Design of high-performance flexible symmetric supercapacitors energized by redox-mediated hydrogels including metal-doped acidic polyelectrolyte

The fabrication of flexible supercapacitors was achieved by employing the novel redox-activated polymer electrolytes comprising poly(vinylphosphonic acid) (PVPA) and nickel nitrate Ni(NO₃)₂, Ni. The hydrogels, PVPA/NiX, were produced in various contents, in which X denotes the doping fraction of Ni in PVPA. The structure, thermal, and morphology of the materials were characterized, and then they were applied for construction of supercapacitors. The performance evaluations of the fabricated devices were carried out by electrochemical impedance spectroscopy, galvanostatic charge-discharge, and cyclic voltammetry experiments. Flexible supercapacitor devices assembled with activated carbon (AC) electrodes and PVPA/NiX hydrogels produced 793 F g⁻¹ specific capacitance with 30 times enhanced capacitance compared with Ni-free system. The energy density of 103.1 Wh kg⁻¹ was yielded from the device at a power density of 500 W kg⁻¹. The supercapacitor demonstrated an excellent performance during 5.000 charge-discharge cycles, while preserving 84% of its initial capacitance. The supercapacitor constructed of 1 × 5 cm dimension, successfully operates the LED after charging at 3 V.     

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.     

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.     

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).     

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.     

Interconnected NiS-nanosheets@porous carbon derived from Zeolitic-imidazolate frameworks (ZIFs) as electrode materials for high-performance hybrid supercapacitors

Nickel sulfide-based materials have shown great potential for electrode fabrication owing to their high theoretical specific capacitance but poor conductivity and morphological aggregation. A feasible strategy is to design hybrid structure by introducing highly-conductive porous carbon as the supporting matrix. Herein, we synthesized hybrid composites consisting of interconnected NiS-nanosheets and porous carbon (NiS@C) derived from Zeolitic-imidazolate frameworks (ZIFs) using a facile low-temperature water-bath method. When employed as electrode materials, the as-prepared NiS@C nanocomposites present remarkable electrochemical performance owing to the complex effect that is the combined advantages of double-layer capacitor-type porous carbon and pseudocapacitor-type interconnected-NiS nanosheets. Specifically, the NiS@C nanocomposites exhibit a high specific capacitance of 1827 F g⁻¹ at 1 A g⁻¹, and excellent cyclic stability with a capacity retention of 72% at a very high current density of 20 A g⁻¹ after 5000 cycles. Moreover, the fabricated hybrid supercapacitor delivers 21.6 Wh kg⁻¹ at 400 W kg⁻¹ with coulombic efficiency of 93.9%, and reaches 10.8 Wh kg⁻¹ at a high power density of 8000 W kg⁻¹, along with excellent cyclic stability of 84% at 5 A g⁻¹ after 5000 cycles. All results suggest that NiS@C nanocomposites are applicable to high-performance electrodes in hybrid supercapacitors and other energy-storage device applications.     

Electrochemical profile of nano-particle CoAl double hydroxide/active carbon supercapacitor using KOH electrolyte solution

A nano-structured CoAl double hydroxide with an average particle size of 60–70 nm was prepared by a chemical co-precipitation. It was used as a positive electrode for the asymmetric hybrid supercapacitor in combination with an active carbon negative electrode in KOH electrolyte solution. The electrochemical capacitance performance of this kind of hybrid supercapacitor was investigated by means of cyclic voltammetry, electrochemical impedance spectroscopy and galvanostatic charge–discharge tests. A specific capacitance of 77 F g⁻¹ with a specific energy density of 15.5 wh kg⁻¹ was obtained for the hybrid supercapacitor within the voltage range of 0.9–1.5 V. The supercapacitor also exhibits a good cycling performance and keep 90% of initial capacity over 1000 cycles.     

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).     

Biomass-derived graphene-based nanocomposite: A facile template for decoration of ultrathin nickel–aluminum layered double hydroxide nanosheets as high-performance supercapacitors

One promising approach to design of high performance supercapacitors is based on the coupling the conductive porous carbon matrixes and the electroactive components. However, the main challenge to this goal is the maintaining the long cycling life, high power and high energy densities of the related capacitors. Herein, we reported on an electroactive composite based on biomass derived 3D graphene coupled with nickel-aluminum layer double hydroxides for manufacturing a cathode material in a supercapacitor. The electrode exhibits a remarkable specific capacitance of 1390 F g⁻¹ at 1 Ag^-1, and ultrahigh rate capability of 60% from 1 to 30 Ag^-1, as well as excellent cycling stability with a capacitance retention of 92% after 5000 cycles. Furthermore, the electrode was used as the positive electrode against a Vulcan XC-72R as the negative electrode to assemble an asymmetric supercapacitor. The asymmetric supercapacitor device exhibited a maximum energy density of 173 Wh kg⁻¹ and power density of 28.8 kW kg⁻¹ as well as excellent cycling stability of 92% after 5000 cycles. The asymmetric supercapacitor could lighted up LED lamps with different colors more than 24 min. The work showed promising performance of further application in electrochemical devices.     

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.     

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.     

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.     

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.     

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.     

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.     

Rational design of hierarchical core-shell structured CoMoO4@CoS composites on reduced graphene oxide for supercapacitors with enhanced electrochemical performance

Engineering multicomponent active materials as an advanced electrode with the rational designed core-shell structure is an effective way to enhance the electrochemical performances for supercapacitors. Herein, three-dimensional self-supported hierarchical CoMoO₄@CoS core-shell heterostructures supported on reduced graphene oxide/Ni foam have been rationally designed and prepared via a facile approach. The unique structure and the synergistic effects between two different materials, as well as excellent electronic conductivity of the reduced graphene oxide, contribute to the increased electrochemically active site and enhanced capacitance. The core-shell CoMoO₄@CoS composite displays the superior specific capacitance of 3380.3 F g⁻¹ (1 A g⁻¹) in the three-electrode system and 81.1% retention of the initial capacitance even after 6000 cycles. Moreover, an asymmetric device was successfully prepared using CoMoO₄@CoS and activated carbon as positive/negative electrodes. It is worth mentioning that the device delivered the high energy density of 59.2 W h kg⁻¹ at the power density of 799.8 W kg⁻¹ and the excellent cycle performance (about 91.5% capacitance retention over 6000 cycles). These results indicate that the core-shell CoMoO₄@CoS composites offers the novelty strategy for preparation of electrodes for energy conversion and storage devices.     

High energy density PbO2/activated carbon asymmetric electrochemical capacitor based on lead dioxide electrode with three-dimensional porous titanium substrate

A PbO₂/AC asymmetric electrochemical capacitor (AEC) with energy density as high as 49.4 Wh kg⁻¹, power density of 433.2 W kg⁻¹ and specific capacitance of 135.2 F g⁻¹ was fabricated with PbO₂ electrodeposited on three-dimensional porous titanium (3D-Ti/PbO₂) and activated carbon. The high electrochemical active surface of 3D-Ti/PbO₂ resulted in high specific capacity making it suitable for use as positive electrode in PbO₂/AC AEC. The fabricated AEC demonstrated good power performance with an energy density conservation of 30 Wh kg⁻¹ at power density of 2078 W kg⁻¹. The fabricated AEC also showed excellent cycling stability with capacitance retention of 99.2% after 1000 cycles.     

Divulging the electrochemical hydrogen storage of ternary BNP-doped carbon derived from biomass scaled to a pouch cell supercapacitor

Activated carbon materials have been studied extensively as electrode materials for supercapacitors (SCs), but their poor capacitance and energy density have hampered their growth. We present a one-step synthesis of a ternary boron-nitrogen-phosphorous-doped carbon (BNPC) from biomass hemp fibre to determine its electrochemical hydrogen storage ability using SC applications. FESEM micrographs reveal mixed morphologies like square, diamond and cylindrical-shaped nanosheets, confirming the hetero-atom doping into the carbon skeleton. The optimized BNPC electrode delivers a half-cell specific capacitance and hydrogen-storage capacity of 520 Fg^-1 (1 Ag^-1) and 360 mAhg⁻¹ (10 mVs⁻¹), respectively. To demonstrate the practicability of the as-prepared BNPC electrode, a symmetric pouch-cell supercapacitor device was assembled which exhibits a full-cell specific capacitance of 262.56 Fg^-1 at 1 Ag^-1 and a specific energy of ~118 Wh kg⁻¹ at a specific power of ~5759 Wkg^-1 with an operating potential window of 1.8 V and 99.7% capacitance retention over 10,000 cycles. This excellent electrochemical performance can be ascribed to the synergetic properties of fast-electrolyte-ion diffusion due to the doping of heteroatoms into the carbon matrix, high conductivity and high specific surface area and effective microporosity of BNPC (1555.5 m²g^-1). Also, the chemical stability of the BNPC materials, was investigated with density functional theory (DFT)-single point calculations, where the least molecular orbital energy gap was obtained by the BNPC, which confirms its structural stability. Thus, the prepared ternary BNP-doped carbon derived from biomass has provided a new direction to enhance the electrochemical energy storage potential.     

N/S dual-doped graphene with high defect density for enhanced supercapacitor properties

N/S dual-doped graphene was prepared by one-pot process using graphene oxide as raw material and thiourea and urea as reduction-dopants. The field emission scanning electron microscopy (FESEM), X-ray powder diffraction (XRD), Raman spectroscopy (Raman), nuclear magnetic resonance (NMR) spectroscopy, X-ray photoelectron spectroscopy (XPS), and other means were used to characterize the microstructure and morphology of the samples. The electrochemical properties of the samples were tested by cyclic voltammetry, electrochemical alternating impedance and constant current charge-discharge techniques, and compared with graphene and nitrogen-doped graphene. Results show that the defect density of graphene can be increased more effectively by N/S dual doping than by nitrogen doping, and the contents of doped nitrogen and sulfur have a significant effect on the morphology and performance of the samples. The specific surface area of the best sample reaches 275.8 m² g⁻¹, and its conductivity is 477.6 S m⁻¹. When the window voltage is −1.2-0 V, the best sample shows superior specific capacitance of 386.5 F g⁻¹ and a high energy density of 69.6 Wh kg⁻¹ at a scan rate of 10 mV s⁻¹. At the current density of 10 A g⁻¹, after 5000 constant current charge/discharge cycles, the specific capacitance retention rate is 94.5%, showing excellent cyclic stability.