Polar Materials Research Articles

Study of Integer Spin S = 1 in the Polar Magnet β-Ni(IO3)2.

Polar magnetic materials exhibiting appreciable asymmetric exchange interactions can potentially host new topological states of matter such as vortex-like spin textures; however, realizations have been mostly limited to half-integer spins due to rare numbers of integer spin systems with broken spatial inversion lattice symmetries. Here, we studied the structure and magnetic properties of the S = 1 integer spin polar magnet β-Ni(IO3)2 (Ni2+, d8, 3F). We synthesized single crystals and bulk polycrystalline samples of β-Ni(IO3)2 by combining low-temperature chemistry techniques and thermal analysis and characterized its crystal structure and physical properties. Single crystal X-ray and powder X-ray diffraction measurements demonstrated that β-Ni(IO3)2 crystallizes in the noncentrosymmetric polar monoclinic structure with space group P21. The combination of the macroscopic electric polarization driven by the coalignment of the (IO3)− trigonal pyramids along the b axis and the S = 1 state of the Ni2+ cation was chosen to investigate integer spin and lattice dynamics in magnetism. The effective magnetic moment of Ni2+ was extracted from magnetization measurements to be 3.2(1) µB, confirming the S = 1 integer spin state of Ni2+ with some orbital contribution. β-Ni(IO3)2 undergoes a magnetic ordering at T = 3 K at a low magnetic field, μ0H = 0.1 T; the phase transition, nevertheless, is suppressed at a higher field, μ0H = 3 T. An anomaly resembling a phase transition is observed at T ≈ 2.7 K in the Cp/T vs. T plot, which is the approximate temperature of the magnetic phase transition of the material, indicating that the transition is magnetically driven. This work offers a useful route for exploring integer spin noncentrosymmetric materials, broadening the phase space of polar magnet candidates, which can harbor new topological spin physics.

Lithiated Sulfur-Incorporated, Polymeric Cathode for Durable Lithium-Sulfur Batteries with Promoted Redox Kinetics.

Even though lithium-sulfur (Li-S) batteries have made much progress in terms of the delivered specific capacity and cycling stability by the encapsulation of sulfur within conductive carbon matrixes or polar materials, challenges such as low active sulfur utilization and unacceptable Coulombic efficiency are still hindering their commercial use. Herein, a lithium-rich conjugated sulfur-incorporated, polymeric material based on poly(Li2S6-r-1,3-diisopropenylbenzene) (DIB) is developed as a cathode material for high rate and stable Li-S batteries. Motivated by extra Li+ ions affording fast Li+ redox kinetics across the conjugated aromatic backbones, the Li-rich sulfur-based copolymer exhibits high delivery capacities (934 mAh g-1 at 120 cycles), impressive rate capabilities (727 mAh g-1 even under a current of 2 A g-1), and long electrochemical cycling performance over 500 cycles. Moreover, by use of the elastic nature and thermoplastic properties of the sulfur-incorporated, polymeric material, a prototype of a flexible Li-S pouch cell is constructed by using a poly(Li2S6-r-DIB) copolymer cathode and paired with the flexible carbon cloth/Si/Li anode, which exhibits stable electrochemical performance (658 mAh g-1 after 100 cycles) and operational capability even under folding at various angle (30°, 60°, 90°, 120°, 150°, 180°). This work extends the molecular-design approach to obtaining a high-performance organosulfur cathode material by introducing extra Li+ ions to promote redox kinetics, which provides valuable guidance for the development of high-performance Li-S batteries for practical applications.

Comparative analysis of dielectric, shear mechanical and light scattering response functions in polar supercooled liquids

The studies of molecular dynamics in the vicinity of liquid–glass transition are an essential part of condensed matter physics. Various experimental techniques are usually applied to understand different aspects of molecular motions, i.e., nuclear magnetic resonance (NMR), photon correlation spectroscopy (PCS), mechanical shear relaxation (MR), and dielectric spectroscopy (DS). Universal behavior of molecular dynamics, reflected in the invariant distribution of relaxation times for different polar and weekly polar glass-formers, has been recently found when probed by NMR, PCS, and MR techniques. On the other hand, the narrow dielectric permittivity function ε*(f) of polar materials has been rationalized by postulating that it is a superposition of a Debye-like peak and a broader structural relaxation found in NMR, PCS, and MR. Herein, we show that dielectric permittivity representation ε*(f) reveals details of molecular motions being undetectable in the other experimental methods. Herein we propose a way to resolve this problem. First, we point out an unresolved Johari–Goldstein (JG) β-relaxation is present nearby the α-relaxation in these polar glass-formers. The dielectric relaxation strength of the JG β-relaxation is sufficiently weak compared to the α-relaxation so that the narrow dielectric frequency dispersion faithfully represents the dynamic heterogeneity and cooperativity of the α-relaxation. However, when the other techniques are used to probe the same polar glass-former, there is reduction of relaxation strength of α-relaxation relative to that of the JG β relaxation as well as their separation. Consequently the α relaxation appears broader in frequency dispersion when observed by PCS, NMR and MR instead of DS. The explanation is supported by showing that the quasi-universal broadened α relaxation in PCS, NMR and MR is captured by the electric modulus M*(f) = 1/ε*(f) representation of the dielectric measurements of polar and weakly polar glass-formers, and also M*(f) compares favorably with the mechanical shear modulus data G*(f).

Nanometric phonon spectroscopy for diamond and cubic boron nitride

Local phonon properties near heterointerfaces or lattice defects are key for controlling various material properties such as thermal conductivity and thermoelectricity. However, high-spatial-resolution measurements of bulk phonons have hardly been established, even in typical nonpolar and polar bulk materials such as diamond and cubic boron nitride (c-BN), respectively. Here, we demonstrate nanometric measurements of phonon dispersions and mapping using a heterojunction of diamond and c-BN single crystals. To achieve high spatial/energy resolution, we use a monochromated (\ensuremath{\sim}20--30 meV) electron nanoprobe, a high-sensitivity scintillator for counting inelastically scattered electrons, and the Richardson--Lucy deconvolution. The diamond phonon dispersion is first measured under a large-scattering-vector condition, particularly for the \ensuremath{\Gamma} point. Differential scattering cross sections of optical and acoustic-phonon modes in diamond and c-BN are also measured, and the totals of their modes are on the order of ${10}^{\ensuremath{-}5}\phantom{\rule{0.16em}{0ex}}\mathrm{n}{\mathrm{m}}^{2}$ for both crystals.

On the Role of Long-Range Electrostatics in Machine-Learned Interatomic Potentials for Complex Battery Materials

Modeling complex energy materials such as solid-state electrolytes (SSEs) realistically at the atomistic level strains the capabilities of state-of-the-art theoretical approaches. On one hand, the system sizes and simulation time scales required are prohibitive for first-principles methods such as the density functional theory. On the other hand, parameterizations for empirical potentials are often not available, and these potentials may ultimately lack the desired predictive accuracy. Fortunately, modern machine learning (ML) potentials are increasingly able to bridge this gap, promising first-principles accuracy at a much reduced computational cost. However, the local nature of these ML potentials typically means that long-range contributions arising, for example, from electrostatic interactions are neglected. Clearly, such interactions can be large in polar materials such as electrolytes, however. Herein, we investigate the effect that the locality assumption of ML potentials has on lithium mobility and defect formation energies in the SSE Li7P3S11. We find that neglecting long-range electrostatics is unproblematic for the description of lithium transport in the isotropic bulk. In contrast, (field-dependent) defect formation energies are only adequately captured by a hybrid potential combining ML and a physical model of electrostatic interactions. Broader implications for ML-based modeling of energy materials are discussed.

Super-Planckian thermal radiation between 2D phononic hBN monolayers

Near-field radiation heat transfer (NFRHT) in two-dimensional (2D) hexagonal boron nitride (hBN) monolayer and its composite symmetric-based structure was investigated. Contrary to three-dimensional (3D) materials, the splitting of modes (in 2D materials) into the longitudinal optical (LO) and transverse optical (TO) phononic modes disappears at the Γ-point even in some polar materials. The conductivity of atomic thin hBN monolayer depends on the LO phonon frequency under the long wavelength limit. Exploiting such concept, the electromagnetic local density of states (EM-LDOS) accounting for the near-field radiation spectrum was evaluated in free-space close to an interface with the hBN monolayer as well as composite structures. An intense narrow peak of LDOS was found in the case of hBN monolayer caused by the surface phonon polariton (SPhP) resonance. This peak was modified in the case of hBN-graphene composite due to hybridization, which strongly depends on two factors – the distance of observer (in vacuum) from interface and graphene Fermi energy. It was found that the flux density between monolayer hBN gets 2.8-fold enhanced as compared to the monolayer graphene configuration under 0.11 eV Fermi energy applied at a vacuum gap of 15 nm. The possibility of tuning Fermi energy has great potentials in designing thermally controlled devices.

Utilization of activated carbons produced from some natural materials in the purification of used frying oil

The activated carbons (ACs) from shells of horse chestnut, chestnut, acorn, pistachio, apricot kernel, and wood shavings were evaluated to recover used oil (UO). The effects of the amount of AC, adsorption time, and temperature on the purification of the UO were investigated using the apricot kernel shells due to the high apricot production of Turkey. The kinetic evaluation was also done. The percentage improvements (PIs) in total polar materials (TPM), free fatty acids (FFA), p-anisidine value (p-AV), conjugated diene content (CD), and color of UO were found as 100, 56, 92, 51, and 90% for the apricot kernel AC in the column treatment. The most effective other ACs in decreasing FFA, p-AV, CD, and color were the horse chestnut (59%), chestnut (74%), chestnut (43%), and pistachio (72%), respectively. Consequently, these ACs can be used for the purification of UO. Practical applications Industrial wastes cause environmental pollution if they are ejected into river, sea, and soil. Therefore, they should be purified or treated for different purposes. In this study, the industrial wastes from the food and forest industries were used for the production of activated carbon to purify the used oil. The results showed that these activated carbons could be utilized for the regeneration of used oils. The most economical treatment is to blend the activated carbon with used frying oil for a certain time and remove it through centrifugation and filtration. The purified oil has the potential to be used in the biodiesel production.

Waterborne Polyurethane Enhanced, Adhesive, and Ionic Conductive Hydrogel for Multifunctional Sensors

In the past two decades, ionic conductive hydrogel has attracted tremendous research interests for their intrinsic characteristics in the field of flexible sensor. However, synchronous achievement of high mechanical strength, satisfied ionic conductivity, and broad adhesion to various substrates is still a challenge. Herein, a novel zwitterionic composite hydrogel that displayed excited strechability (up to 900%), satisfied strength (about 30kPa), high ionic conductivity (1.2 mScm-1 ), and adhesion to polar and nonpolar materials is fabricated though the combination of waterborne polyurethanes (PU) and poly(sulfobetaine zwitterion-co-acrylamide) (SAm). Especially, this facile strategy demonstrates that PU has a synergistic effect on enhancing mechanical strength and ionic conductivity for ionic conductive hydrogel. Moreover, the hydrogel-based strain/stress sensor shows high sensitivity, wide sensing range, great stability, and accuracy for human body movements detecting and voice recognition. This novel ionic conductive hydrogel has promoted the development of wearable devices.

Co9S8-C-Li2S composite synthesized via synchronous carbothermal reduction process as cathode material for high-performance Li-ion-S batteries

An economic and convenient synchronous carbothermal reduction is introduced to prepare Co9S8-C-Li2S composite as cathode material for Li-ion-S battery. The synthesized Co9S8-C-Li2S composite greatly reduces the cost of Li2S cathode. Furthermore, small particles of Li2S and Co9S8 are formed in-situ at the same time and distribute uniformly in carbon matrix. Meanwhile, the formation of the polar material Co9S8 effectively inhibits the “shuttle effect”, regulates the electrochemical reaction between Li2S and S, and significantly reduces the activation voltage of Li2S. As a result, Li-ion-S battery with Co9S8-C-Li2S cathode exhibits a lower active voltage of 2.5 V and a higher initial charge specific capacity of 1166 mA h g−1.

Spin and Orbital Effects on Asymmetric Exchange Interaction in Polar Magnets: M(IO3)2 (M = Cu and Mn).

Magnetic polar materials feature an astonishing range of physical properties, such as magnetoelectric coupling, chiral spin textures, and related new spin topology physics. This is primarily attributable to their lack of space inversion symmetry in conjunction with unpaired electrons, potentially facilitating an asymmetric Dzyaloshinskii-Moriya (DM) exchange interaction supported by spin-orbital and electron-lattice coupling. However, engineering the appropriate ensemble of coupled degrees of freedom necessary for enhanced DM exchange has remained elusive for polar magnets. Here, we study how spin and orbital components influence the capability of promoting the magnetic interaction by studying two magnetic polar materials, α-Cu(IO3)2 (2D) and Mn(IO3)2 (6S), and connecting their electronic and magnetic properties with their structures. The chemically controlled low-temperature synthesis of these complexes resulted in pure polycrystalline samples, providing a viable pathway to prepare bulk forms of transition-metal iodates. Rietveld refinements of the powder synchrotron X-ray diffraction data reveal that these materials exhibit different crystal structures but crystallize in the same polar and chiral P21 space group, giving rise to an electric polarization along the b-axis direction. The presence and absence of an evident phase transition to a possible topologically distinct state observed in α-Cu(IO3)2 and Mn(IO3)2, respectively, imply the important role of spin-orbit coupling. Neutron diffraction experiments reveal helpful insights into the magnetic ground state of these materials. While the long-wavelength incommensurability of α-Cu(IO3)2 is in harmony with sizable asymmetric DM interaction and low dimensionality of the electronic structure, the commensurate stripe AFM ground state of Mn(IO3)2 is attributed to negligible DM exchange and isotropic orbital overlapping. The work demonstrates connections between combined spin and orbital effects, magnetic coupling dimensionality, and DM exchange, providing a worthwhile approach for tuning asymmetric interaction, which promotes evolution of topologically distinct spin phases.

Tuning the intrinsic electric field of Janus-TMDs to realize high-performance β-Ga2O3 device based on β-Ga2O3/Janus-TMD heterostructures

Although two-dimensional (2D) transition metal dichalcogenides (TMDs) have been employed for improving the optoelectronic performance of a β-Ga2O3 solar-blind photodetector, how to employ the intrinsic electric field (Ein) of 2D materials to tune the optoelectronic performance of β-Ga2O3 devices further has not yet been demonstrated. Here, by investigating the optoelectronic properties of β-Ga2O3/Janus-TMD heterostructures with different Eins, we found that the heterostructures exhibit type-I band alignment when the Ein direction points to the contact interface, whereas it demonstrates type-II band alignment for the opposite Ein direction. Compared with the former, the latter possesses more stability, stronger charge transport efficiency, higher optical absorption, and lower exciton binding energy, which are further improved as the intensity of the Ein enlarges. The band offsets of all β-Ga2O3/Janus-TMD heterostructures can be enlarged when the Ein is enhanced by altering the chalcogens in the Janus-TMDs, whereas they are reduced when the Ein is enlarged by altering the metals. The underlying mechanisms are due to the direction and intensity of Ein for Janus-TMDs directly affecting its band levels, band bending of β-Ga2O3 surface and charge transfer at the β-Ga2O3/Janus-TMD interface. These findings reveal the role of Ein in asymmetrical polar 2D materials on the optoelectronic performances of β-Ga2O3 devices, and provide a guideline to design high performance Ga2O3 optoelectronic devices.

A pH‐Neutral Polyelectrolyte Hole Transport Layer for Improved Energy Band Structure at the Anode/PTB7 Junction and Improved Solar Cell Performance

In organic solar cells (OSCs), interfacial properties between the donor phase and hole transport layers (HTLs) are critical factors which govern charge extraction efficiency. Many ionic and polar materials are known to function as effective interfacial layers; however, an understanding of how ionic moieties affect the electronic band structure and characteristics of OSCs is lacking. Herein, a new, pH‐neutral polyelectrolyte is introduced that resolves several problems which are encountered with the commonly used HTL, poly(3,4‐ethylenedioxythiopene):polystyrenesulfonate (PEDOT:PSS). An effective p‐type polyelectrolyte dopant is designed, comprising an anionically charged PSS backbone with easily reduced Cu2+ counterions (Cu:PSS), and interfacial properties for HTL/donor interfaces by photoelectron spectroscopy are analyzed. The effects of the polyelectrolyte on interfacial energy levels and charge extraction efficiency between the active layer and HTL are quantified. Using optimized processing conditions, the efficiency can be improved from 8.31% to 9.28% in conventional OSCs compared with a standard PEDOT:PSS HTL. The energy‐level alignment at the HTLs/donor interface determined by UV photoelectron spectroscopy measurements reveals the origin of distinct differences in device performances. The reduced ionization potential (IP) and hole injections barrier (Φh) at the HTL/donor interface play a crucial role in efficient charge extraction in conventional OSCs.

Coupling Charge and Topological Reconstructions at Polar Oxide Interfaces.

In oxide heterostructures, different materials are integrated into a single artificial crystal, resulting in a breaking of inversion symmetry across the heterointerfaces. A notable example is the interface between polar and nonpolar materials, where valence discontinuities lead to otherwise inaccessible charge and spin states. This approach paved the way for the discovery of numerous unconventional properties absent in the bulk constituents. However, control of the geometric structure of the electronic wave functions in correlated oxides remains an open challenge. Here, we create heterostructures consisting of ultrathin SrRuO_{3}, an itinerant ferromagnet hosting momentum-space sources of Berry curvature, and LaAlO_{3}, a polar wide-band-gap insulator. Transmission electron microscopy reveals an atomically sharp LaO/RuO_{2}/SrO interface configuration, leading to excess charge being pinned near the LaAlO_{3}/SrRuO_{3} interface. We demonstrate through magneto-optical characterization, theoretical calculations and transport measurements that the real-space charge reconstruction drives a reorganization of the topological charges in the band structure, thereby modifying the momentum-space Berry curvature in SrRuO_{3}. Our results illustrate how the topological and magnetic features of oxides can be manipulated by engineering charge discontinuities at oxide interfaces.

Raman Spectra of Bulk and Few-Layer GeSe From First-Principles Calculations

Raman spectra play a significant role in the study of polar materials. Herein, we report the influence of strain and interlayer shift on vibration responses in bulk and few-layer ferrovalley material GeSe in different polarization states (ferroelectric/FE and antiferroelectric/AFE) based on density functional theory and density functional perturbation theory calculations. We find Ag1 mode shifts by about 10 cm−1 from monolayer to bilayer and trilayer due to the interlayer coupling. The Ag3 mode on behalf of FE mode is observed that is consistent with the experiments in bulk and few-layer GeSe. Meanwhile, in our calculations, with the transition between AFE and FE state in the bilayer and trilayer, the Raman frequency of Ag2 and Ag3 mode decrease obviously whereas that of Ag1 mode increases. Interestingly, the Raman peaks shifted a lot due to the strain effect. We expect these variations in the Raman spectroscopy can be employed to identify the status of GeSe films, e.g., the AFE or FE state, and the number of layers in experiments.

Guest-Mediated Hierarchical Self-Assembly of Dissymmetric Organic Cages to Form Supramolecular Ferroelectrics

Guest-Mediated Hierarchical Self-Assembly of Dissymmetric Organic Cages to Form Supramolecular Ferroelectrics

Low hysteresis and enhanced figure-of-merit of pyroelectric energy conversion at compatible phase transformation

The pyroelectricity of polar materials provides great potential for electricity generation from waste heat. The pyroelectric effect of the material can be magnificently enhanced at a first-order phase transformation due to the abrupt jump in spontaneous polarization within a narrow temperature range. Here, we show that the performance of energy conversion by phase transformation is inversely resonant with the hysteresis of thermally driven structural transformations in a (Ba1−xSrx) (Hf0.02Ce0.005Ti0.975)O3 system, corresponding to a singular lattice distortion mode satisfying the crystallographic compatibility condition. Among the finely tuned Sr compositions from 0.04 to 0.10, we discovered that Sr0.07 composition is a promising material candidate in this material system for pyroelectric energy conversion. Our work suggests a rational strategy of material development for pyroelectric energy conversion applications.

Sunflower Oil–Beeswax Oleogels Are Promising Frying Medium for Potato Strips

AbstractSunflower oil–beeswax oleogels at 3% (BWO‐3) and 8% (BWO‐8) organogelator concentration are prepared to evaluate oleogels as frying medium for potato strip frying against commercial sunflower oil (SO). Rheological and thermal analyses of oleogels prove that the samples are fully solid (20±3 °C) and totally liquid (180 °C), and thermoreversible. Fresh and used (after frying) fat analyses show that free fatty acidity (FFA), peroxide value (PV) and total polar materials (TPM) are enhanced in all samples at the 7th h, but the relative enhancement levels are lower in oleogel samples. Potato strips fried in oleogels absorb significantly less oil (11.97% and 12.07%) than the control sample (15.20%). Potatoes fried in oleogels are also more bright and yellower than the control sample. Textural profile of the fried potatoes indicates that the samples fried in oleogels are harder, springier, and gummier than that of the control sample. Sensory analysis shows that oleogel fried potatoes get higher sensory scores. Also, overall acceptability of potatoes fried in BWO‐8 sample is the highest (8.50) among all. The prepared oleogels are found quite promising frying medium in this study. Further studies with other types of oleogels in extended period frying of various foods are suggested.Practical applications: The development of innovative frying techniques to produce healthier products with lower fat and calorie values are still a remarkable research area. Oleogelation is an emerging strategy used for solid‐like oil designing and based on the formation of 3D networks by the addition of organogelators. Oleogelation is accepted as a healthy strategy to structure liquid oils into solid consistency, and oleogels have great edible applications in processed foods, and can be used as a frying medium. This work can guide the use of sunflower oil–beeswax oleogels as a frying medium and allow the development of more healthy fried snacks.

Electronic Doping and Enhancement of n‐Channel Polycrystalline OFET Performance through Gate Oxide Modifications with Aminosilanes

AbstractSelf‐assembled monolayers (SAMs) are widely employed in organic field‐effect transistors to modify the surface energy, surface roughness, film growth kinetics, and electrical surface potential of the gate oxide to control the device's operating voltage. In this study, amino‐functionalized SAM molecules are compared to pure alkylsilane SAMS in terms of their impact on the electrical properties of organic field‐effect transistors, using the n‐type polycrystalline small molecule semiconductor material N,N′‐dioctyl‐3,4,9,10‐perylenedicarboximide (PTCDI‐C8). In order to understand the electronic impact of the amino groups, the effect of both the number of amino‐containing functional groups and the SAM molecular length are systematically studied. Though amino‐functionalized SAM materials have been studied previously, this study is, for the first time, able to shed light on the nature of the doping effect that occurs when the gate oxide is treated with polar aminosilane materials. By a comprehensive theoretical study of the interface on the molecular level, it is shown that the observed shift in the threshold voltage is caused by free charges, which are attracted to the PTCDI‐C8 and are stabilized there by protonated aminosilanes. This attraction and the voltage shift can be systematically tuned by varying the length of the neutral terminal chain of the aminosilane.

Determination of the spherical part of the couple-stress in a polar fibre-reinforced elastic plate subjected to pure bending

This communication provides initial information and understanding of the manner in which a newly developed theoretical mechanism (Soldatos in Int J Solids Struct 202:217–225, 2020) is applied in specific boundary value problems met in polar linear elasticity of fibrous composites and thus enables the determination of the spherical part of the couple-stress tensor. In this context, it tests the applicability of the implied mechanism/method in the case that a rectangular plate reinforced by a single family of unidirectional fibres is subjected to pure bending. The problem solution is obtained for either non-polar or polar material behaviour, where fibres are considered perfectly flexible or resistant in bending, respectively, and provides clear evidence of the correctness of the principal argument that underpins the proposed method. Namely, that the general rotation field of the plate deformation differs from the fibre rotation field. That newly discovered method enables an extra energy term that emerges in the strain energy function of the fibrous composite plate to relate with the spherical part of the couple-stress tensor outside conventional equilibrium conventions. It thus leads to the determination of the spherical part of the couple-stress and its distribution throughout the plate body in a complete and comprehensive manner.

Decoration of carbon nanofibers with bimetal sulfides as interlayer for high performance lithium-sulfur battery

In order to obtain high-performance lithium-sulfur (Li-S) batteries, the rapid capacity loss caused by the notorious polysulfide shuttle effect is an urgent challenge to be solved. It is widely reported that polysulfides are trapped in electrolytes due to the strong chemisorption of polar materials in Li-S batteries. Here, a free-standing NiCo2S4 nanoparticles decorated carbon nanofibers (NiCo2S4-CNFs) interlayer is prepared via electrospinning and simple hydrothermal method for the application in Li-S batteries. Three-dimensional carbon fibers (CNFs) skeleton builds a highly conductive carbon network, which provides a large quantities of transmission paths for electrons and ions. Uniformly distributed NiCo2S4 nanoparticles act as an absorbent of the long-chain lithium polysulfides (LiPSs) and a catalyst to accelerate the conversion of sulfur species. Meticulous designed NiCo2S4-CNFs interlayer significantly improves the capacity retention rate and cycle stability of Li-S batteries. It supplies an initial specific capacity of 1421 mAh g−1 at 0.1 C, and its capacity remains at 918 mAh g−1 after 200 cycles at 0.2 C. Even at a high current density of 1 C, it still possesses a reversible specific capacity of 515 mAh g−1 after 500 cycles and extremely low capacity decay of 0.06% per cycle. More importantly, the NiCo2S4-CNFs interlayer still delivers excellent electrochemical performance with a higher sulfur loading of 4.5 mg cm−2, which verifies its huge commercial application potential.