taking advantage of the synergistic effects of the different components in the conducting polymer hydrogel and the merits of the proposed synthesis strategies, the prepared supercapacitor device with CPH as electrode exhibited high area-normalized capacitance (2.2 F cm⁻²), high gravimetric capacitance (1573.6 F g⁻¹) as well as high energy density of 0.18 mWh cm⁻² (or 128.7 Wh Kg⁻¹) at 0.08  mW cm⁻² (or 55.1 W kg⁻¹). This study did not only represent a novel all-solid-state, high performance, flexible supercapacitor with potential applications in flexible energy-related devices, but also developed a new method for enhancing capacitances and mechanical stability of all-solid-state flexible supercapacitor.     

Facile one pot sonochemical synthesis of CoFe2O4/MWCNTs hybrids with well-dispersed MWCNTs for asymmetric hybrid supercapacitor applications

In this study, a facile sonochemical strategy is used for the fabrication of CoFe₂O₄/MWCNTs hybrids as an electrode material for supercapacitor applications. FE-SEM image demonstrates the uniformly well-distributed MWCNTs as well as porous structures in the prepared CoFe₂O₄/MWCNTs hybrids, suggesting 3D network formation of conductive pathway, which can enhance the charge and mass transport properties between the electrodes and electrolytes during the faradic redox reactions. The as-fabricated CoFe₂O₄/MWCNTs hybrids with the MWCNTs concentration of 15 mg (CFC15) delivers maximum specific capacitance of 390 F g⁻¹ at a current density of 1 mA cm⁻², excellent rate capability (275 F g⁻¹ at 10 mA cm⁻²), and outstanding cycling stability (86.9% capacitance retention after 2000 cycles at 3 mA cm⁻²). Furthermore, the electrochemical performance of the CFC15 is superior to those of pure CoFe₂O₄ and other CoFe₂O₄/MWCNTs hybrids (CFC5, CFC10 and CFC20), indicating well-dispersion MWCNTs and uniform porous structures. Also, as-fabricated asymmetric supercapacitor device using the CoFe₂O₄/MWCNTs hybrids as the positive electrode and activated carbon as the negative electrode materials shows the outstanding supercapacitive performance (high specific capacitance, superior cycling stability and good rate capability) for energy storage devices. It delivers a capacitance value of 81 F g⁻¹ at 3 mA cm⁻², ca. 92% retention of its initial capacitance value after 2000 charge-discharge cycles and excellent energy density (26.67 W h kg⁻¹) at high power density (~319 W kg⁻¹).     

Co-precipitation synthesis of nickel cobalt hexacyanoferrate for binder-free high-performance supercapacitor electrodes

Prussian blue analogue with a typical metal-organic framework has been widely used as an electrode material in supercapacitor. In this work, nickel cobalt hexacyanoferrate (Ni₂CoHCF) was grown on nickel foam directly using a simple co-precipitation method. The as-prepared Ni₂CoHCF was tested by transmission electron microscope, scanning electron microscope, X-ray diffraction and X-ray electron energy spectrum. The results showed that Ni₂CoHCF has a unique open face-centered cubic structure. The Ni₂CoHCF was used to set an asymmetric supercapacitor directly. A series of electrochemical tests showed that Ni₂CoHCF had an excellent electrochemical performance. The specific capacitance of the supercapacitor was 585 C g⁻¹ (1300.0 F g⁻¹, 162.5 mAh g⁻¹) at the current density of 0.5 A g⁻¹. After 2000 cycles, it still maintained 85.57% of its initial specific capacitance at the current density of 10 A g⁻¹. The energy density was 30.59 Wh kg⁻¹ at the power density of 378.7 W kg⁻¹. The results show that the supercapacitor constructed by Ni₂CoHCF as an electrode material has high-current charge-discharge capacity, high energy density and long cycle life.     

High-density oxygen-enriched graphene hydrogels for symmetric supercapacitors with ultrahigh gravimetric and volumetric performance

The contradiction between the porous structure and density of graphene materials makes it unable to meet the dual requirements of the next generation supercapacitors for gravimetric capacitance and volumetric capacitance. Herein, we successfully synthesized high-density oxygen-enriched graphene hydrogels (HOGHs) by a one-step hydrothermal method using high concentration graphene oxide (GO) solution and trometamol as precursors. The as-prepared HOGHs samples present a dense 3D network structure and moderate specific surface areas, which leads to a high packing density. In addition, the HOGHs samples also contain abundant oxygen-containing functional groups and some nitrogen-containing functional groups. These heteroatomic functional groups can provide pseudocapacitance for the electrode materials. Therefore, the HOGH-140 based symmetric supercapacitor shows ultrahigh gravimetric and volumetric specific capacitance (325.7 F g⁻¹, 377.8 F cm⁻³), excellent rate performance and cycling stability. Simultaneously, the symmetric binder-free supercapacitor exhibits high gravimetric specific energy density (11.3 Wh kg⁻¹) and volumetric specific energy density (13.1 Wh L⁻¹) in 6 M KOH, respectively. These outstanding properties make the material have a good application prospect in the field of compact energy storage devices.     

Walnut shell-derived hierarchical porous carbon with high performances for electrocatalytic hydrogen evolution and symmetry supercapacitors

Walnut Shell-derived hierarchical porous carbon has been successfully synthesized by the efficient KOH activation process. The hierarchical porous carbon material activated at 600 °C, has the specific micropore area of 1037.31 m² g⁻¹ and micropore volume of 0.51 cm³ g⁻¹, which leads to have electrochemical performances of the hydrogen evolution reaction (HER) and supercapacitors. Specifically, as the hydrogen evolution reaction electrocatalyst, the walnut shell-derived carbon material activated at 600 °C exhibits a lower onset potential of 6.00 mV, a smaller Tafel slope of 69.76 mV dec⁻¹ and outstanding stability above long-term cycling. As a supercapacitor electrode material, the sample possesses specific capacitance of 262.74 F g⁻¹ at 0.5 A g⁻¹, the remarkable rate capability of 224.60 F g⁻¹ at even 10 A g⁻¹ and good long-term stability. A symmetric supercapacitor shows the highly energy density of 7.97 Wh kg⁻¹ at a power density of 180.80 W kg⁻¹. This novel and low-cost biomass material is very promising for the electrocatalytic water splitting and supercapacitors.     

Formation of hierarchical 3D cross-linked porous carbon with small addition of graphene for supercapacitors

In the present paper, starch was used as raw material to prepare carbon material with low-temperature hydrothermal route and hierarchical three-dimensional cross-linked porous carbon was successfully synthesized with the help of a small amount of graphene for high-performance supercapacitors. It's found that presence of graphene is a crucial condition for the formation of 3D porous carbon and graphene acts as a skeleton in the porous carbon. This kind of carbon material exhibited very high surface area of 1887.8 m² g⁻¹ and delivered excellent electrochemical performance. Its specific capacitance can reach 141 F g⁻¹ at 0.5 A g⁻¹ and more importantly, after 10,000 cycles 98.6% of initial specific capacitance can be maintained. To explore the practical application of the 3D porous carbon, an asymmetric supercapacitor coin-type device was assembled with 3D porous carbon and graphene as electrode materials in organic electrolyte. The constructed device exhibited high energy density of 48.5 Wh·kg⁻¹ at a power density of 1.5 kW kg⁻¹ and still maintains 39.625 Wh·kg⁻¹ under the high power density (15 kW kg⁻¹). These results will promote the rapid development of 3D porous carbon prepared by low-temperature route and the application in supercapacitors.     

One-pot sonochemical synthesis of hierarchical MnWO4 microflowers as effective electrodes in neutral electrolyte for high performance asymmetric supercapacitors

In this article, manganese tungstate (MnWO₄) microflowers as electrode materials for high performance supercapacitor applications are prepared by a one-pot sonochemical synthesis. The crystalline structure and morphology of MnWO₄ microflowers are characterized through X-ray diffraction, field emission scanning electron microscopy. The electrochemical properties of the MnWO₄ microflowers are investigated using cyclic voltammograms, galvanostatic charge/discharge and electrochemical impedance spectroscopy. The MnWO₄ microflowers as electrode materials possess a maximum specific capacitance of 324 F g⁻¹ at 1 mA cm⁻² in the potential window from 0 to +1 V and an excellent cycling stability of 93% after 8000 cycles at a current density of 3 mA cm⁻². An asymmetric supercapacitor device is fabricated using the MnWO₄ and iron oxide (Fe₃O₄)/multi-wall carbon nanotube as the positive and negative electrode materials, it can be cycled reversibly at a potential window at 1.8 V. The fabricated ASC device can deliver a high energy density of 34 Wh kg⁻¹ at a power density of 500 W kg⁻¹ with cycling stability of 84% capacitance retained after 3000 cycles. The above results demonstrate that MnWO₄ microflowers can be used as promising high capacity electrode materials in neutral electrolyte for high performance supercapacitors.     

A comparative study of various polyelectrolyte/nanocomposite electrode combinations in symmetric supercapacitors

A more practical, nontoxic and cheaper electrolyte, poly(2-acrylamido-2-methyl-1-propanesulfonic acid) (PAMPS) was used to construct supercapacitors with different nanocomposite electrodes. The flexible devices were fabricated including active carbon (AC) electrode and nanocomposites electrodes of AC/nano-silica (nano-SiO₂) and AC/multiwalled carbon nanotubes (MWCNTs) at various weight percentages. The symmetrical cell made from AC electrodes generated a maximum specific capacitance (Cs) of 315 F g⁻¹ at 0.5 A g⁻¹. The energy density of this device was 55.5 Wh kg⁻¹ at a power density of 690 W kg⁻¹. Excellent performance was achieved after 5000 charge-discharge cycles where the supercapacitor maintains 92% of its activity. The energy storage capability of the supercapacitors was also investigated with the addition of nano-SiO₂ and MWCNTs. The Cs of the supercapacitors made with the electrodes AC/nano-SiO₂ (5%, 10%, 25% and 50%) were 172, 228, 247 and 55 F g⁻¹, respectively. Similarly, the capacity of the device including the electrodes of AC/MWCNTs (5%, 10%, 25% and 50%) varied as 191, 244, 93 and 20 F g⁻¹ at 0.5 A g⁻¹. The maximum energy density of the devices having nano-SiO₂ and MWCNT were 44.4 Wh kg⁻¹ and 43.8 Wh kg⁻¹, respectively at a power density of 520 W kg⁻¹. A supercapacitor with certain dimension successfully operated a light-emitting diode (LED).     

Fabrication of a ternary PANI@Fe3O4@CFs nanocomposite as a high performance electrode for solid-state supercapacitors

In this work, a solid-state high performance supercapacitor is fabricated based on a ternary polyaniline@Fe₃O₄@carbon fibers nanocomposite. To prepare the polyaniline@Fe₃O₄@carbon fibers electrodes, a two-step method including electrophoretic deposition of Fe₃O₄ nanoparticles on carbon fibres followed by an in situ polymerization process of polyaniline is utilized. The results show that the polyaniline@Fe₃O₄@carbon fibers nanocomposite with a layer by layer microstructure is successfully formed. The fabricated nanocomposite represents a specific surface area of 3.12 m² g⁻¹. The electrochemical measurements in a three-electrode configuration reveals a high specific capacitance of 245.5 F g⁻¹ at 0.5 A g⁻¹ and an excellent cycle stability (82.44% after 1000 cycle) of the polyaniline@Fe₃O₄@carbon fibers electrode. The as-fabricated solid-state supercapacitor based on the polyaniline@Fe₃O₄@carbon fiber nanocomposite cloth with a surface area of 25 cm² powers up a blue light-emitting diode for 4 min and delivers a high energy density of 78.6 Wh.kg⁻¹ at a power density of 1047.5 W kg⁻¹.     

A new Co-ZIF derived nanoporous cobalt-rich carbons with high-potential-window as high-performance electrodes for supercapacitors

In this work, a Co-ZIF material and the derived nanoporous cobalt-rich carbons by direct carbonization of this Co-ZIF material were synthesized and used as electrode materials for supercapacitors. This ZIF material exhibited a high specific capacitance of 160.3 F g⁻¹ at 0.5 A g⁻¹, an excellent rate capability (73.72 F g⁻¹ at 10 A g⁻¹), and a good cycling stability with 100% of its initials specific capacitance after 8000 cycles. In addition, the obtained derived nanoporous carbons displayed ideal capacitor behaviors and were promising electroactive materials for supercapacitors at low current density. The nanoporous carbon obtained at 650 °C possessed a highest specific capacitance of 393 F g⁻¹ at 0.5 A g⁻¹ and a wide potential application range of −1.0–0.33 V. In addition, a symmetric supercapacitor device consisting of Z-C-650 and activated carbon exhibited a maximum energy density of 61.23 Wh Kg⁻¹ at a power density of 700 W kg⁻¹ and predicted that Z-C-650 could be used as a potential energy storage material.     

Facile fabrication of comb-like porous NiCo2O4 nanoneedles on Ni foam as an advanced electrode for high-performance supercapacitor

It is very desirable to develop the high-performance supercapacitors to meet the rapidly growing demands for energy-autonomous operation and miniaturization of devices. Herein, comb-like porous NiCo₂O₄ nanoneedles on the three-dimension (3D) nickel foam (NF) have been successfully synthesized through a facile pulsed laser ablation (PLA) approach without any post-treatments and surfactant (denoted as NiCo₂O₄-PLA). The influence of working solution during the fabricated process on the properties of NiCo₂O₄-PLA has been demonstrated in detail in terms of the crystalline structure, specific surface area, morphology, and electrochemical performance. Benefiting from the large specific surface (261.4 m² g⁻¹), abundant pores, and highly conductive scaffold, the NiCo₂O₄-PLA binder-free electrode exhibits an outstanding specific capacitance (1650 F g⁻¹ at a current density of 1 A g⁻¹) and eminent cycling performance (91.78% retention after a 12,000-cycle test at a current density of 10 A g⁻¹) compared with the control samples. The assembled asymmetric device (NiCo₂O₄-PLA//AC-ASCs) delivers the high specific capacitance of 126.9 F g⁻¹ at the current density of 1 A g⁻¹, the large energy density of 56.7 Wh kg⁻¹ at a power density of 756 W kg⁻¹, and the low internal resistance. The attractive results strongly prove that it is an ideal candidate for advanced supercapacitor application.     

Core-shell structured ZIF-7@ZIF-67 with high electrochemical performance for all-solid-state asymmetric supercapacitor

Zeolitic imidazolate frameworks (ZIFs) are considered as a promising material for energy storage in recent years. Here, core-shell structured ZIF-7@ZIF-67 is synthesized in this work. The core-shell structured material can promote electron transfer of inner-outer metals ions of ZIF-7@ZIF-67, quicken diffusion of electrolyte ions and improve the capacitance performance compared to the ZIF-7 and ZIF-67. ZIF-7@ZIF-67 delivers good energy storage ability with a specific capacitance of 518.9 F g⁻¹ at a current density of 1 A g⁻¹ and remarkable stability with a retention of 99.6% after 4000 cycles in the three-electrode system. Furthermore, an all-solid-state asymmetric supercapacitor (ASC) device is assembled based on core-shell structured ZIF-7@ZIF-67 as positive electrode. Impressively, the ASC device displays an energy density of 31 Wh kg⁻¹ at a power density of 400 W kg⁻¹ and an excellent cyclic stability with 99.5% retention after 10,000 cycles at a current density of 10 A g⁻¹. Finally, two all-solid-state ASCs are contacted to power various lighting-emitting diodes (LED). The red LED can be kept glowing for over 10 min. These electrochemical characteristics suggest that core-shell structured ZIF-7@ZIF-67 is a potential material for energy storage device with long-life cyclic stability.     

Large-scale single-step synthesis of wrinkled N–S doped 3D graphene like nanosheets from Tender palm shoots for high energy density supercapacitors

Herein, we present a simple, large-scale and low-cost process to develop hierarchically porous N–S co-doped 3D wrinkled graphene like nanosheets (3D H-GNS) from carbonization of biomass Tender palm shoots and NaHCO₃. Non-corrosive and non-toxic Na₂CO₃ acts as a reaction mean to control the activation process, developing 3D H-GNS with a high specific surface area of 2095 m² g^?1. A 3D H-GNS-900 electrode exhibits a high specific capacitance of 529 F g^?1 (1.5 A g^?1) and 330 F g^?1 (1 A g^?1) in 1 M H₂SO₄ for 3-electrode and 2-electrode systems respectively. Further, a longer cycle life with 93% capacitance retention over 10,000 cycles at 5 A g^?1 is realized. Also, we are successful in fabricating biocompatible solid-state flexible supercapacitor device with 3D H-GNS-900 electrodes in organic electrolyte with 3 V voltage range, demonstrating to run a toy fan and lightning a LED for 15 min after charging for 60 s.     

A hybrid PEMFC/supercapacitor device with high energy and power densities based on reduced graphene oxide/Nafion/Pt electrode

Proton exchange membrane fuel cells (PEMFCs) possess high energy and low power densities, while supercapacitors are characterized by high power and low energy densities. A hybrid PEMFC/supercapacitor device (HPSD) with high energy and power densities was proposed and fabricated for the first time using a reduced graphene oxide/Nafion/Pt electrode in this study. The reduced graphene oxide (rGO) was a capacitive material, and Pt was used as the electrocatalyst. Nafion ionomers adsorbed onto the rGO sheets surface and connected the rGO sheets and the electrolyte (Nafion membrane), thus increasing the utilization rate and specific capacitance of rGO. During the half-cell tests, the rGO/Nafion/Pt electrode exhibited better pulse discharge and galvanostatic discharge performance than the conventional Nafion/Pt electrode. Due to the unique synergy of electrochemical reaction current and capacitance current during the discharge process, the HPSD exhibited a higher power density (26.2 kW kg⁻¹) than the PEMFC (23.9 kW kg⁻¹). The energy density (12.7 kWh kg⁻¹) exhibited by HPSD was close to that of the PEMFC (13.5 kWh kg⁻¹). Therefore, the concept of HPSD is to create a new method for developing next-generation electrochemical devices with high energy and power densities.     

Symmetric redox supercapacitor with conducting polyaniline electrodes

Polyaniline doped with HCl (Pani-HCl) and LiPF₆ (Pani-LiPF₆) are prepared and used as the active electrode material of symmetric redox supercapacitors. The system using Et₄NBF₄ as an electrolyte solution has lower internal resistance and larger specific discharge capacitance, and thus, it is suitable for use in a polyaniline redox supercapacitor. The capacitance of Pani-HCl decreases during ∼400 cycles and then becomes constant at ∼40 F g⁻¹. On the other hand, the polyaniline electrode doped with lithium salt like LiPF₆ shows a specific discharge capacitance of ∼107 F g⁻¹ initially and ∼84 F g⁻¹ at 9000 cycles.     

A free-standing electrode based on 2D SnS2 nanoplates@3D carbon foam for high performance supercapacitors

A reasonable formation of an electrode material with three-dimensional (3D) microstructure for supercapacitors was proposed. Two-dimensional (2D) SnS₂ nanoplates were uniformly in situ grown on 3D carbon foam (CF) through a controllable strategy. The composite displayed excellent electrochemical performance due to the synergistic effect of SnS₂ and CF. The SnS₂@CF-2 composite containing 23.92 wt% of SnS₂ has a superior specific capacitance of 283.6 F g⁻¹ at the current density of 1 A g⁻¹. Moreover, a symmetric supercapacitor based on SnS₂@CF-2 composite has a capacitance of 82.5 F g⁻¹ at 1 A g⁻¹ and a high energy density of 13.9 Wh kg⁻¹ at the power density of 551.7 W kg⁻¹.     

A cross-linked sheet structured poly(3,4-ethylenedioxythiophene) grown on Ni foam: Morphology control and application for long-life cyclic asymmetric supercapacitor

In this work, a cross-linked sheet structured conducting polymer ploy(3,4-ethylenedioxythiophene) (PEDOT) decorated on Ni foam is synthesized via one-step electrodeposition using the sodium p-toluenesulfonate (STSA) as surfactant and applied for supercapacitor electrode. The surfactants play a vital role in controlling the morphologies of PEDOT leading to the electrochemical performance difference. The optimized PEDOT electrode exhibits the highest capacitance of 711.6 mF cm⁻² at 3.0 mA cm⁻² in the three-electrode system. An asymmetric device (PEDOT/STSA//AC) is constructed by PEDOT/STSA (the positive electrode), activated carbon (AC) (the negative electrode) as well as 1 M Na₂SO₄ (the electrolyte). The device has been worked in a high-voltage range of 0–1.5 V, which displays the satisfied energy density of 14.0 Wh·kg⁻¹ at 535.5 W kg⁻¹. Furthermore, the PEDOT/STSA//AC device presents excellent rate capability and long-time cyclic stability.     

Embedding Co2P nanoparticles into N&P co-doped carbon fibers for hydrogen evolution reaction and supercapacitor

The demands for highly efficient and low-cost electrochemically active materials are still urgent needs for the fields of electro-catalysis and supercapacitor. Herein, a facile strategy for preparing high-efficient bi-functional electrode material was reported. The electrode material was prepared through embedding Co₂P nanoparticles in the binary co-doped carbon nanofibers (Co₂P@N&P-CNFs). This unique structure can effectively prevent the Co₂P from detaching and provide abundant active sites. Materials prepared in this work showed the superior hydrogen evolution reaction (HER) performance with overpotential of 192 mV at a current density of 10 mA cm^?2 and remarkable stability for 20 h. Moreover, the asymmetric supercapacitor (ASC) was fabricated using the Co₂P@N&P-CNFs as the positive electrode material and carbon nanofibers (CNFs) as the negative electrode material, which shows an outstanding cycle stability (91.5% of the initial capacitance is retained throughout 10,000 charge-discharge tests) and a high E of 22.31 Wh kg^?1 at the P of 225.02 W kg^?1 at 0.3 A g^?1. This work offers an effective route in designing bi-functional active materials for HER and supercapacitor.     

One-step hydrothermal preparation of bi-functional NiS2/reduced graphene oxide composite electrode material for dye-sensitized solar cells and supercapacitors

To screen out suitable electrode materials and overcome the shortcomings of the existed electrode materials for the application in dye-sensitized solar cells and supercapacitors, NiS₂/reduced graphene oxide (NiS₂/rGO) composite material was prepared by a simple one-step hydrothermal method in this paper and applied in the field of both dye-sensitized solar cells and supercapacitors as electrode material. In an electrolyte of 6 M KOH, the NiS₂/rGO composite material with bilayer capacitance characteristics exhibited a high specific capacitance of 259.20 F g⁻¹ at the current density of 0.6 A g⁻¹, which was significantly higher than that of rGO (188.94 F g⁻¹). Moreover, at a current density of 2 A g⁻¹, the NiS₂/rGO composite material had 92.85% capacitance retention after 2000 cycles. When applied as counter electrode material for the dye-sensitized solar cells, the NiS₂/rGO composite material counter electrode exhibited a satisfactory photoelectric conversion efficiency (η) of 3.16% under standard simulated sunlight (AM 1.5 G), which was significantly higher than that of single rGO counter electrode (improved by 90.40%). The NiS₂/rGO composite electrode material prepared by a simple one-step hydrothermal method is a potential bi-functional composite electrode materials for both dye-sensitized solar cells and supercapacitors.