Multichannel Carbon Research Articles

Multichannel Carbon Nanofibers: Pioneering the Future of Energy Storage.

Multichannel carbon nanofibers (MCNFs), characterized by complex hierarchical structures comprising multiple channels or compartments, have attracted considerable attention owing to their high porosity, large surface area, good directionality, tunable composition, and low density. In recent years, electrospinning (ESP) has emerged as a popular synthetic technique for producing MCNFs with exceptional properties from various polymer blends, driven by phase separation between polymers. These interactions, including van der Waals forces, covalent bonding, and ionic interactions, are crucial for MCNF production. Over time, the applications of MCNFs have expanded, making them one of the most intriguing topics in material research. MCNFs with tailored porous channels, controllable dimensions, confined spaces, high surface areas, designed architectures, and easy electrolyte access to active walls are considered optimal for electrochemical energy storage (EES) technologies. This review provides an exhaustive overview of the working principle, synthesis methods, and structural properties of MCNFs, and examines their advantages, limitations, and potential for producing multichannel architectures. Furthermore, this review explores the relationship between the composition of MCNF electrode materials for EES devices (supercapacitors and batteries) and their electrochemical performance. This review also addresses future directions and challenges in the development and utilization of MCNFs and provides insights into potential research avenues for advancing this exciting field.

Encapsulation of Sn Sub‐Nanoclusters in Multichannel Carbon Matrix for High‐Performance Potassium‐Ion Batteries

AbstractSub‐nanoclusters with ultra‐small particle sizes are particularly significant to create advanced energy storage materials. Herein, Sn sub‐nanoclusters encapsulated in nitrogen‐doped multichannel carbon matrix (denoted as Sn‐SCs@MCNF) are designed by a facile and controllable route as flexible anode for high‐performance potassium ion batteries (PIBs). The uniformly dispersed Sn sub‐nanoclusters in multichannel carbon matrix can be precisely identified, which ensure us to clarify the size influence on the electrochemical performance. The sub‐nanoscale effect of Sn‐SCs@MCNF restrains electrode pulverization and enhances the K+ diffusion kinetics, leading to the superior cycling stability and rate performance. As freestanding anode in PIBs, Sn‐SCs@MCNF manifests superior K+ storage properties, such as exceptional cycling stability ( around 331 mAh g−1 after 150 cycles at 100 mA g−1) and rate capability. Especially, the Sn‐SCs@MCNF||KFe[Fe(CN)6] full cell demonstrates impressive reversible capacity of around 167 mAh g−1 at 0.4 A g−1 even after 200 cycles. Theoretical calculations clarify that the ultrafine Sn sub‐nanoclusters are beneficial for electron transfer and contribute to the lower energy barriers of the intermediates, thereby resulting in promising electrochemical performance. Comprehensive investigation for the intrinsic K+ storage process of Sn‐SCs@MCNF is revealed by in situ analysis. This work provides vital guidance to design sub‐nanoscale functional materials for high‐performance energy‐storage devices.

Encapsulation of Sn Sub-Nanoclusters in Multichannel Carbon Matrix for High-Performance Potassium-Ion Batteries.

Sub-nanoclusters with ultra-small particle sizes are particularly significant to create advanced energy storage materials. Herein, Sn sub-nanoclusters encapsulated in nitrogen-doped multichannel carbon matrix (denoted as Sn-SCs@MCNF) are designed by a facile and controllable route as flexible anode for high-performance potassium ion batteries (PIBs). The uniformly dispersed Sn sub-nanoclusters in multichannel carbon matrix can be precisely identified, which ensure us to clarify the size influence on the electrochemical performance. The sub-nanoscale effect of Sn-SCs@MCNF restrains electrode pulverization and enhances the K+ diffusion kinetics, leading to the superior cycling stability and rate performance. As freestanding anode in PIBs, Sn-SCs@MCNF manifests superior K+ storage properties, such as exceptional cycling stability ( around 331 mAh g-1 after 150 cycles at 100 mA g-1) and rate capability. Especially, the Sn-SCs@MCNF||KFe[Fe(CN)6] full cell demonstrates impressive reversible capacity of around 167 mAh g-1 at 0.4 A g-1 even after 200 cycles. Theoretical calculations clarify that the ultrafine Sn sub-nanoclusters are beneficial for electron transfer and contribute to the lower energy barriers of the intermediates, thereby resulting in promising electrochemical performance. Comprehensive investigation for the intrinsic K+ storage process of Sn-SCs@MCNF is revealed by in situ analysis. This work provides vital guidance to design sub-nanoscale functional materials for high-performance energy-storage devices.

MOF derivatives anchored to multichannel hollow carbon fibers with gradient structures for corrosion resistance and efficient electromagnetic wave absorption

With the rapid development of 5G technology and the interconnection of industrial production, electromagnetic pollution has become a serious problem. Achieving lightweight and controllable loads of absorbers while obtaining corrosion-resistant absorbers with high electromagnetic response properties is still considered a huge challenge. In this work, carbon fiber with a multichannel hollow structure is obtained by PAN/PS hybrid electrospinning and subsequent high-temperature roasting process. The spatial structure inside the carbon fiber plays an active role in optimizing the impedance matching characteristics of the absorber. In addition, bimetallic metal-organic frameworks (MOFs) derivatives are obtained by a precisely controlled ion exchange as well as a high-temperature gas-phase selenization process. The resulting introduction of a non-homogeneous interface induces interfacial polarization and improves the absorption behavior of the absorber. The analysis of the experimental results shows that the electromagnetic wave (EMW) absorption performance can be effectively enhanced due to the mechanisms of interface polarization and dipole polarization. The prepared NiSe/ZnSe/MHCFs composite can obtain excellent EMW absorption properties in C, X, and Ku bands by adjusting the thickness. Structural design and component modulation play a crucial role in realizing the strong absorption and wide bandwidth of the absorber. Radar cross-section calculations indicate that NiSe/ZnSe/MHCFs have tremendous potential in practical military stealth technology. And the prepared composite coating can provide periodic corrosion resistance to Q235 steel sheet when dealing with complex and extreme environments.

Construction of Co9S8/SnS heterostructures encapsulated in multi-channel carbon nanofibers as long-term stable anodes for sodium-ion batteries

This study presents the design and fabrication of multi-channel self-supported anode materials Co9S8/SnS@MCNFs, through the electrospinning technique. The high compatibility of Co9S8 and SnS at the interface enables the synthesis of a more complete heterostructure within the material, enhancing the electrochemical reaction process through rational heterostructure design. Additionally, the incorporation of high theoretical capacity SnS improves sodium storage performance. The design of multi-channel carbon nanofibers (MCNFs) effectively addresses challenges such as material volume expansion and metal particle aggregation during cycling by providing large specific surface areas and enabling carbon encapsulation. The resulting pore structure and heterostructure formation, coupled with introduction of more defects, enhance the availability of Na+ active sites for electrochemically reversible processes. As expected, Co9S8/SnS@MCNFs exhibit remarkable initial coulombic efficiency (ICE = 92.6 %) and demonstrate stable long-term cycling performance (222.5 mA h g−1 at 2 A g−1 after 400 cycles) for sodium storage, with only a 0.18 % decay rate per cycle. These findings suggest promising application for the electrode material in sustained high-current discharges and long-endurance performance.

Ni nanoparticles embedded in multi-channel carbon nanofibers: Self-supporting electrodes for bifunctional catalysis of hydrogen and oxygen evolution reactions

Nitrogen-doped carbon nanofibers with multi-channels loaded with nanoscale nickel particles (Ni-MNCNF) were achieved by the combination of coaxial electrospinning and pyrolysis. Which was used as a self-supporting electrode for electrochemical hydrogen and oxygen evolution reactions. The multi-channels of the fiber facilitated the fast mass transfer as well as endowed it with more exposed active sites. In addition, nanoscale Ni crystals were dispersed evenly on the fiber walls due to the confinement effect of carbon materials. Furthermore, carbon nanofibers provided an excellent conductive network, which expedited the charge transfer rate and further enhanced catalytic activity. At a current density of 10 mA cm−2, the overpotentials for the hydrogen evolution reaction (HER) were only 65 mV and 203 mV in alkaline and acidic electrolytes, respectively, and the overpotential for the oxygen evolution reaction (OER) was 193 mV in an alkaline electrolyte, promoting its potential industrial applications and reducing the negative impact on the environment. This research presented a strategy for designing self-supporting transition metal-based catalysts with superior activity.

Molybdenum single-atoms decorated multi-channel carbon nanofibers for advanced lithium-selenium batteries.

The cathode in lithium-selenium (Li-Se) batteries has garnered extensive attention owing to its superior specific capacity and enhanced conductivity compared to sulfur. Nonetheless, the adoption and advancement of Li-Se batteries face significant challenges due to selenium's low reactivity, substantial volume fluctuations, and the shuttle effect associated with polyselenides. Single-atom catalysts (SACs) are under the spotlight for their outstanding catalytic efficiency and optimal atomic utilization. To address the challenges of selenium's low chemical activity and volume expansion in Li-Se batteries, through electrospun, we have developed a lotus root-inspired carbon nanofiber (CNF) material, featured internal multi-channels and anchored with molybdenum (Mo) single atoms (Mo@CNFs). Mo single atoms significantly enhance the conversion kinetics of selenium (Se), facilitating rapid formation of Li2Se. The internally structured multi-channel CNF serves as an effective host matrix for Se, mitigating its volume expansion during the electrochemical process. The resulting cathode, Se/Mo@CNF composite, exhibits a high discharge specific capacity, superior rate performance, and impressive cycle stability in Li-Se batteries. After 500 cycles at a current density of 1 C, it maintains a capacity retention rate of 82% and nearly 100% coulombic efficiency (CE). This research offers a new avenue for the application of single-atom materials in enhancing advanced Li-Se battery performance.

Achieving High-Rate and Stable Sodium-Ion Storage by Constructing Okra-Like NiS2/FeS2@Multichannel Carbon Nanofibers.

Transition metal sulfides (TMSs) are considered as promising anode materials for sodium-ion batteries (SIBs) due to their high theoretical capacities. However, the relatively low electrical conductivity, large volume variation, and easy aggregation/pulverization of active materials seriously hinder their practical application. Herein, okra-like NiS2/FeS2 particles encapsulated in multichannel N-doped carbon nanofibers (NiS2/FeS2@MCNFs) are fabricated by a coprecipitation, electrospinning, and carbonization/sulfurization strategy. The combined advantages arising from the hollow multichannel structure in carbon skeleton and heterogeneous NiS2/FeS2 particles with rich interfaces can provide facile ion/electron transfer paths, ensure boosted reaction kinetics, and help maintain the structural integrity, thereby resulting in a high reversible capacity (457 mA h g-1 at 1 A g-1), excellent rate performance (350 mA h g-1 at 5 A g-1), and outstanding long-term cycling stability (93.5% retention after 1100 cycles). This work provides a facile and efficient synthetic strategy to develop TMS-based heterostructured anode materials with high-rate and stable sodium storage properties.

Unraveling the Nucleation and Growth Mechanism of Potassium Metal on 3D Skeletons for Dendrite-Free Potassium Metal Batteries.

Designing three-dimensional (3D) porous carbonaceous skeletons for K metal is one of the most promising strategies to inhibit dendrite growth and enhance the cycle life of potassium metal batteries. However, the nucleation and growth mechanism of K metal on 3D skeletons remains ambiguous, and the rational design of suitable K hosts still presents a significant challenge. In this study, the relationships between the binding energy of skeletons toward K and the nucleation and growth of K are systematically studied. It is found that a high binding energy can effectively decrease the nucleation barrier, reduce nucleation volume, and prevent dendrite growth, which is applied to guide the design of 3D current collectors. Density functional theory calculations show that P-doped carbon (P-carbon) exhibits the highest binding energy toward K compared to other elements (e.g., N, O). As a result, the K@P-PMCFs (P-binding porous multichannel carbon nanofibers) symmetric cell demonstrates an excellent cycle stability of 2100 h with an overpotential of 85 mV in carbonate electrolytes. Similarly, the perylene-3,4,9,10-tetracarboxylic dianhydride || K@P-PMCFs cell achieves ultralong cycle stability (85% capacity retention after 1000 cycles). This work provides a valuable reference for the rational design of 3D current collectors.

Multifunctional Heterostructured Fe3O4-FeTe@MCM Electrocatalyst Enabling High-Performance Practical Lithium-Sulfur Batteries Via Built-in Electric Field.

The development of capable of simultaneously modulating the sluggish electrochemical kinetics, shuttle effect, and lithium dendrite growth is a promising strategy for the commercialization of lithium-sulfur batteries. Consequently, an elaborate preparation method is employed to create a host material consisting of multi-channel carbon microspheres (MCM) containing highly dispersed heterostructure Fe3O4-FeTe nanoparticles. The Fe3O4-FeTe@MCM exhibitsa spontaneous built-in electric field (BIEF) and possesses both lithophilic and sulfophilic sites, rendering it an appropriate host material for both positive and negative electrodes. Experimental and theoretical results reveal that the existence of spontaneous BIEF leads to interfacial charge redistribution, resulting in moderate polysulfide adsorption which facilitates the transfer of polysulfides and diffusion of electrons at heterogeneous interfaces. Furthermore, the reduced conversion energy barriers enhanced the catalytic activity of Fe3O4-FeTe@MCM for expediting the bidirectional sulfur conversion. Moreover, regulated Li deposition behavior is realized because of its high conductivity and remarkable lithiophilicity. Consequently, the battery exhibited long-term stability for 500 cycles with 0.06% capacity decay per cycle at 5 C, and a large areal capacity of 7.3mAhcm-2 (sulfur loading: 9.73mgcm-2) at 0.1 C. This study provides a novel strategy for the rational fabrication of heterostructure hosts for practical Li-S batteries.

Zero-Strain Sodium Lanthanum Titanate Perovskite Embedded in Flexible Carbon Fibers as a Long-Span Anode for Lithium-Ion Batteries.

"High-capacity" graphite and "zero-strain" spinel Li4Ti5O12 (LTO) occupy the majority market of anode materials for Li+ storage in commercial applications. Nevertheless, their intrinsic drawbacks including the unsafe potential of graphite and unsatisfactory capacity of LTO limit the further development of lithium-ion batteries (LIBs), which is unable to satisfy the ever-increasing demands. Here, a novel Na0.35La0.55TiO3 perovskite embedded in multichannel carbon fibers (NLTO-NF) is rationally designed and synthesized through an electrospinning method. It not only has the advantages of a respectable specific capacity of 265 mAh g-1 at 0.1 A g-1 and superb rate capability, but it also possesses the zero-strain characteristic. Impressively, an ultralong cycling life with 96.3% capacity retention after 9000 cycles at 2 A g-1 is achieved in the half cell, and 90.3% of capacity retention ratio is obtained after even 2500 cycles at 1 A g-1 in the coupled LiFePO4/NLTO-NF full cell. This study introduces a new member with excellent performance to the zero-strain materials family for next-generation LIBs.

Self-supporting multi-channel Janus carbon fibers: A new strategy to achieve an efficient bifunctional electrocatalyst for overall water splitting

A new type of self-supporting multi-channel Janus carbon fibers with efficient water splitting has been successfully manufactured using a specially designed parallel spinneret through electrospinning technology and subsequent carbonization technique. Every single Janus fiber composes of a half side of Mo2C and the other half side of Ni components as Mo2C, Ni embedded in N-doped multi-channel Janus carbon fibers ([Mo2C/C]//[Ni/C]-NMCFs) for overall water splitting. Under optimized condition, the hydrogen evolution reaction overpotential of [Mo2C/C]//[Ni/C]-NMCFs (62 mV) is just 24 mV higher than 20 wt% Pt/C (38 mV) at a current density of 10 mA cm−2. Furthermore, it achieves current density of 10 mA cm−2 to require an overpotential of 324 mV for oxygen evolution reaction. Additionally, the cell assembled by the identical [Mo2C/C]//[Ni/C]-NMCFs catalyst as both the cathode and anode needs only 1.607 V at a current density of 10 mA cm−2, which is only 0.022 V higher than that of Pt/C-IrO2 electrodes. Moreover, [Mo2C/C]//[Ni/C]-NMCFs catalyst also exhibits a long-term stability. The synergistic effect and unique heterostructure of Mo2C and Ni enhance the catalytic activity.

Achieving a Quasi‐Solid‐State Conversion of Polysulfides via Building High Efficiency Heterostructure for Room Temperature Na–S Batteries

AbstractThe practical application of room temperature sodium–sulfur (RT Na–S) batteries are prevented by the sulfur insulation, the severe shuttling effect of high‐order sodium polysulfides (Na2Sn, 4 ≤ n ≤ 8), and the sluggish reaction kinetics. Therefore, designing an ideal host material to suppress the polysulfides shuttle process and accelerate the redox reactions of soluble NaPSs to Na2S2/Na2S is of paramount importance for RT Na–S batteries. Here, a quasi‐solid‐state transformation of NaPSs is realized by building high efficiency MoC‐W2C heterostructure in freestanding multichannel carbon nanofibers via electrospinning and calcination methods (MoC‐W2C‐MCNFs). The multichannel carbon nanofibers are interlinked micro‐mesoporous structures that can accommodate volume change of electrode materials and confine the entire redox process of NaPSs (restraining the polysulfides shuttle process). Meanwhile, the MoC‐W2C heterostructure with abundant heterointerfaces can facilitate electron/ion transport and accelerate conversion of NaPSs. Consequently, the S/MoC‐W2C‐MCNFs cathode delivers a high capacity of 640 mAh g−1 after 500 cycles at 0.2 A g−1 and an excellent reversible performance of 200 mAh g−1 after ultralong 3500 cycles at 4 A g−1. What's more, the heterostructure catalytic mechanism (a quasi‐solid‐state transformation) is proposed and confirmed in carbonate electrolyte by combining experimentally and theoretically.

Construction of Phosphorus‐Functionalized Multichannel Carbon Interlayers for Dendrite‐Free Metallic Zn Anodes

Zn metal anodes are usually subject to grave dendrite growth during platting/stripping, which dramatically curtails the lifespan of aqueous Zn‐ion batteries and capacitors. To address above problems, in our work, a novel phosphorus‐functionalized multichannel carbon interlayer was designed and covered on Zn anodes. The results demonstrated that the multichannel structure combined with the three‐dimensional meshy skeleton can provide more sufficient space for Zn deposition, thereby effectively inhibiting the growth of zinc dendrites. Meanwhile, theoretical calculations also confirmed that the P–C and P=O functional groups from phosphorus‐functionalized multichannel carbon interlayer have the decisive influence in reducing the zinc nucleation potential and depositing uniformly zinc. Concretely, the symmetrical battery assembled with phosphorus‐functionalized multichannel carbon interlayer‐covered Zn anodes possessed a long lifetime of 3300 h at 2 mA cm−2 with 1 mAh cm−2. Furthermore, the full cell with activated carbon cathodes exhibited a high specific capacity of 80.5 mAh g−1 and outstanding cycling stability without capacity decay after 15 000 cycles at a high current density of 5 A g−1. The superior electrochemical performance exceeded that of most reported papers. Consequently, our synthesized zincophilic interlayer with the unique structure has superior prospects for application in stabilizing zinc anodes and prolonging the lifespan of batteries.

Construction of Fe Nanoclusters/Nanoparticles to Engineer FeN4 Sites on Multichannel Porous Carbon Fibers for Boosting Oxygen Reduction Reaction

AbstractFe–N–C catalysts are emerging as promising alternatives to Pt‐based catalysts for the oxygen reduction reaction (ORR), while they still suffer from sluggish reaction kinetics due to the discontented binding affinity between the Fe‐N4 sites and oxygen‐containing intermediates, and unsatisfactory stability. Herein, a flexible multichannel carbon fiber membrane immobilized with atomically dispersed Fe‐N4 sites and neighboring Fe nanoclusters/nanoparticles (FeN4‐FeNCP@MCF) is synthesized. The optimized geometric and electronic structures of the Fe atomic sites brought by adjacent Fe nanoclusters/nanoparticles and hierarchically porous structure of the carbon matrix endow FeN4‐FeNCP@MCF with outstanding ORR activity and stability, considerably outperforming its counterpart with FeN4 sites only and the commercial Pt/C catalyst. Liquid and solid‐state flexible zinc–air batteries employing FeN4‐FeNCP@MCF both exhibit outstanding durability. Theoretical calculation reveals that the Fe nanoclusters can trigger remarkable electron redistribution of the FeN4 sites and modulate the hybridization of central Fe 3d and O 2p orbitals, facilitating the activation of O2 molecules and optimizing the adsorption capacity of oxygen‐containing intermediates on FeN4 sites, and thus accelerating the ORR kinetic. This work offers an effective approach to constructing coupling catalysts that have single atoms coexisting with nanoclusters/nanoparticles for efficient ORR catalysis.

Novel N-doped multichannel carbon nanofiber architecture with porous CoS nanoprisms for high-performance potassium-ion batteries

Novel N-doped multichannel carbon nanofiber architecture with porous CoS nanoprisms for high-performance potassium-ion batteries

ZnS/CuS nanoparticles encapsulated in multichannel carbon fibers as high-performance anode materials for flexible Li-ion capacitors

ZnS/CuS nanoparticles encapsulated in multichannel carbon fibers as high-performance anode materials for flexible Li-ion capacitors

Highly flexible multilayer MXene hollow carbon nanofibers confined with Fe3C particles for high-performance lithium-ion batteries

Designing electrode structures with excellent mechanical properties, fast electrochemical kinetics and stability is important for the development of flexible wearable electrodes. In this paper, a hollow carbon nanofiber composite of Ti3C2Tx MXene and Fe3C nanoparticles is designed. The synergistic effect of Ti3C2Tx MXene and Fe3C nanoparticles forms a strong conductive channel with the hollow channel to form a dual conductive channel, which plays an important role in the preparation of high-performance lithium-ion batteries. Benefiting from the advantages of the above structure, the Fe3C@MXene/hollow multichannel carbon fibers (Fe3C@MXene/HMCFs) electrodes at a current density of 0.2 A/g achieve an initial capacity of 1294 mA h g−1 and a high reversible capacity of 831 mA h g−1 after 200 turns of charge/discharge cycles.

A two-step electrochemical biosensor based on Tetrazyme for the detection of fibrin.

In this study, an electrochemical biosensor was constructed for the detection of fibrin, specifically by a simple two-step approach, with a novel artificial enzyme (Tetrazyme) based on the DNA tetrahedral framework as signal probe. The multichannel screen-printed electrode with the activated surface cannot only remove some biological impurities, but also serve as a carrier to immobilize a large number of antigen proteins. The DNA tetrahedral nanostructure was employed to ensure the high sensitivity of the probe for biological analysis. The hemin was chimeric into the G-quadruplex to constitute the complex with peroxidase catalytic activity (hemin/G4-DNAzyme), subsequently, Tetrazyme was formed through combining of this complex and DNA tetrahedral nucleic acid framework. The artificial enzyme signal probe formed by the covalent combination of the homing peptide (Cys-Arg-Glu-Lys-Ala, CREKA), which is the aptamer of fibrin and the new artificial enzyme is fixed on the surface of the multichannel carbon electrode by CREKA-specific recognition, so as to realize the sensitive detection of fibrin. The feasibility of sensing platform was validated by cyclic voltammetry (CV) and amperometric i-t curve (IT) methods. Effects of Tetrazyme concentration, CREKA concentrations and hybridization time on the sensor were explored. Under the best optimal conditions of 0.6μmol/L Tetrazyme, 80μmol/L CREKA, and 2.5h reaction time, the immunosensor had two linear detection ranges, 10-40nmol/L, with linear regression equation Y = 0.01487X-0.011 (R2 = 0.992), and 50-100nmol/L, with linear regression equation Y = 0.00137X+0.6405 (R2 = 0.998), the detection limit was 9.4nmol/L, S/N≥3. The biosensor could provide a new method with great potential for the detection of fibrin with good selectivity, stability, and reproducibility.

Competing polysulfides conversion between edge-N and embedded CoS2 within multichannel carbon nanofibers

The practical application of lithium-sulfur batteries (LSBs) is hindered by a range of challenges, including slow conversion kinetics and inevitable shuttle effect of lithium polysulfide (LiPSs) intermediates, low electrical conductivity and rigorous volume expansion of sulfur. To address these challenges, we initiatively propose a competing catalytic mechanism dominated by two functional components, which aims to accelerate the liquid–liquid–solid conversion for the sulfur reduction reaction (SRR). To achieve this goal, we construct multichannel carbon fibers decorated with edge nitrogen and CoS2 nanoparticles (CoS2/NMCNF) as the cathode host for LSBs. The internal channels provide spatial constraints towards alleviating volume expansion and accelerating electron/ion transmission. Moreover, based on theoretical calculations and experiments, there is a competition between edge nitrogen and embedded CoS2 for catalytic conversion of LiPSs, of which CoS2 plays a major role in the liquid–liquid conversion (Li2S6–Li2S4), while edge-N accelerates the liquid–solid conversion (Li2S4–Li2S2). Consequently, the prepared CoS2/NMCNF electrode has an excellent performance with high initial specific capacity (1,437.9 mAh/g at 0.2C), excellent cycling stability at 3.0C (only about 0.032% capacity decay per cycle after 650cycles), and maintaining good cycling stability even when the sulfur loading increases to 4.10 mg cm−2. This work demonstrates a unique competing catalytic mechanism for the liquid–liquid–solid conversion process of LSBs.