High-performance Supercapacitor Electrode Research Articles

High-performance supercapacitor electrodes for energy storage using activated carbons from argan husks, date seeds and olive stones

High-performance supercapacitor electrodes for energy storage using activated carbons from argan husks, date seeds and olive stones

Construction of hierarchical and core-shell structured Co3O4@MnO2@NiO nanoarrays as binder-free electrodes for high-performance asymmetric supercapacitors

Remarkable specific capacity and excellent cycle stability of the electrode materials are vital prerequisites for their practical applications. Transition metal oxide-based materials have been extensively explored and employed as electrode materials for asymmetric supercapacitors. However, the actual specific capacitances of these materials are still far lower than their theoretically predicted values. Thus, it is essential to design transition metal oxide with novel structures in order to maximize their specific capacity and cycle stability. Herein, we constructs hierarchical and core-shell structured Co3O4@MnO2@NiO arrays on nickel foam (Co3O4@MnO2@NiO/NF) through a three-step hydrothermal-annealing process, and use them as a direct binder-free electrode for pseudocapacitors. The as-prepared layered hierarchical Co3O4@MnO2@NiO/NF electrode exhibits an impressive specific capacitance of 6.42 F cm−2 (2054 F g−1) at 1 mA cm−2 in a three-electrode configuration, which is largely because of the synergistic effect among Co3O4, MnO2 and NiO. Furthermore, the 3D nanoarray structure can provides a larger specific surface area, a rapid diffusion path, and more active sites that allow to achieve improved electrochemical performance. In addition, the assembled Co3O4@MnO2@NiO/NF//AC/NF ASC all-solid-state asymmetric supercapacitor (ASC) displays a remarkable energy density (30.7 Wh kg−1 at 400.4 W kg−1), demonstrating that this all-solid-state ASC owns considerable potential for practical applications in such high-performance energy storage devices.

Se-doped cobalt-nickel sulfide hollow nanospheres with heterostructure and engineered defects as high-performance electrode for supercapacitors

Porous structures with heterogeneous interfaces and defects are an important way to enhance electrochemically active sites and facilitate electron transfer, while also improving the permeability of the electrolyte and the rate of ion transport. In this study, Se-doped cobalt-nickel sulfide (Se-CoNi2S4) hollow nanospheres with heterostructure and defects were prepared from CoNi metal-organic framework (MOF) as substrate by sequential sulfidation and selenization treatments. Notably, the hollow structure not only offers additional ion transport channels to promote rapid transfer of ions in the electrolyte but also provides an increased number of electrochemically active sites. The morphology and electrochemical performance of Se-CoNi2S4 nanospheres with different levels of Se doping were compared. From the results, Se doping not only enhances the conductivity of CoNi2S4 but also increases its charge storage capacity. As an electrode material, the synthesized Se-CoNi2S4 composite that was synthesized demonstrated a notable specific capacitance of 1260 F g−1 at 1 A g−1. Additionally, when Se-CoNi2S4 was utilized as the anode and activated carbon served as the cathode in an asymmetric supercapacitor, it achieved an energy density of 44.6 Wh kg−1 at a power density of 827 W kg−1. After undergoing 10,000 cycles, this device demonstrated exceptional cycling stability, retaining 80.2 % of its initial capacitance. Therefore, the synthesized electrode material Se-CoNi2S4 has significant potential for energy storage applications.

Facile synthesis of MWCNT hexagonal needles grown on interconnected honeycombs like MnCo2O4/MnO2 nanoporous electrode for high-performance asymmetric supercapacitor

The construction of a honeycomb-like structure composed of MnCo2O4/MnO2was effectively achieved using a combination of hydrothermal processing and heat treatment. The whole surface of the MnCo2O4/MnO2 honeycomb is coated with neatly arranged hexagonal nano needles made of MWCNT, leading to a substantial enhancement in the specific surface area. At 1 A/g, the supercapacitor electrode composed of MnCo2O4/MnO2@MWCNT composite exhibited an exceptional specific capacitance of around 1539 F/g. Furthermore, it maintained approximately 95.5 % of its capacity even after undergoing 10,000 cycles. The asymmetric capacitor device, with MnCo2O4/MnO2@MWCNT and AC electrode, has a power density of 1537.8 W kg−1 and an energy density of 48.78 Wh kg−1. The MnCo2O4/MnO2composite exhibits exceptional rate performance, significant capacitance, and excellent cycle performance due to the synergistic effect between MnCo2O4/MnO2 and MWCNT, as well as the high specific surface area and unique structure. Consequently, it presents a viable option for the advancement of high-efficiency electrochemical super capacitors in the next generation.

Bamboo-templated MOF-67-derived carbon: A high-performance electrode for supercapacitors

Carbon-based supercapacitors are highly regarded for their high specific power and long cycle life. However, they often face the challenge of low specific energy and difficulty in simultaneously improving both specific energy and specific power. In this study, a high-performance composite electrode was prepared using the cross-section of bamboo as raw material, followed by KOH activation, in-situ growth of ZIF-67, and carbonization. The bamboo-derived porous carbon showed significant improvement in performance indicators such as specific capacitance and energy density. Electrochemical characterization in a three-electrode system showed that at a current density of 1 mA cm−2, our composite electrode material achieved a peak specific capacitance of 24.7 F cm−2. When assembled into a symmetric supercapacitor, it can provide an energy density of 1.00 mWh cm−2 at a power density of 2.49 mW cm−2. Notably, at a substantial current density of 30 mA cm−2, the electrode maintained a capacitance retention of 96.2 % after 10,000 cycles. These results not only highlight the potential of bamboo-derived porous carbon but also point to a broad avenue for the preparation of energy storage devices by combining MOFs with bamboo.

In-situ N, P co-doped porous carbon derived from biomass waste for supercapacitors

The development of heteroatom-doped porous carbon derived from biomass waste with high-performance electrodes for supercapacitors has been drawn extensive research. Herein, N, P co-doped porous carbon (NPC) was successfully synthesized using Chinese fir sawdust as a carbon source, NaOH as an activator, urea as a nitrogen source, and melamine phosphate as the phosphorus and nitrogen source by pretreatment with low-temperature NaOH/urea system. The low-temperature pretreatment and melamine phosphate greatly promoted the porous structure and uniform distributions of heteroatom about the NPC. The optimized NPC exhibits high specific surface area (1849 m2/g), hierarchical porous structure with high mesoporosity (87.3 %), appropriate heteroatom content (3.32 at% N, 0.36 at% P), and excellent wettability. This unique facilitates improved electrolyte diffusion efficiency and ion transfer rate. In the three-electrode system, the specific capacitance of the NPC electrode is as high as 260 F/g at 0.5 A/g and remains at 235 F/g at 10 A/g, and the charge transfer resistance is very low (0.08 Ω). In addition, the assembled symmetric supercapacitors deliver an energy density of 15.9 Wh/kg at a power density of 246 W/kg, a long cycling life with 90 % capacitance retention after 5000 cycles. The environment-friendly NPC has a broad development prospect for carbon-based high-performance electrodes for supercapacitors.

Theoretical and experimental studies on 2D β-NiS battery-type electrodes for high-performance supercapacitor

Recently, quirky features and eccentric structures of transition metal sulfides have grasped great attention to remove roadblocks and unwrap fresh avenues for electrodes in energy storage devices. Herein, we developed a 2D beta phase nickel sulfide nanosheets (2D β-NiS NSs) electrode with remarkable enhancement in charge storage properties. When served as active electrodes for electrochemical tests, 2D NiS NSs exhibited ultra-high capacitance of 2693 Fg−1 at 1 mVs−1 and specific capacity of 219 mAhg−1 at 1 Ag−1. The symmetric battery type solid-state supercapacitor device comprising 2D β-NiS NSs electrodes exhibits specific capacity of 83.43 mAhg−1at 2 Ag−1 over broad potential range of 0.7V with good cycling performance, and energy and power density of 28.9 Whkg−1 (@ 2 Ag−1) and 21 kWkg−1 (@ 6 Ag−1) respectively. Complementary first-principles density functional theory (DFT) calculations accomplished to explore the electrolyte ion interactions with nickel sulfide nanostructures defining 2D NiS NSs as a potential candidate for real-time applications.

Ultra-small one-dimensional rice-like CoMoO4 nanorods as a promising pseudocapacitive electrode for high-performance supercapacitors

The demand for sustainable energy sources increases as society progresses. Supercapacitors possess a long lifespan, have a high power density, are ecologically sound, and have the ability to rapidly charge and discharge. Among the several binary transition metal oxides (BTMOs), metal molybdates (AMoO4) are notable for their significant redox activity, widespread availability, affordability, and small ecological footprint. The exceptional theoretical capacitance of CoMoO4, resulting from the presence of active cobalt ions, distinguishes it from other materials. However, the synthesis of CoMoO4 in nanostructured forms presents a challenge. This study introduces a straightforward one-pot solvothermal technique for producing ultra-small, one-dimensional (1D) rice-like CoMoO4 nanorods. The electrochemical performance of rice-like CoMoO4 nanorods as a supercapacitor electrode material was thoroughly investigated, along with larger CoMoO4 nanorods made using the hydrothermal process for comparison. The structural, morphological, and surface characteristics of the rice-like CoMoO4 nanorods were comprehensively examined. The nanorods, formed like rice grains, exhibited exceptional ability to store electric charge, with an outstanding specific capacitance of 1608.8 F g−1. They demonstrated remarkable cycling stability, retaining 96 % of their capacitance after numerous charge and discharge cycles, indicating their durability and reliability. The nanorods also exhibited a high rate capability of 71 %, which is crucial for applications that demand quick energy delivery. This capability enables the nanorods to maintain considerable capacitance even at higher charge-discharge rates. The results indicate that rice-like CoMoO4 nanorods can be used as a material in supercapacitors.

Graphene oxide from coconut shells for high-performance supercapacitor application

Globally, the demand for materials with high ultrafast charge rates yet slow discharge continues to rise which has resulted in extensive research into supercapacitors. Although the current supercapacitors can meet such demands, the high processing cost coupled with the use of toxic chemicals remains a major concern. In this study, porous graphene oxide (GO) with a unique morphology was synthesized by an improved Tour’s method for supercapacitor application using coconut shells as a precursor. The structure of the synthesized material consists of partially graphitized walls of porous GO. The surface morphology, the defects created in the GO, and the specific surface area of the as-synthesized materials were studied. When evaluated as an electrode material for supercapacitors, a specific capacitance of 173 F/g at 0.5 A/g in 0.5 M Na2SO4 and 139 F/g at 0.5 A/g in 2 M KOH was recorded. Moreover, a high capacitance retention of 99.3% was recorded after 1000 cycles, confirming the good cyclic stability of the synthesized electrode material. The good electrochemical performance can be attributed to the electrode material’s intrinsic structural and compositional superiorities. These findings indicate the potential of using coconut shells as a precursor for the synthesis of high-performance graphene-based supercapacitor electrodes with improved cost-effectiveness and reduced environmental impact.

Ultrasound-assisted fungal self-growth and heteroatom doping for the preparation of high-performance lignocellulose-based supercapacitor electrodes

Biomass materials are widely used as supercapacitor electrode materials due to their cost-effectiveness and eco-friendliness. In this work, ultrasound-assisted impregnation was employed for the thorough mixing of the liquid medium, and fungal treatment was conducted on the three main components of lignocellulose to prepare a fungi-modified heteroatom-doped lignocellulose-based carbon material (LCF-NP). The effects of heteroatom doping, the content of the three main components, and fungal modification on the electrochemical performance of lignocellulose-based carbon materials was investigated. The results revealed the synergistic effect of heteroatom doping and fungal treatment on the electrochemical performance. Compared with its counterpart free of fungal treatment, LCF-NP has a more reasonable pore structure and exhibits excellent electrochemical performance. LCF-NP porous carbon material has the highest specific surface area (792 m2/g), large pore volume (0.523 cm3/g), and ideal specific capacitance (1940 mF/cm2) under the conditions of 1.0 M Na2SO4 electrolyte and current density of 0.5 mA/cm2. After 10,000 cycles, there is almost no loss of capacitance. These results indicate that the joint utilization of heteroatom doping and fungal treatment has a promising application prospect in pore structure regulation and electrochemical performance improvement. This study provides a new strategy for the preparation of lignocellulose-based carbon electrode materials.

Shape Tailored Nano-Ceria as High Performance Supercapacitor Electrode Material

Electrochemical energy storage devices herald a brighter future, offering efficient and sustainable solutions to meet the escalating global energy demands. The current work investigates the development and characterization of different ceria nanostructures (nanorod, nanocube, and nanopolyhedra) as effective electrode materials for supercapacitor applications. The electrode materials are systematically characterized using various spectroscopic and non-spectroscopic techniques. Galvanostatic charge-discharge, electrochemical impedance spectroscopy, and cyclic voltammetry techniques are used to evaluate the electrochemical performance of the electrode materials. The optimum material for the said application is cerium nanorod which has the maximum specific capacitance of 437.27 F/g in acid electrolytes. The current-voltage (I-V) characteristics of the ceria nanostructures exhibit hysteresis behavior; ceria nanorod showing coexistence of memristive and memcapacitive nature. The loop area of the hysteresis curve, derived from the ratio of OFF resistance to ON resistance (ROFF/RON) at 4 V, yields approximate values of 1.08, 1.33, and 1.57 for ceria nanocubes, ceria nanopolyhedra, and ceria nanorods, respectively. Impedance vs. frequency analysis of the samples was also carried out to study their electrical and transport properties. The results obtained from electrochemical analyses are complimented by electrical studies.

In situ construction of sea urchin-like structural NiCo-LDH coated cobalt‑nitrogen co-doped carbon as high-performance electrode for supercapacitor

Nickel‑cobalt layered double hydroxide (NiCo-LDH) has received much attention in the field of supercapacitor electrodes due to its multiple oxidation states and good electrochemical activity. However, NiCo-LDH often suffers from structural instability and low conductivity in practical applications. In this study, sea urchin-like structural NiCo-LDH coated cobalt‑nitrogen co-doped carbon (NiCo-LDH@Co-NC-x) electrode materials were prepared by in situ growth of NiCo-LDH on the surface of cobalt‑nitrogen co-doped carbon nanosheets (Co-NC) using a one-step hydrothermal method. The results show that the NiCo-LDH@Co-NC-2 electrode material exhibits excellent electrochemical performance, its specific capacitance is up to 1909 F g−1 at a current density of 1 A g−1, and capacitance retention of 69.5 % (only 26.2 % for NiCo-LDH) can be achieved after 10,000 cycles at a current density of 10 A g−1. This is because the abundant and uniformly distributed Co nanoparticles on Co-NC provide nucleation sites for the in-situ growth of NiCo-LDH, effectively improving the interface binding between Co-NC and NiCo-LDH, enhancing the structural stability of NiCo-LDH, and ensuring highly efficient electron transport throughout the NiCo-LDH@Co-NC-2 electrode. An asymmetric supercapacitor (NiCo-LDH@Co-NC-2//AC) was further assembled with NiCo-LDH@Co-NC-2 and activated carbon (AC) as positive and negative electrodes, respectively, achieving an energy density as high as 36.8 Wh kg−1 at a power density of 750 W kg−1. These findings suggest that the NiCo-LDH@Co-NC-2 composite can be a promising candidate for high-performance supercapacitor electrode.

Free-standing snowflake-like Mn-doped ZnO@CoCo2O4 nanofilm boosting cycle stability and energy density of supercapacitor

CoCo2O4 is considered as one of the most promising electrode materials owing to its inherently electrochemical performance and low cost. Nevertheless, the further practical application of CoCo2O4 as high-performance electrode material is hindered by its weak cycle stability. Herein, a free-standing snowflake-like Mn-doped ZnO@CoCo2O4 (MZCC) nanofilm is synthesized via hydrothermal method. The unique snowflake structure of this nanofilm composite exhibits obviously large specific surface area, thus promoting the redox reaction of the electrode material. The specific capacitance of the MZCC attains 1245F g−1 at 0.5 A/g. Furthermore, the assembled supercapacitor device with the MZCC and active carbon shows an energy density of 25.7 Wh kg−1 at a power density of 400 W kg−1. The device also demonstrated intriguingly outstanding cyclic stability, maintaining its original specific capacitance of 80.1 % after 3000 cycles at 2 A/g. This study delivers an effective method to construct high-performance free-standing metal oxide nanofilm electrodes for advanced supercapacitors.

Construction of ultra-thin NiMo3S4 nanosheet sphere electrode for high-performance hybrid supercapacitor

The construction of electrode materials with rational morphology and structure based on bimetallic sulfides is crucial to improve the performance of supercapacitors. Ultra-thin three-dimensional nickel molybdenum sulfide nanosheet spheres (NiMo3S4 NSSs) are grown on nickel foam (NF) using a one-step hydrothermal synthesis. NiMo3S4 NSSs have a diameter of ∼ 5 μm and nanosheet thickness of 200 nm. The effects of increasing the hydrothermal synthesis time and molar concentration ratios of Ni2+ to MoO42- on the morphologies of the NiMo3S4 are investigated. Due to the synergistic effect of NiMo3S4 NSSs and bimetallic ions which can provide a larger solution contact areas and improve the redox activity, the electrode exhibits good electrochemical properties. The specific capacity of NiMo3S4 NSSs/NF electrode can reach 1002.4 C/g (1 A/g). After being assembled into a hybrid supercapacitor (HSC) with activated carbon (AC), the energy density can reach 72.1 Wh/kg at the power density of 749.9 W/kg. In addition, the HSC shows an excellent stability of 89 % after 10, 000 charge-discharge cycles (10 A/g).

Incorporating Ag into Nd-Succinate MOF: Tunned electrochemical supercapacitor behaviour of Ag modified Nd-Succinate and electrochemical reaction mechanism

The electrode materials must be tailored to achieve higher energy and power densities and thus improve the supercapacitor's performance. This study explores the impact of incorporating Silver (Ag) into a Neodymium-Succinate Metal Organic Framework (Nd-Succinate) on supercapacitor behaviour. Initially, the Nd-Succinate MOF was characterized by structural, morphological, and spectroscopic characterizations. Subsequently, Ag/Nd-Succinate was synthesized and characterized. The electrochemical performance of Ag/Nd-Succinate was evaluated in a 6 M KOH electrolyte; the results indicated a significant enhancement in supercapacitor performance upon incorporating Ag into parent Nd-Succinate. From galvanostatic Charge-Discharge cycles (GCD), the capacitance for Ag/Nd-Succinate was determined to be 1389 F/g, i.e., 42 % higher than that of bare Nd-Succinate which was measured at 978 F/g. at a current density of 1.25 A/g. Ag/Nd-Succinate showcased an 89 % retention value for multiple retention cycles, slightly higher than the retention value obtained (84 %) for Nd-Succinate. The results of electrochemical experiments (Cyclic voltammetry (CV) and Electrochemical Impedance Spectra (EIS)) provided information about the nature of electron transfer and capacitance enhancement upon the introduction of Ag into Nd-Succinate. These findings provide valuable information on modifying MOFs and introducing metal that will help produce high-performance supercapacitor electrodes.

Tensile-endurable nanolayered polypyrrole templated by liquid crystal for high-performance stretchable supercapacitors

Ordered architectures favorable for energy storage are hard to build and preserve on stretchable electrodes owing to the elongation-induced variation in morphology. Herein, we demonstrate the construction of nanolayered polypyrrole (PPy) on stretchable polymeric electrodes via lyotropic liquid crystal (LLC) template for the first time. In situ graft polymerization of PPy onto swollen polyacrylamide-co-poly(2-hydroxy ethyl acrylate) in an aqueous Lα LLC gives stretchable electrodes with nanolayered PPy rooted in expandable wrinkles. The nanolayered PPy electrode could be stretched up to 330 % strain and keep intact after 2,000 stretch-release cycles owing to reversible unfolding of wrinkles. By virtue of the well-arranged PPy nanolayers, the stretchable electrode exhibits a high electrical conductivity of 154 S cm−1 and gives a capacitance of 1143 mF cm−2 after assembled into a supercapacitor with H2SO4 polyacrylamide hydrogel. In addition, the capacitance retention remains 94.6 % after 2,000 stretch-release cycles accompanied by galvanostatic charge–discharge. The LLC templating graft polymerization of conjugated polymers on elastic substrates paves a way to develop nanostructured stretchable electrodes for high-performance wearable supercapacitors.

A thiophene-sulfur doping porous organic Polymer/reduced graphene oxide composite for high-performance supercapacitor electrode

Porous organic polymers (POPs) are a type of promising materials which can be used in energy storage devices. In this study, we synthesized a novel thiophene-sulfur doping POPTAB-TPDA through Schiff-base condensation reaction between 1,3,5-triaminobenzene (TAB) and 2,5-thiphenedialdehyde (TPDA) at ambient temperature and pressure. With the reduced graphene oxide (rGO) as a template, thiophene-sulfur doping POPTAB-TPDA-rGO composite was obtained by in-situ synthesis under the same condition. As supercapacitor active electrode material, the stable value of specific capacitance of the POPTAB-TPDA-rGO composite (232.4 F g−1) is higher than that of pristine POPTAB-TPDA (193.5 F g−1) at a current density of 0.5 A g−1. The assembled asymmetric supercapacitor utilizing POPTAB-TPDA-rGO composite as positive material has an energy density of 38.7 W h kg−1 with the power density of 1619.2 W kg−1, displaying a better result than POPTAB-TPDA-based device. Furthermore, the POPTAB-TPDA-rGO-based supercapacitor exhibits an excellent cycle duration, with 81.7 % retention of its highest capacitance after 7000 cycles. This superior electrochemical performance of the composite could be attributed to three aspects: the reversible redox reaction processes of thiophene-sulfur units, the porous structure of POPTAB-TPDA facilitating ion transmission, and the good electron conductivity of rGO template.

3,6-Dimethoxythieno[3,2-b]thiophene-Based Bifunctional Electrodes for High-Performance Electrochromic Supercapacitors Prepared by One-Step Electrodeposition.

An integrated visual energy system consisting of conjugated polymer electrodes is promising for combining electrochromism with energy storage. In this work, we obtained copolymer bifunctional electrodes poly(3,6-dimethoxythieno[3,2-b]thiophene-co-2,3-dihydrothieno[3,4-b][1,4]dioxin-3-ylmethanol)(P(TT-OMe-co-EDTM)) by one-step electrochemical copolymerization, which exhibits favorable electrochromic and capacitive energy storage properties. Because of the synergistic effect of PTT-OMe and PEDTM, the prepared copolymers show better flexibility. Moreover, the morphology and electrochemical properties of the copolymers could be adjusted by depositing different molar ratios of 3,6-dimethoxythieno[3,2-b]thiophene (TT-OMe) and 2,3-dihydrothieno[3,4-b][1,4] dioxin-3-ylmethanol (EDTM). The P(TT-OMe-co-EDTM) electrodes realized a high specific capacitance (190 F/g at 5 mV/s) and recognizable color conversion. This work provides a novel and simple way to synergistically improve electrochromic and energy storage properties and develop thiophene-based conducting polymers for electrochromic energy storage devices.

Eu-viologen based bimetal–organic frameworks nanosheets with Mn atoms anchored on Eu-µ-O skeletons as high-performance negative electrode for flexible asymmetric supercapacitors

Exploring advanced negative electrode materials is imperative to develop high-performance asymmetric supercapacitors for breaking through current energy density limits of supercapacitors, but remains challenging. Herein, a strategy is proposed to create a novel negative electrode by anchoring Mn single-atoms on Eu-viologen metal–organic frameworks (EV-Mn MOFs) nanosheets flowery architectures that self-supported on oxidized carbon cloths (OCC). Such EV-Mn/OCC achieves a negative broadened voltage window (−1 ∼ 0 V) and boosted areal capacitance (840.82 mF cm−2), which is four folds of the isostructural EV/OCC without Mn atoms and surpasses most of currently reported negative electrodes. Also, the EV-Mn/OCC manifests good cycling stability (∼80 % retention for 10,000 cycles). As deduced by the thorough studies of X-ray absorption fine spectra and X-ray photoelectron spectroscopies, the enhanced pseudocapacitance of EV-Mn/OCC definitely correlates to the valence modulation of Mn and Eu through internal electron transfer via Eu-O-Mn bonds on Eu-µ-O skeleton in EV-Mn MOFs. Subsequently, the constructed flexible all-solid-state symmetric supercapacitors employing EV-Mn/OCC as negative electrode can deliver a high energy density (86.89 μWh cm−2) at 1600 μW cm−2, outperforming many asymmetric devices based on traditional negative electrode materials. This work can spur the development of single-atom metallic electronic-modulation strategy for MOFs negative electrode material (MOFs-NEM), and accelerate their applications in flexible energy conversion and storage devices.

Zeolitic imidazolate framework derived stellate shaped cobalt-molybdenum hybrid sulfide microflower for enhanced supercapacitor properties

Zeolitic imidazolate frameworks (ZIFs) represent a class of material exhibiting a well-defined geometry. The ZIF derivatives are known to inherit the parent morphology and have emerged as a potential platform for developing superior electrode materials. In this study, leaf-like ZIF-67 is synthesized using a chemical route and employed as the sacrificial template in one-pot hydrothermal sulfurization for preparing Co3S4-Mo15S19, cobalt‑molybdenum hybrid sulfide (CMS/NF). The unique stellate-shaped architecture of the CMS/NF microflowers enhances the exposure of the redox active sites, improving charge storage and exhibiting superior performance. On account of the synergy of the metal ions and stellate-shaped hierarchical architecture, the CMS/NF hybrid sulfide shows an excellent specific capacitance value of 3283 F g−1 at a current density of 1 A g−1 with capacitance retention of 77.7 % at 10 A g−1. An asymmetric supercapacitor device based on CMS/NF hybrid sulfide with aqueous KOH electrolyte exhibits a high specific energy of 40.8 Wh kg−1 at 400 W kg−1 with excellent cycling life of 81 % after 5000 cycles with ∼100 % coulombic efficiency. In addition, the density functional theory-based simulations have been carried out for the Co3S4-Mo15S19 hybrid system to develop a better understanding. From the total density of states, it is concluded that compared to the pristine structures, the hybrid system has enhanced states close to the Fermi level, confirming the conductivity improvement. Computed quantum capacitance for the pristine and hybrid systems corroborates the experimental capacitance consequences. Hence, the theoretical examinations warrant our electrochemical results and provide insight into developing high-performance supercapacitor electrodes.