Nitrogen-doped Hollow Carbon Research Articles

Efficient PMS activation toward degradation of bisphenol A by metal-free nitrogen-doped hollow carbon spheres

Peroxymonosulfate (PMS) activation methods conventionally face challenges such as high energy consumption and the risk of metal leaching, limiting their practical application. Metal-free catalysts often face the problem of low catalytic activity. This study designed an in-situ nitrogen-doped hollow carbon catalyst (DNC-9), which offers balances efficient catalytic performance and metal-free catalysis. The results indicate that the DNC-9/PMS system effectively degrades bisphenol A, achieving complete degradation over a broad pH range (3.0–9.0). Through structure modification, the degradation efficiency of bisphenol A compared with SiO2@DNC-9/PMS system was improved by around 6 times and the degradation kinetic rate can reach 0.346 min−1. DNC-9 can activate PMS, resulting in a higher concentration of singlet oxygen without the generation of free radicals. Graphitic nitrogen in DNC-9 plays a crucial role in this activation, offering adsorption sites that facilitate decomposition of PMS and generating 1O2. In addition, graphitic nitrogen forms a transient active intermediate, DNC-9-PMS*, enhancing bisphenol A degradation. The catalyst recovers its high activity to complete bisphenol A removal with 15 min after thermal regeneration in cyclic experiments, demonstrating its potential as a practical solution for the efficient degradation of emerging contaminants.

Nitrogen-doped hollow carbon spheres decorated with NiCo alloy nanoparticles for high-performance supercapacitor electrode

Nitrogen-doped hollow carbon spheres (NHCSs) decorated with NiCo alloy nanoparticles (NPs) were prepared and examined for their prospective role as high-performance electrode materials. The NHCSs were synthesized through a silica-assisted synthesis method, followed by the decoration of NiCo alloy NPs onto the NHCSs using a simple wet impregnation method, employing a 1:1 M ratio of Co to Ni elements. The NiCo/NHCS-23, composed of NHCSs with 23 wt% of NiCo alloy NPs, exhibited a specific capacitance (Csp) of 536 F g−1 when tested in a 6 M KOH solution at a current density of 1 A g−1. This high Csp is attributed to the synergistic effect of the faradaic charge storage provided by NiCo alloy NPs and the N-doped hollow carbon structure. The N content of the NHCSs and NiCo/NHCS-23 was found to be 1.9 % and 2.2 %, respectively. Symmetric supercapacitor (SSC) devices were assembled using two NiCo/NHCS-23 electrodes and a 0.5 M tetraethylammonium tetrafluoroborate/propylene carbonate electrolyte. The resulting SSC device operated within a potential window of 3.5 V and exhibited an energy density of 16.1 Wh kg−1 at the power density of 250 W kg−1. The SSC device demonstrated impressive cycling stability, maintaining 90.0 % capacitance and 83.1 % Coulombic efficiency after 5000 cycles. These results suggest that NiCo/NHCS nanocomposites have significant potential for utilization in high-energy storage applications.

Recyclable fabrication of hollow N-doped amorphous carbon nanospindles with abundant short-range curved carbon fragments as bifunctional anode for lithium/sodium ion storage

A recyclable hard-template method is proposed to exploit spindle-shaped hollow nitrogen-doped amorphous carbon (h-NAC) with a large number of short-range curved carbon fragments as anodes for lithium/sodium ion batteries (LIBs/SIBs). Besides providing adsorption sites due to the high existence of oxygen-containing functional groups (CO and COOH), the heavily exposed edge regions also provide a favorable storage environment with high adsorption energy for Li+/Na+ due to their short-range curved structure. Importantly, the etching solution of hard templates can be recycled to generate the FeOOH nanospindles as a precursor through a simple chemical titration, which supplies a new idea for the green preparation of hollow materials. The h-NAC electrode is proven to be bifunctional for storing lithium and sodium ions, displaying favorable rate capability (255 mAh g−1 and 106 mAh g−1 at 5 A g−1 for LIBs and SIBs, respectively). After 1000 cycles at 1 A g−1, the reproducible capacities of the LIBs and SIBs kept 496 mAh g−1 and 181 mAh g−1, respectively.

Spray Pyrolysis Regulated FeCo Alloy Anchoring on Nitrogen-Doped Carbon Hollow Spheres Boost the Performance of Zinc-Air Batteries.

Low-cost and high-efficiency non-precious metal-based oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) bifunctional catalysts are the key to promoting the commercial application of metal-air batteries. Herein, a highly efficient catalyst of Fe0.18Co0.82 alloy anchoring on the nitrogen-doped porous carbon hollow sphere (FexCo1-x/N-C) is intelligently designed by spray pyrolysis (SP). The zinc in the SP-derived metal oxides and metal-organic framework volatilize at high temperature to construct a hierarchical porous structure with abundant defects and fully exposes the FeCo nanoparticles which uniformly anchor on the carbon substrate. In this structure, the coexistence of Fe0.18Co0.82 alloy and binary metal active sites (Fe-Nx/Co-Nx) guarantees the Fe0.2Co0.8/N-C catalyst exhibiting an excellent half-wave potential (E1/2 ═ 0.84V) superior to 20% Pt/C for ORR and a suppressed overpotential (280mV) than RuO2 for OER. Assembled rechargeable Zn-air battery (RZAB) demonstrates a promising specific capacity of 807.02mAhg-1, peak power density of 159.08mWcm-2 and durability without electrolyte circulation (550h). This work proposes the design concept of utilizing an oxide core to in situ consume the porous carbon shell for anchoring metal active sites and construct defects, which benefits from spray pyrolysis in achieving precise control of the alloy structure and mass preparation.

FeNi decorated nitrogen-doped hollow carbon spheres as ultra-stable bifunctional oxygen electrocatalyst for rechargeable zinc-air battery with 2.7% decay after 300 hours cycling.

Research on non-noble metal bifunctional electrocatalysts with high efficiency and long-lasting stability is crucial for many energy storage devices such as zinc-air batteries. In this report, nitrogen-doped porous hollow carbon spheres with a size of about 300 nm were fabricated using a modified Stöber method and decorated with an FeNi alloy through a pyrolytic reduction process, resulting in a promising bifunctional electrocatalyst for both the oxygen evolution reaction and oxygen reduction reaction. The as-prepared FeNi@NHCS electrocatalyst exhibits excellent bifunctional activity in KOH electrolyte, attributed to its mesoporous structure, large specific surface area, and the strong coupling between the FeNi nanoalloy and nitrogen-doped carbon carriers. The electrocatalyst demonstrates excellent ORR performance with E1/2 = 0.828 V and OER activity with Ej=10 mA = 1.51 V. A zinc-air battery using FeNi@NHCS as the air electrode achieves an open-circuit voltage of 1.432 V and a maximum power density of 181.8 mW cm-2. After 300 h of galvanostatic charge-discharge cycles, the charge-discharge voltage gap (ΔU) of the battery had only decayed by 2.7%, demonstrating superior cycling stability.

Platinum-group-metal quaternary alloys with lattice defects for enhanced oxygen electrocatalysis.

We propose a facile coreduction method to synthesize a platinum-group-metal quaternary alloy anchored on nitrogen-doped hollow carbon spheres (PtPdRuIr/HCS) by using [MClx]y--1-butyl-3-methylimidazole (M = Pt, Pd, Ru, and Ir) ionic liquid. Owing to the steric hindrance of the imidazolium cations, Pt-group metal atoms of different sizes can be deposited at approximately the same pace for the growth of an alloy with lattice defects. The lattice-distorted PtPdRuIr/HCS exhibits enhanced activity toward oxygen electroreduction when benchmarked against Pt counterparts.

Boosting sodium-ion batteries performance by N-doped carbon spheres featuring porous and hollow structures.

Carbon materials are considered among the most promosing candidates for sodium ion batteries because of their competitive performance. Nevertheless, they suffer from low initial coulombic efficiencies (ICEs) and limited electrochemical performance. Herein, nitrogen-doped hollow carbon spheres (NHCSs) with a distinct porous structure are developed by a template-assisted carbonization of dopamine, followed by a template removal procedure. This advanced structural design, coupled with the surface chemistry of carbonized polydopamine, leads to an impressive ICE of 89.18% and a reversible capacity stabilized at ∼700 mA h g-1 at 50 mA g-1 after 100 cycles. Compared to commercial hard carbon anodes, NHCSs demonstrate superior rate performance, delivering a capacity of ∼200 mA g h-1 at 5 A g-1 with minimal capacity fading of ∼0.057 mA h g-1 per cycle over 1000 cycles. These findings highlight the potential of NHCSs as a high-performance anode material for sodium-ion batteries, offering both high efficiency and excellent cycling stability.

Poly (3, 4-propylenedioxythiophene)/Hollow carbon sphere composites supported Pt NPs to facilitate methanol oxidation reactions

Direct methanol fuel cells (DMFCs) are thought of as portable, sustainable, and non-polluting energy devices. The exploration of efficient and affordable catalysts for the methanol oxidation reaction (MOR) is significant for the industrial application of DMFCs. In this study, nitrogen-doped hollow carbon spheres (HCS) derived from polydopamine were proposed for the catalyst support for platinum nanoparticles (Pt NPs) for serving as the anode catalyst for DMFCs, and a composite support material was fabricated by in-situ oxidation of 3,4-ethylenedioxythiophene (ProDOT) with HCS to get core-shell structured poly(3,4-propylenedioxythiophene) (PProDOT)-embellished hollow carbon spheres (HCS) (PProDOT/HCS) for further improving the catalytic activity for supported catalyst. The results indicated that the platinum (Pt) on the surface of HCS was well dispersed, and the Pt became smaller and more evenly distributed with the introduction of PProDOT. Simultaneously, the Schottky junction formed between PProDOT and Pt NPs contributes to enhanced charge transfer and catalytic activity of the catalyst. Notably, the core-shell structure of the ternary catalyst, its excellent charge transfer capability, and the interaction between platinum and the support contribute to its high electrocatalytic activity. Electrochemical tests demonstrated that the PProDOT/HCS/Pt catalyst exhibited a mass activity of 1169.6 mA mg−1Pt for methanol oxidation in acidic electrolytes, surpassing the activity of the HCS/Pt catalyst (472.4 mA mg−1Pt) and commercial Pt/C (281.0 mA mg−1Pt).

Synergistic effect between Ni single atoms and Ni nanoparticles for effectively boosting sustainable co-electrolysis of CO2 and hydrazine

The intrinsic performance of single atom catalysts (SACs) to electrochemical CO2 reduction reaction (ECRR) is limited due to the absence of synergistic active sites. Herein, Ni single atom (NiSAs) and Ni nanoparticles (NiNPs) are co-loaded on nitrogen-doped hollow carbon spheres (N-HCSs) by a one-step calcination method, which exhibits high CO selectivity in H-type cell with aqueous solution or an ionic liquid as electrolyte. Particularly, NiSAs-NPs-N-HCSs demonstrate a CO selectivity of 98.98%, yielding an industrial level CO current density of 152.7 mA cm−2 in flow cell. In situ Raman spectroscopy and in situ infrared characterization technology confirm that *COOH and *CO are important intermediates in the ECRR process. Theoretical computations suggest that coexisting NiNPs can reduce the energy barrier of *COOH, thereby improving the ECRR performance, indicating the synergistic effect between NiSAs and NiNPs in the ECRR process. Moreover, NiSAs-NPs-N-HCSs is applied to the membrane electrode assembly system coupling the hydrazine oxidation reaction (HzOR), which can significantly reduce the voltage about 836 mV at 100 mA cm−2.

Surface-induced Co/Co9S8 nanodots embedded in nitrogen-doped hollow carbon nanocubes for high-performance overall water splitting

To obtain highly efficient water splitting, it is crucial to develop electrocatalysts with suitable structures, morphologies, and electronic states. we have developed a novel synthesis method that utilizes a sophisticated MOF-engaged approach to fabricate multi-dimensional Co/Co9S8 nano-heterojunctions (Co/Co9S8-NHs) that penetrate the hollow nanocubes, the as-prepared sample is referred to Co/Co9S8@HCNCs. Specifically, Co nanoparticles are encased and strung by single-phased Co9S8, generating Co/Co9S8 core/shell heterojunctions with an average size of 8 nm in the mesoporous walls of the carbon nanocubes. The as-prepared electrocatalyst shows exceptional stability and activity for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), contributing to the abundant active sites and fast mass transfer. Therefore, the uniquely designed heterostructure enables the remarkable OER and HER activities, delivering a current density of 10 mA cm−2 at the ultralow overpotential of 190 mV and 140 mV, separately. Furthermore, the Co/Co9S8@HCNCs can be scaled up and utilized as electrodes in industrial electrolyzers for water splitting. The device shows a consistent cell voltage of 1.52 V at the current density of 10 mA/cm2 over 30 h. This research demonstrates a facile and straightforward approach to developing complex catalytic interfaces on a nanoscale level, leading to increased catalytic activity through the exploitation of nano-heterojunction structures.

Nitrogen-doped hollow carbon spheres as efficient metal-free peroxymonosulfate activator for degradation of organic pollutant

Developing effective metal-free catalytic materials via constructing copious surface-exposed active sites to promote peroxymonosulfate (PMS) activating for degradation of hazardous organics is highly desirable toward practical application. In this study, we report the utilization of N-functionalized hollow carbon spheres (N-HCS) as efficient PMS activator for Rhodamine B (RhB) degradation. Results indicate that N-doping of hollow carbon spheres can introduce an abundance of pyridinic N and CO sites, which serve as catalytically active sites for PMS activation toward RhB degradation. The fabricated catalyst exhibits excellent performances with a degradation efficiency of 100 % and a rate constant of 0.0566 min−1 for RhB degradation under optimal conditions. Besides, the developed N-HCS catalyst displays a good reusability, maintaining a high degradation efficiency after the 5th run. Quenching tests and electron spin resonance characterization results reveal the coexistence of radical and non-radical degradation pathways, and SO4− and 1O2 are demonstrated as the dominant reactive oxygen species. This architecture integrated surface microenvironment engineering strategy can be extended to regulate the degradation performance of carbon-based materials for PMS activation toward removing other organic pollutants.

Hollow Nitrogen-Doped Carbon Spheres with Presiding Graphitic Nitrogen for Oxygen Reduction Reaction

Hollow nitrogen-doped carbons, a class of metal free electrocatalysts, offer a wide range of modifications due to their tunable diameter and carbon wall thickness. Herein, hollow nitrogen-doped carbon spheres (HNCS-1000) with numerous structural defects, thin carbon wall of about 8 nm, high (sp2-sp3)/sp3 bond ratio of 3.11 and graphitic-N proportion of 71.4% are prepared using a double pyrolysis strategy. When employed as ORR catalyst in O2-saturated 0.1 M KOH solution, HNCS-1000 retains high onset and halfwave potentials of 1.03 V and 0.88 V, respectively. In addition, it also demonstrates excellent stability/durability with 90.25% current density retention after 84000 s continuous chronoamperometric operation and only 33 mV loss in halfwave potential after 7000 CV cycles. Overall, the ORR performance of HNCS-1000 surpasses most of the previously reported nitrogen-doped carbon catalysts, and it is among the best catalysts for ORR in alkaline environment.

Electrocatalytic response of nitrogen-doped hollow carbon spheres modified glassy carbon electrode for sulphite detection in water

In this work, the glassy carbon electrode (GCE) surface was modified with nitrogen-doped hollow carbon spheres (N-HCSs) to achieve a new electrochemical sulphite sensor (N-HCSs/GCE) in water samples. The N-HCSs were explored for electrocatalytic behavior through voltammetric approaches using a routine three-electrode system. The findings revealed an admirable efficiency for modified electrodes towards sulphite oxidation, highlighting the effectiveness of our as-produced sulphite sensor. The differential pulse voltammetry was utilized under obtained optimal circumstances to study the as-developed sensor, the results of which underlined linear electrochemical current in relation to sulphite concentration, with dynamic range as wide as 1.0-100.0 μM and limit of detection as narrow as 0.35 μM. Moreover, N-HCSs/GCE had commendable practical applicability for sensing sulphite present in real specimens with voltammetric techniques.

Highly active CoP embedded in hollow nitrogen-doped carbon as an efficient bifunctional electrocatalyst for rechargeable zinc-air batteries

Aqueous zinc-air batteries provide a possibility to replace fossil fuels. However, developing bi-functional electrocatalysts with high activity, low-cost and environmental friendliness for zinc-air batteries remains a challenge. In this work, we report an efficient bifunctional electrocatalyst (H–CoP@NC) that is fabricated by phosphating a hollow metal organic framework (MOF) prepared using a self-template method. The H–CoP@NC exhibits a half-wave potential of 0.81V (vs. RHE) for the oxygen reduction reaction (ORR), and an overpotential of 390 mV for the oxygen evolution reaction (OER) at a current density of 10 mA cm−2. Remarkably, the H–CoP@NC assembled zinc-air battery possesses a voltage gap of 0.82 V at a current density of 50 mA cm−2, and the voltage gap increases by only 0.01 V after 730 continuous charge and discharge cycles. This excellent electrocatalytic activity for ORR and OER can be attributed to the hollow structure, which improves mass transport during the electrocatalytic reaction, and the synergistic effect between CoP and heteroatom doped carbon skeletons which provide a high density of exposed active sites.

NbN quantum dots anchored hollow carbon nanorods as efficient polysulfide immobilizer and lithium stabilizer for Li-S full batteries

The shuttle effect of lithium polysulfides (LiPSs) and uncontrollable lithium dendrite growth seriously hinder the practical application of lithium-sulfur (Li-S) batteries. To simultaneously address such issues, monodispersed NbN quantum dots anchored on nitrogen-doped hollow carbon nanorods (NbN@NHCR) are elaborately developed as efficient LiPSs immobilizer and Li stabilizer for high-performance Li-S full batteries. Density functional theory (DFT) calculations and experimental characterizations demonstrate that the sulfiphilic and lithiophilic NbN@NHCR hybrid can not only efficiently immobilize the soluble LiPSs and facilitate diffusion-conversion kinetics for alleviating the shuttling effect, but also homogenize the distribution of Li+ ions and regulate uniform Li deposition for suppressing Li-dendrite growth. As a result, the assembled Li-S full batteries (NbN@NHCR-S||NbN@NHCR-Li) deliver excellent long-term cycling stability with a low decay rate of 0.031% per cycle over 1000 cycles at high rate of 2 C. Even at a high S loading of 5.8 mg cm−2 and a low electrolyte/sulfur ratio of 5.2 µL mg−1, a large areal capacity of 6.2 mA h cm−2 can be achieved in Li-S pouch cell at 0.1 C. This study provides a new perspective via designing a dual-functional sulfiphilic and lithiophilic hybrid to address serious issues of the shuttle effect of S cathode and dendrite growth of Li anode.

Regulating the Spin State Configuration in Bimetallic Phosphorus Trisulfides for Promoting Sulfur Redox Kinetics.

Lithium-sulfur (Li-S) batteries suffer from sluggish kinetics due to the poor conductivity of sulfur cathodes and polysulfide shutting. Current studies on sulfur redox catalysis mainly focus on the adsorption and catalytic conversion of lithium polysulfides but ignore the modulation of the electronic structure of the catalysts which involves spin-related charge transfer and orbital interactions. In this work, bimetallic phosphorus trisulfides embedded in Prussian blue analogue-derived nitrogen-doped hollow carbon nanocubes (FeCoPS3/NCs) were elaborately synthesized as a host to reveal the relationship between the catalytic activity and the spin state configuration for Li-S batteries. Orbital spin splitting in FeCoPS3 drives the electronic structure transition from low-spin to high-spin states, generating more unpaired electrons on the 3d orbit. Specifically, the nondegenerate orbitals involved in the high-spin configuration of FeCoPS3 result in the upshift of energy levels, generating more active electronic states. Such tailored electronic structure increases the charge transfer, influences the d-band center, and further modifies the adsorption energy with lithium polysulfides and the potential reaction pathways. Consequently, the cell with FeCoPS3/NC host exhibits an ultralow capacity decay of 0.037% per cycle over 1000 cycles. This study proposed a general strategy for sculpting geometric configurations to enable spin and orbital topology regulation in Li-S battery catalysts.

Nitrogen-doped hollow mesoporous carbon spheres for efficient oxygen reduction

Extensive investigations have been devoted to nitrogen-doped carbon materials as catalysts for the oxygen reduction reaction (ORR) in various conversion technologies. In this study, we introduce nitrogen-doped carbon materials with hollow spherical structures. These materials demonstrate significant potential in ORR activity within alkaline media, showing a half-wave potential of 0.87 V versus the reversible hydrogen electrode (RHE). Nitrogen-doped hollow carbon spheres (N-CHS) exhibit unique characteristics such as a thin carbon shell layer, hollow structure, large surface area, and distinct pore features. These features collectively create an optimal environment for facilitating the diffusion of reactants, thereby enhancing the exposure of active sites and improving catalytic performance. Building upon the promising qualities of N-CHS as a catalyst support, we employ heme chloride (1 wt%) as the source of iron for Fe doping. Through the carbonization process, Fe-N active sites are effectively formed, displaying a half-wave potential of 0.9 V versus RHE. Notably, when implemented as a cathode catalyst in zinc-air batteries, this catalyst exhibits an impressive power density of 162.6 mW cm−2.

A Gram Scale Soft-Template Synthesis of Heteroatom Doped Nanoporous Hollow Carbon Spheres for Oxygen Reduction Reaction.

Heteroatom-doped nanoporous carbon materials with unique hierarchical structures have been shown to be promising supports and catalysts for energy conversion; however, hard-template methods are limited by their inflexibility and time-consuming process. Soft-template methods have been suggested as an alternative, but they are limited by their picky requirements for stable reactions and the few known precursors for small-batch synthesis. In this study, a gram-scale soft-template-based silica-assisted method was investigated for producing nitrogen-doped hollow nanoporous carbon spheres (N-HNCS). Nitrogen doping is accomplished during preparation with enhanced electrocatalytic activity without complicating the methodology. To investigate the effect of the unique structural characteristics of N-HNCS (specific surface area: 1250 m2 g-1; pore volume: 1.2 cm3 g-1), cobalt was introduced as an active center for the oxygen reduction reaction. Finely tuned reaction conditions resulted in well-dispersed cobalt particles with minimal agglomeration. This sheds light on the advancement of new experimental procedures for developing more active and promising non-noble catalysts in large and stable batches.

Metal-organic framework derived hollow nitrogen-doped carbon sphere with cobalt phosphide in carbon nanotube for efficient oxygen evolution

The sluggish kinetics of the electrocatalytic oxygen evolution reaction (OER) pose a significant challenge in the field of overall water splitting. Transition metal phosphides have emerged as promising catalysts for OER by modulating the charge distribution of surrounding atoms. In this study, we employed self-sacrificing templates to fabricate hollow N-doped carbon spheres containing small-sized Co2P embedded within carbon nanotubes through high-temperature calcination and phosphorization, referred to as HNCS-CNT-CoP. The obtained HNCS-CNT-CoP electrocatalyst exhibited excellent OER performance in an alkaline electrolyte due to the optimization of OH* adsorption energy and the large specific surface area created by the hollow structure. It demonstrated a low overpotential of 302 mV at a current density of 10 mA cm−2 and a low Tafel slope of 68.5 mV dec−1, attributed to the electron transport facilitated by the in situ formed carbon nanotubes. Furthermore, theoretical calculations revealed a suitable reaction energy (1.17 eV) in the critical formation of Co2P-*OOH for HNCS-CNT-CoP, significantly lower than the the rate-determining step of HNCS-CNT-Co (10.08 eV). These findings highlight the significance of hollow structures and Co2P-doping in the design of highly active non-noble metal OER electrocatalysts, enabling the reduction of energetic reaction barriers for future applications.

High energy density pouch-type supercapacitor achieved by MOFs derived 3D hollow N-doped carbon with Fe2O3 and hierarchical CuCo2S4@NiFe-LDH core-shell nanostructures

The multicomponent rational control and distinctive architectural design of electrode materials remain critical factors for enhancing the energy density of supercapacitors. Herein, metal-organic framework (MOF)-derived three-dimensional (3D) hollow nitrogen-doped carbon (NHCs) with Fe2O3 core-shell composite negative electrode materials (NHCs@Fe2O3) were developed. In this framework, 1) the high specific surface area caused by the distinctive core-shell structure facilitated the electrolyte infiltration in the hollow skeleton, which shortened the ion transport path and enabled fast electron transfer; and 2) the synergistic effect of the nitrogen-containing groups of the hollow carbon and the reversible Faraday reaction of metal oxides increased the ratio of the pseudocapacitance. These phenomena were the primary reasons for the enhanced capacity of the core-shell electrode. Additionally, hierarchical CuCo2S4@layered double hydroxide (NiFe-LDH) nanobelt core-shell heterostructure arrays integrated on the nickel foam were used for the positive electrode materials. The asymmetric pouch-type supercapacitor assembled with NHCs@Fe2O3 (negative electrode) and CuCo2S4@NiFe-LDH (positive electrode) exhibited a high energy density of 68.6 W h kg–1 at a power density of 828.9 W kg–1. This work offers an effective strategy for fabricating multicomponent core-shell materials and optimizing the interactions between the components to enhance the electrochemical performance in energy storage applications.