Sulfur Cathode Research Articles

Hyphae‐mediated bioassembly of carbon fibers derivatives for advanced battery energy storage

AbstractIngenious design and fabrication of advanced carbon‐based sulfur cathodes are extremely important to the development of high‐energy lithium‐sulfur batteries, which hold promise as the next‐generation power source. Herein, for the first time, we report a novel versatile hyphae‐mediated biological assembly technology to achieve scale production of hyphae carbon fibers (HCFs) derivatives, in which different components including carbon, metal compounds, and semiconductors can be homogeneously assembled with HCFs to form composite networks. The mechanism of biological adsorption assembly is also proposed. As a representative, reduced graphene oxides (rGOs) decorated with hollow carbon spheres (HCSs) successfully co‐assemble with HCFs to form HCSs@rGOs/HCFs hosts for sulfur cathodes. In this unique architecture, not only large accommodation space for sulfur but also restrained volume expansion and fast charge transport paths are realized. Meanwhile, multiscale physical barriers plus chemisorption sites are simultaneously established to anchor soluble lithium polysulfides. Accordingly, the designed HCSs@rGOs/HCFs‐S cathodes deliver a high capacity (1189 mA h g−1 at 0.1 C) and good high‐rate capability (686 mA h g−1 at 5 C). Our work provides a new approach for the preparation of high‐performance carbon‐based electrodes for energy storage devices.

Improving Rate Performance of Encapsulating Lithium-Polysulfide Electrolytes for Practical Lithium-Sulfur Batteries.

The cycle life of high-energy-density lithium-sulfur (Li-S) batteries is severely plagued by the incessant parasitic reactions between Li metal anodes and reactive Li polysulfides (LiPSs). Encapsulating Li-polysulfide electrolyte (EPSE) emerges as an effective electrolyte design to mitigate the parasitic reactions kinetically. Nevertheless, the rate performance of Li-S batteries with EPSE is synchronously suppressed. Herein, the sacrifice in rate performance by EPSE is circumvented while mitigating parasitic reactions by employing hexyl methyl ether (HME) as a co-solvent. The specific capacity of Li-S batteries with HME-based EPSE is nearly not decreased at 0.1 C compared with conventional ether electrolytes. With an ultrathin Li metal anode (50 μm) and a high-areal-loading sulfur cathode (4.4 mgS cm-2 ), a longer cycle life of 113 cycles was achieved in HME-based EPSE compared with that of 65 cycles in conventional ether electrolytes at 0.1 C. Furthermore, both high energy density of 387 Wh kg-1 and stable cycle life of 27 cycles were achieved in a Li-S pouch cell (2.7 Ah). This work inspires the feasibility of regulating the solvation structure of LiPSs in EPSE for Li-S batteries with balanced performance.

Improving Rate Performance of Encapsulating Lithium‐Polysulfide Electrolytes for Practical Lithium−Sulfur Batteries

AbstractThe cycle life of high‐energy‐density lithium−sulfur (Li−S) batteries is severely plagued by the incessant parasitic reactions between Li metal anodes and reactive Li polysulfides (LiPSs). Encapsulating Li‐polysulfide electrolyte (EPSE) emerges as an effective electrolyte design to mitigate the parasitic reactions kinetically. Nevertheless, the rate performance of Li−S batteries with EPSE is synchronously suppressed. Herein, the sacrifice in rate performance by EPSE is circumvented while mitigating parasitic reactions by employing hexyl methyl ether (HME) as a co‐solvent. The specific capacity of Li−S batteries with HME‐based EPSE is nearly not decreased at 0.1 C compared with conventional ether electrolytes. With an ultrathin Li metal anode (50 μm) and a high‐areal‐loading sulfur cathode (4.4 mgS cm−2), a longer cycle life of 113 cycles was achieved in HME‐based EPSE compared with that of 65 cycles in conventional ether electrolytes at 0.1 C. Furthermore, both high energy density of 387 Wh kg−1 and stable cycle life of 27 cycles were achieved in a Li−S pouch cell (2.7 Ah). This work inspires the feasibility of regulating the solvation structure of LiPSs in EPSE for Li−S batteries with balanced performance.

Enhancing lithium-sulfur battery performance with biomass-derived graphene-like porous carbon and NiO nanoparticles composites

Despite the promising specific discharge capacity and energy density, lithium-sulfur batteries (LSBs) encounter challenges related to the lithium polysulfides (LiPSs) shuttle effect and volume expansion during extended cycling. A pivotal aspect of this research lies in the strategic synthesis of a hybrid of non-polar and polar compounds, creating an effective host and separator modifier tailored for LSBs for improvement of their electrochemical characteristics. Precisely, high-specific surface area graphene-like porous carbon (GPC) was successfully synthesized from inexpensive and abundant rice husk (RH) waste via step-by-step carbonization and thermo-chemical activation, and subsequently used as a porous matrix for sulfur cathode preparation using the melt-diffusion technique. Furthermore, composites based on GPC decorated with NiO nanoparticles were synthesized with varying GPC to Ni(NO3)2 ratios and utilized as an efficient separator modifier. The obtained results revealed that the cell consisting of GPC@S cathode and GPC-NiO-20 modified separator exhibited accelerated LiPSs redox reactions and suppressed the shuttle effect. In particular, the GPC@S/GPC-NiO-20 cell demonstrated excellent initial discharge capacity (1519 mAh g−1 at 0.2 C), promising long-term cycling performance (capacity decay of 0.091 % per cycle over 400 cycles at 1 C), and remarkable rate performance (568 mAh g−1 at 2 C).

Self-Assembly of Ultrathin, Ultrastrong Layered Membranes by Protic Solvent Penetration.

Flexible membranes with ultrathin thickness and excellent mechanical properties have shown great potential for broad uses in solid polymer electrolytes (SPEs), on-skin electronics, etc. However, an ultrathin membrane (<5 μm) is rarely reported in the above applications due to the inherent trade-off between thickness and antifailure ability. We discover a protic solvent penetration strategy to prepare ultrathin, ultrastrong layered films through a continuous interweaving of aramid nanofibers (ANFs) with the assistance of simultaneous protonation and penetration of a protic solvent. The thickness of a pure ANF film can be controlled below 5 μm, with a tensile strength of 556.6 MPa, allowing us to produce the thinnest SPE (3.4 μm). The resultant SPEs enable Li-S batteries to cycle over a thousand times at a high rate of 1C due to the small ionic impedance conferred by the ultrathin characteristic and regulated ionic transportation. Besides, a high loading of the sulfur cathode (4 mg cm-2) with good sulfur utilization was achieved at a mild temperature (35 °C), which is difficult to realize in previously reported solid-state Li-S batteries. Through a simple laminating process at the wet state, the thicker film (tens of micrometers) obtained exhibits mechanical properties comparable to those of thin films and possesses the capability to withstand high-velocity projectile impacts, indicating that our technique features a high degree of thickness controllability. We believe that it can serve as a valuable tool to assemble nanomaterials into ultrathin, ultrastrong membranes for various applications.

Advanced Polymers in Cathodes and Electrolytes for Lithium-Sulfur Batteries: Progress and Prospects.

Lithium-sulfur (Li-S) batteries, which store energy through reversible redox reactions with multiple electron transfers, are seen as one of the promising energy storage systems of the future due to their outstanding advantages. However, the shuttle effect, volume expansion, low conductivity of sulfur cathodes, and uncontrollable dendrite phenomenon of the lithium anodes have hindered the further application of Li-S batteries. In order to solve the problems and clarify the electrochemical reaction mechanism, various types of materials, such as metal compounds and carbon materials, are used in Li-S batteries. Polymers, as a class of inexpensive, lightweight, and electrochemically stable materials, enable the construction of low-cost, high-specific capacity Li-S batteries. Moreover, polymers can be multifunctionalized by obtaining rich structures through molecular design, allowing them to be applied not only in cathodes, but also in binders and solid-state electrolytes to optimize electrochemical performance from multiple perspectives. The most widely used areas related to polymer applications in Li-S batteries, including cathodes and electrolytes, are selected for a comprehensive overview, and the relevant mechanisms of polymer action in different components are discussed. Finally, the prospects for the practical application of polymers in Li-S batteries are presented in terms of advanced characterization and mechanistic analysis.

Pitaya peel-derived carbon film through one-step carbonization as a functional interlayer for lithium sulfur battery

To address the persistent challenge of soluble lithium polysulfides (LiPSs) migration in lithium-sulfur batteries, this study introduces a functional conductive interlayer derived from a cost-effective porous carbon film, innovatively synthesized through one-step carbonization of pitaya peel waste. The porous structure and abundant oxygen-containing functional groups in the resulting film successfully restrict LiPSs diffusion and boost the redox dynamics of LiPSs. Electrochemical evaluation reveals that the sulfur cathode with the proposed interlayer outperforms a pure sulfur cathode, exhibiting superior discharge capacity and cycling stability. The research presents a simplified and economical method for interlayer fabrication, contributing to sustainable advancements in lithium-sulfur battery technology.

Accelerated Li2S conversion in sparingly-solvating electrolytes enabled with dipole-dipole interaction for wide-temperature Li-S batteries

Utilizing sparingly-solvating electrolytes (SSEs), which suppress the dissolution of lithium polysulfides (Li2S4−8, LPSs), could reduce electrolyte consumption and thus retrieve the energy density competitiveness of lithium-sulfur batteries (LSBs). However, SSEs-based LSBs suffer from sluggish kinetics and rapid capacity degradation due to the accumulation of Li2S in the cathode. The catalytic approach, which is widely used to promote the sulfur conversion in ether-based LSBs, is rarely explored in SSEs-based LSBs due to the lack of a catalyst workable in the absence of dissolved LPSs. Here, by embedding CuS nanoparticles, which have high dipole-dipole interaction with Li2S, as polar sites into the carbon matrix of the sulfur cathode, we homogenize the Li2S deposition and accelerate the conversion kinetics. As a result, the cell with S/KB@CuS cathode realized a remarkable initial discharge capacity of 1469.5 mAh g−1 (87.7% of the theoretical value) with a reduced polarization potential (0.526V). Even at a low temperature of −15°C, the cell with S/KB@CuS cathode still delivered a capacity-retention of 799.0 mAh g−1 after 100 cycles. More importantly, the universality of the as-proposed dipole-dipole-interaction strategy is demonstrated with many other SSEs and polar additives.

Constructing Resilient Cross‐Linked Network Toward Stable All‐Solid‐State Lithium‐Sulfur Batteries

AbstractLithium‐sulfur batteries utilizing sulfide solid electrolytes hold considerable potential for achieving both high energy density and enhanced safety. However, the substantial volume changes experienced by sulfur during cycling result in mechanical stress accumulation, leading to mechanical degradation and thereby degrading overall electrochemical performance. In this study, a stress‐buffer strategy is proposed to address this challenge by engineering a mechanically resilient crosslinked structure for the composite sulfur cathode. This structure is accomplished through the integration of a highly flexible thermoplastic elastomer (ethylene vinyl acetate, EVA), which enables stress release during sulfur volume variations by the repeated stretching and shrinking of EVA, thereby maintaining stable ionic/electronic diffusion channels within the electrode. By virtue of the mechanically stable architecture, the stress evolution experienced by the entire sulfur electrode is substantially reduced, witnessing a remarkable decrease of ≈33.7%. Consequently, the S‐EVA composite cathode demonstrates exceptional electrochemical performance, especially cycling stability. Notably, the S‐EVA composite cathode, with a high loading of 7.5 mg cm−2, exhibits stable cycling performance close to 3.0 mAh cm−2 within 50 cycles. This work not only offers novel insights into mitigating the mechanical stress within the electrode but also paves the way for developing durable high‐performance all‐solid‐state batteries.

Ethylene Glycol‐Containing Acrylic Polyphosphazene Based Cathode Materials via Inverse Vulcanization of Sulfur for Li−S Batteries

AbstractThe cell performance of Li−S batteries can be improved by establishing compatibility with the electrolyte of cathode and enhancing lithium‐ion diffusion (ionic conductivity) or electrical conductivity. In this work, we introduce cathode material based on ethylene glycol‐containing acrylic polyphosphazene. Poly[(2acrylamidoethoxy)‐random‐(methoxyethoxyethoxy)] phosphazenes were synthesized by macromolecular substitution of poly(dichloro)phosphazene with 2‐acrylamidoethanol and diethylene glycol methyl ether in two different ratios (25 and 50 mol% of ethylene glycol methyl ether), abbreviated as MP‐25EG and MP‐50EG, where ethylene glycol chains enhance the electrolyte compatibility and ion transport of the sulfur cathode material. Then, poly[S‐random‐(2acrylamidoethoxy)‐random‐(methoxyethoxyethoxy)] phosphazene polymers, designated as MP‐25EG‐xS or MP‐50EG‐xS (x=50 and 80 wt.% of sulfur) were prepared by inverse vulcanization of polymer with two feed sulfur ratios. Structural characterizations of the polymers were carried out using appropriate standard spectroscopic methods such as 1H and 31P NMR, FT‐IR, DSC and TGA as well as XPS. The electrochemical performance of MP‐25EG‐50S, MP‐25EG‐80S and MP‐50EG‐50S, MP‐50EG‐80S were evaluated and the effect of ethylene glycol was investigated by comparing cell performances. MP‐50EG‐50S demonstrated its promising applicability in Li–S batteries by exhibiting much better electrochemical respond with a discharge capacity of 745 mAh/g at C/5 current density over 100 cycles.

Influence of carbon structure/porosity on the electrochemical performance in Li–sulfur batteries

The porous structure of three different, commercially available porous carbonaceous materials is investigated by the αS-plot method and by the t-plot method. Subsequently, the electrochemical properties of sulfur-free porous carbon electrodes from inspected materials are studied by cyclic voltammetry. The comparison of double-layer capacitances with the corresponding adsorption isotherms of N2 reveals the role of micropores during the capacitive charging of carbons by Li+. The studied carbons are added to the sulfur cathodes and evaluated. The cyclic voltammograms show no contribution of micropores in the carbon structure to the electrochemical processes taking place in the lithium–sulfur coin cell. The highest specific capacity of 816 mAh/g is observed for material with the lowest content of micropores in the structure (14%). The partially mesoporous and partially microporous (65%) sample and the predominantly microporous one (87%), show specific capacities of 664 mAh/g and 560 mAh/g, respectively. The galvanostatic cycling of lithium–sulfur coin cells with carbonaceous additives reveals that the mesopores and macropores in the carbon structure increase the specific charge capacity of the lithium–sulfur batteries and that the micropores improve the cycling stability of these batteries.Graphical abstract

Hit two birds with one stone: A bi-functional selenium-substituted organosulfur polymer additive for high-performance lithium-sulfur batteries

Sluggish reaction kinetics of sulfur cathode and high reactivity of lithium anode hinder the commercialization of Li-S batteries. Employing the electrolyte additive to regulate the states of active material is a facile and effective way to solve the above issues. Herein, the bifunctional selenium substituted lithium polythioctic acid (PTA-Se) was prepared as an additive of electrolyte via in-situ polymerization and substitution method. Such additives can promote the conversion of polysulfides and facilitate the homogenization of Li-ion flux. The active selenium sites provide a kinetically favorable pathway for polysulfide conversion. The introduction of additives also facilitates the formation of elastic and uniform solid electrolyte phase interface (SEI) film on the surface of lithium anode. As results, Li-S batteries assembled with PTA-Se additive demonstrates a high initial capacity of 1319 mAh g−1 at 0.2C with 1000 mAh g−1 remaining after 150 cycles, corresponding to a 0.16 % capacity decay per cycle. At a high rate of 5C, the cell still achieves a reversible capacity of 517 mAh g−1. This work opens a new avenue for designing effective electrolyte additive and achieving high-performance Li-S batteries.

Phosphor-Doped Carbon Network Electrocatalyst Enables Accelerated Redox Kinetics of Polysulfides for Sodium-Sulfur Batteries.

Lithium-ion batteries, which have dominated large-scale energy storage for the past three decades, face limitations in energy density and cost. Sulfur, with its impressive capacity of 1675 mAh g-1 and high theoretical energy density of 1274 Wh kg-1, stands out as a promising cathode material, leading to a growing focus on sodium-sulfur (Na-S) batteries as an alternative to address lithium resource scarcity. Nevertheless, the development is restrained by poor conductivity, volume expansion of the sulfur cathode, and the shuttle effect of sodium polysulfides (Na2Sn) in the electrolytes. In this study, a facile method is designed to fabricate phosphor-doped carbon (phos-C), which is then used as a sulfur matrix. This micromesoporous phos-C network enhances sulfur utilization, increases overall cathode conductivity, and effectively mitigates the shuttling of Na2Sn. During the discharge process, phos-C can absorb soluble Na2Sn and increase the conductivity of sulfur, while serving as a reservoir for electrolyte and Na2Sn, thereby preventing their infiltration into the anode and reducing the loss of sodium. As a result, the well-designed sulfur-loaded phos-C (S/phos-C) cathode, employed in the Na-S battery, demonstrates a capacity of 1034 mAh g-1 at 0.1 C (1 C = 1675 mA g-1) and an excellent rate capability of 339 mAh g-1 at 10 C, coupled with a prolonged cycling life up to 2000 cycles at 1 C, exhibiting an ultralow capacity decay rate of 0.013% per cycle. Overall, this study introduces an efficient method for creating long-lasting Na-S batteries.

Investigation of the Chemisorption-Catalysis Behavior of Sulfur Species on the Electrocatalysts Designed by Co-regulation Strategy of Anions and Cations.

Li-S batteries possess high energy density and have been one of the most promising energy storage systems. For sulfur cathodes, the electrochemical performance is still seriously hindered by the polysulfide shuttling and sluggish conversion kinetics. It has been demonstrated to be one effective strategy to address the above issues via designing electrocatalysts with robust affinity and catalytic capacity towards polysulfides. However, it is still a great challenge to rapidly and economically discover high-performance electrocatalysts. Herein, using density functional theory calculation, we studied the chemisorption-catalysis behavior of sulfur species on a series of electrocatalysts (MCo2 X4 , M=Co, Zn, Cu, Ni, Fe, and Mn, X=O, S, and Se) to assess the effect of the anions and cations co-regulation on their electronic structure, chemisorption behavior, and catalytic property. FeCo2 Se4 and CuCo2 Se4 combined appropriate chemisorption with superior electronic conductivity and sulfur reduction catalytic capacity have been predicted as novel electrocatalysts for high-performance Li-S batteries. This study gives theoretical guidance for rapid discovery of high-efficient electrocatalyst to boost the electrochemical performance of sulfur cathodes.

Anion-Regulated Sulfur Conversion in High-Content Carbon Layer Confined Sulfur Cathode Maximizes Voltage and Rate Capability of K-S Batteries.

Potassium-sulfur (K-S) batteries have attracted attention in large-scale energy storage systems. Small-molecule/covalent sulfur (SMCS) can help to avoid the shuttle effect of polysulfide ions via solid-solid sulfur conversion. However, the content of SMCS is relatively low (≤40%), and solid-solid reactions cause sluggish kinetics and low discharge potentials. Herein, SMCS is confined in turbo carbon layers with a content of ≈74.1wt% via a C/S co-deposition process. In the K-S battery assembled by using as-fabricated SMCS@C as cathode and KFSI-EC/DEC as an electrolyte, anion-regulated two-plateau solid-state S conversion chemistry and a novel high discharge potential plateau at 2.5-2.0V with a remarkable reversible capacity of 384mAhg-1 at 3Ag-1 after 1000 cycles are found. The SMCS@C||K full cell showed energy and power density of 72.8Whkg-1 and 873.2Wkg-1, respectively, at 3Ag-1. Mechanismstudiesrevealthat theenlarged carbon layer space enables the diffusion of K+-FSI-ion pairs, and the coulombic attraction between them accelerates their diffusion in SMCS@C. In addition, FSI-regulates sulfur conversion in situ inside thecarbon layers along a two-plateau solid-state reaction pathway, which lowers the free energy and weakens the S─S bond of intermediates, leading to faster and more efficient S conversion.

Application of MXene-Based Materials for Cathode in Lithium-Sulfur Batteries.

The lithium-sulfur (Li-S) batteries have a high theoretical specific capacity of 1675 mAh ⋅ g-1 and have become the most promising high-energy storage system for the next generation batteries technology. However, their applications are hindered by insulated feature and volume expansion of sulfur, as well as the "shuttle effect" of polysulfides. MXenes own metallic conductivity and strong ability of polysulfides adsorption. Besides, their unique two-dimensional (2D) structure, large specific surface area, abundant functional groups, and adjustability are beneficial to overcome the drawbacks of the sulfur cathode. In this review, different mainstream preparation methods and excellent properties of MXenes are summarized. Significant achievements and recent progress of MXene-based cathodes and interlayers applied to Li-S cathodes are concluded later. Finally, the challenges, possible solutions and potential applications of MXenes for Li-S batteries are also presented.

High‐Content Carbon Layer Confined Small‐Molecule/Covalent Sulfur Cathode Enables Long‐Life Calcium–Sulfur Batteries in Hybrid‐Ion Electrolyte

AbstractCalcium‐sulfur (Ca‐S) battery is a promising candidate for large‐scale energy storage system. However, the development of long‐life room‐temperature Ca–S batteries is hindered by the lack of effective sulfur cathode and the incompatibility between electrodes and electrolytes, leading to irreversible sulfur conversion, inefficient calcium plating/stripping and improper cathode/anode‐electrolyte interfaces (CEI/SEI). Herein, a turbo carbon layer confined small‐molecule/covalent sulfur cathode (S@C NS) with a record‐high content of 65.7% and enlarged carbon layer space is prepared via a C/S co‐deposition process. By using such a cathode and optimizing interfacial electrochemistry in LiPF6/Ca(BF4)2‐based hybrid electrolyte, a record‐breaking long‐life room‐temperature Ca‐S battery is reported. The capacity reaches 824.6 mAh g−1 at 100 mA g−1 with a retention of 47.9% after 145 cycles, and 462.1 mAh g−1 at even 500 mA g−1. Mechanism studies demonstrated that a Li/Ca‐based hybrid CEI with porous microstructure is found to facilitate the transfer kinetics of Ca2+ across the CEI; Turbo carbon layers with large inter‐layer space and their strong confinement on small‐molecule sulfur enabled reversible solid‐state sulfur conversion in situ inside the cathode; An effective Li/Ca‐based hybrid SEI formed on anode, allowing reversible Ca plating/stripping with low deposition potential and small overpotential.

High-Entropy MXene as Bifunctional Mediator toward Advanced Li-S Full Batteries.

The development of high-energy-density Li-S batteries (LSBs) is still hindered by the disturbing polysulfide shuttle effect. Herein, with clever combination between "high entropy" and MXene, an HE-MXene doped graphene composite containing multiple element quasi-atoms as bifunctional mediator for separator modification (HE-MXene/G@PP) in LSBs is proposed. The HE-MXene/G@PP offers high electrical conductivity for fast lithium polysulfide (LiPS) redox conversion kinetics, abundant metal active sites for efficient chemisorption with LiPSs, and strong lipophilic characteristics for uniform Li+ deposition on lithium metal surface. As demonstrated by DFT theoretical calculations, in situ Raman, and DRT results successively, HE-MXene/G@PP efficiently captures LiPSs through synergistic modulation of the cocktail effect and accelerates the LiPSs redox reaction, and the lattice distortion effect effectively induces the homogeneous deposition of dendritic-free lithium. Therefore, this work achieves excellent long-term cycling performance with a decay rate of 0.026%/0.031% per cycle after 1200 cycles at 1 C/2 C. The Li||Li symmetric cell still maintains a stable overpotential after 6000 h under 40 mA cm-2/40 mAh cm-2. Furthermore, it delivers favorable cycling stability under 7.8 mg cm-2 and a low E/S ratio of 5.6 μL mg-1. This strategy provides a rational approach to resolve the sulfur cathode and lithium anode problems simultaneously.

Polymeric ionic liquid as binder: A promising strategy for enhancing Li[sbnd]S battery performance

The development of the most promising next-generation LiS batteries with an improved cyclability is one of the greatest challenges nowadays. In this sense, here, a novel imidazolium-based polymeric ionic liquid (PVI10Cl) was successfully synthesized and integrated into a high-performing sulfur cathode. The lithium polysulfide trapping ability of PVI10Cl was confirmed, which helps to accelerate conversion kinetics. This synergetic effect leads to enhanced C-rate response, improving the discharge capacities and reducing the overpotentials even at 1C in comparison with conventional PVdF binder. These features also allow cells to be operated for 100 cycles with excellent capacity retention. All in one, while conventional binders are viewed only as a “glue” to hold the active material together, it has been shown that PVI10Cl binder has additional functions and plays an active role during LiS battery operation.

Interfacial polymerization achieved integration of pore size adjustment, electrostatic repulsion and physical adsorption into one to inhibit polysulfide shuttle for enhanced lithium–sulfur battery

The application of lithium-sulfur battery is seriously hindered by the shuttle of dissolved polysulfide between sulfur cathode and lithium anode, by which is not selectively inhibited by the conventional separator. Developing functional separator is considered as a preferred solution for this issue, but it is always challenged by the tedious preparation process. Herein, interfacial polymerization (IP) is employed to modify the surface property of ZrO2 nanoparticles embedded polyetherimide (PZ) based separator, and the integration of pore size adjustment, electrostatic repulsion and physical adsorption into one is facilely achieved to effectively inhibit the polysulfide shuttle. Consequently, the optimized PZ separator presents a high lithium-ion transference number (0.55) and diffusion coefficient (2.16 × 10−8 cm s−1). Compared with the pristine one, the electrochemical performance of the assembled lithium-sulfur battery is obviously enhanced, and an initial discharge specific capacity of 1242 mAh g−1 and a capacity retention of 68 % after 200 cycles are obtained.