A polyimine aerogel separator with electron cloud design to boost Li-ion transport for stable Li metal batteries.

The separator with high Young's modulus can avoid the danger of large-sized dendrites, but regulating the chemical behavior of lithium (Li) at the separator/anode interface can effectively eliminate the dendrite issue. Herein, a polyimine aerogel (PIA) with accurate nitrogen (N) functional design is used as the functional separator in Li metal batteries to promote uniform Li nucleation and suppress the dendrite growth. Specifically, the imine (N1) and protonated tertiary amine (N2) sites in the molecular structure of the PIA are significantly different in electron cloud density (ECD) distribution. The N1 site with higher ECD and the N2 site with lower ECD tend to attract and repulse Li+ through electrostatic interactions, respectively. This synergy effect of the PIA separator accelerates the interfacial Li+ diffusion on the Li anode to sustain a uniform two-dimensional Li nucleation behavior. Meanwhile, the well-defined nanochannels of the PIA separator show high affinity to electrolyte and bring uniform Li+ flux for Li plating/stripping. Consequently, the dendrites are effectively suppressed by the PIA separator in routine carbonate electrolyte, and the Li metal batteries with the PIA separator exhibit high Coulombic efficiency and stable high-rate cycling. These findings demonstrate that the ingenious marriage of special chemical structure designs and hierarchical pores can enable the separator to affect the interfacial Li nucleation behavior.

A crystalline carbon nitride-based separator for high-performance lithium metal batteries.

Lithium metal anodes with ultrahigh theoretical capacities are very attractive for assembling high-performance batteries. However, uncontrolled Li dendrite growth strongly retards their practical applications. Different from conventional separator modification strategies that are always focused on functional group tuning or mechanical barrier construction, herein, we propose a crystallinity engineering-related tactic by using the highly crystalline carbon nitride as the separator interlayer to suppress dendrite growth. Interestingly, the presence of Cl- intercalation and high-content pyrrolic-N from molten salt treatment along with highly crystalline structure enhanced the interactions of carbon nitride with Li+ and homogenized lithium flux for uniform deposition, as supported by both experimental and theoretical evidences. The Li-Li cell with the modified separator therefore delivered ultrahigh stability even after 3,000 h with dendrite-free cycled electrodes. Meanwhile, the assembled Li-LiFePO4 full-cell also presented high-capacity retention. This work opens up opportunities for design of functional separators through crystallinity engineering and broadens the use of C3N4 for advanced batteries.

Active Dendrite Suppression by Ferroelectric Membrane Separators in Rechargeable Batteries.

Anodic dendrite formation is a critical issue in rechargeable batteries and often leads to poor cycling stability and quick capacity loss. Prevailing strategies for dendrite suppression aim at slowing down the growth rate kinetically but still leaving possibilities for dendrite evolution over time. Herein, we report a complete dendrite elimination strategy using a mesoporous ferroelectric polymer membrane as the battery separator. The dendrite suppression is realized by spontaneously reversing the surface energetics for metal ion reduction at the protrusion front, where a positive piezoelectric polarization is generated and superimposed as the protrusion compresses the separator. This effect is demonstrated first in a Zn electroplating process, and further in Zn-Zn symmetric cells and Zn-NaV3O8·1.5H2O full cells, where the dendritic Zn anode surfaces are completely turned into featureless flat surfaces. Consequently, a substantially longer charging/discharging cycle is achieved. This study provides a promising pathway toward high-performance dendrite-free rechargeable batteries.

Precise Design of a 0.8 nm Pore Size in a Separator Interfacial Layer Inspired by a Sieving Effect toward Inhibiting Polysulfide Shuttling and Promoting Li+ Diffusion.

The incomplete blocking of small-sized polysulfides by pore size and the effect on Li+ transport are generally neglected when the size-sieving effect is employed to suppress the shuttling of polysulfides. Herein, ion-selective modified layers with pore sizes equal to, greater than, and less than 0.8 nm, respectively, on the polypropylene separator are fabricated to obtain the preferable pore size for separation of polysulfides and Li+. As a result, the modified layer with a pore size of 0.8 nm can efficiently inhibit the shuttling of polysulfides and simultaneously boost the diffusion of Li+ under the double effect of the size advantage and electrostatic shielding. Consequently, the battery using a separator with a modified layer having a pore size of 0.8 nm possesses a lower capacity attenuation of 0.047% after 1000 cycles at 2.0 C. This work serves as a vital guide for suppressing polysulfide shuttle using ion-selective sieving effects for lithium-sulfur batteries.

Separators Modified with Ultrathin Montmorillonite/Polymer Nanocoatings Achieve Dendrite-Free Lithium Deposition at High Current Densities.

Fatal dendritic growth in lithium metal batteries is closely related to the composition and thickness of the modified separator. Herein, an ultrathin nanocoating composed of monolayer montmorillonite (MMT), poly(vinyl alcohol) (PVA) on a polypropylene separator is prepared. The MMT was exfoliated into monolayers (only 0.96 nm) by intercalating PVA under ultrasound, followed by cross-linking with glutaraldehyde. The thickness of the nanocoating on the polypropylene separator, as determined using the pull-up method, is only 200-500 nm with excellent properties. As a result, the lithium-symmetric battery composed of it has a low overpotential (only 40 mV) and a long lifespan of more than 7900 h at high current density, because ion transport is unimpeded and Li+ flows uniformly through the ordered ion channels between the MMT layers. Additionally, the separator exhibited excellent cycling stability in Li-S batteries. This study offers a new idea for fabricating ultrathin clay/polymer modified separators for metal anode stable cycling at high current densities.

One-Step Wet-Spinning of High-Energy Density Coaxial Fibrous Supercapacitors Based on In Situ Carbon-Modified Nitrogen-Doped MXene Nanosheets.

Fibrous supercapacitors (SCs) are emerging promising power sources for flexible/wearable electronics and have attracted an extensive amount of attention from researchers. However, the low energy density has always hindered their further development. Here, a coaxial fibrous SC (CFSC) was fabricated by one-step wet-spinning combined with an electrodeposition strategy. Benefiting from the large surface area and abundant pore structure of carbon-modified nitrogen-doped MXene nanosheets (NS), as well as the high conductivity of silver (Ag) NS, the electrolyte ion/electron transport paths are significantly improved. Furthermore, the distributed GO in the P(VDF-HFP) separator could form a high-speed continuous ion transport channel, thus enhancing the ionic conductivity. At a power density of 40-200 µW cm-2, the CFSC shows a high energy density of 0.7-3.39 µWh cm-2. The as-prepared CFSC also maintains an excellent capacitance retention rate of 90.3% even after 15 000 charge-discharge cycles. This work provides a general strategy for manufacturing high-performance, flexible, and wearable SCs.

Electrolyte Superwetting and Electrode Friendly of Porous Membrane for Better Cycling Stability of Lithium Metal Batteries.

Porous polymer membranes as separator plays important roles in separating cathode and anode, storing electrolytes, and transporting ions in energy storage devices. Here, an effective strategy is reported to prepare an electrolyte superwetting membrane, which shows good Li+ transport rate and uniformity, as well as electrode-friendly properties to afford the reduction and oxidation of electrodes. It thereby improves the cycle stability and safety of Li metal batteries. With the arrayed capillaries technique, a thin layer of polyvinylidene fluoride (PVDF) and polyacrylonitrile (PAN) composite is uniformly coated on the surface and pores of polypropylene (PP) membrane with a total thickness of 30 µm. After treating it with n-butyllithium and LiNO3 in turn, a chemically inert membrane with efficient and uniform ion transport is prepared, and the cycle stability of Li||Li symmetric cells is up to 1500 h, 4 times higher than that of PP membrane. Moreover, the Li||LiFePO4 with as-prepared membranes achieve a higher capacity retention rate of 92% after 190 cycles at a current density of 3.6 mA cm-2 and a capacity of 3.6 mAh cm-2, and the Li||NCM721 batteries achieve a capacity retention rate of 71% after 600 cycles at a current density of 1.8 mA cm-2.

Establishing an Ion-Sieving Separator by Depositing Oxygen-Deficient SiOx Layer for Stabilized Zinc Metal Anode.

Stable plating/stripping of Zn metal anode remains a great challenge owing to uncontrollable dendrite growth and side reactions. Ion-sieving separators is a unique and promising solution, that possess Zn2+ permeability and promote Zn2+ transport, can effectively alleviate the abovementioned problems. Ion-sieving on glass fiber separator by deposition of oxygen-deficient SiOx layer via active screen plasma technology is achieved. While having chemical composition similar to the glass fiber, the SiOx nanoparticles contain oxygen-rich vacancies that promoted dissociation of the adsorbed water and generation of the hydroxyl groups. The negatively-charged hydroxylated SiOx layer can repel SO4 2- and attract Zn2+, which can alleviate the side reactions. The strong interplay between hydroxyl groups and Zn2+ can boost Zn affinity and yield fast Zn2+ transport. Consequently, the SiOx-deposited GF separator enabled dendrite-free Zn deposition morphology, which displays lower overpotential of 18 mV and longer cycling life over 2000 h for Zn symmetric cell. Such a separator can also be easily scaled up to prepare the high-performance large-area (4 × 6 cm2) pouch Zn-based devices, showing remarkable flexibility and practicality.

Inorganic Oxide-Based "Hydrophobic-Hydrophilic-Hydrophobic" Separators Systems for Long-Life Zinc-Ion Batteries.

Hydrogen reduction reaction (HER) and corrosion limit the long-life cycle of zinc-ion batteries. However, hydrophilic separators are unable to prevent direct contact between water and electrodes, and hydrophobic separators have difficulty in transporting electrolytes. In this work, an inorganic oxide-based "hydrophobic-hydrophilic-hydrophobic" self-assembled separator system is proposed. The hydrophobic layer consists of a porous structure, which can isolate a large amount of free water to avoid HER and corrosion reactions, and can transport electrolyte by binding water. The middle hydrophilic layer acts as a storage layer consisting of the GF separator, storing large amounts of electrolyte for proper circulation. By using this structure separator, Zn||Zn symmetric cell achieve 2200 h stable cycle life at 5 mA cm-2 and 1mAh cm-2 and still shows a long life of 1800 h at 10 mA cm-2 and 1mAh cm-2. The assembled Zn||VO2 full cell displays high specific capacity and excellent long-term durability of 60.4% capacity retention after 1000 cycles at 2C. The assembled Zn||VO2 pouch full cell displays high specific capacity of 172.5mAh g-1 after 40 cycles at 0.5C. Changing the inorganic oxide materials, the hydrophobic-hydrophilic-hydrophobic structure of the separators still has excellent performance. This work provides a new idea for the engineering of water-based battery separators.

Nanoporous Aramid Nanofiber Separators with High Modulus and Thermal Stability for Safe Lithium-Ion Batteries.

Developing high-safety separators is a promising strategy to prevent thermal runaway in lithium-ion batteries (LIBs), which stems from the low melting temperatures and inadequate modulus of commercial polyolefin separators. However, achieving high modulus and thermal stability, along with uniform nanopores in these separators, poses significant challenges. Herein, the study presents ultrathin nanoporous aramid nanofiber (ANF) separators with high modulus and excellent thermal stability, enhancing the safety of LIBs. These separators are produced using a microfluidic-based continuous printing strategy, where the flow thickness can be meticulously controlled at the micrometer scale. This method allows for the continuous fabrication of nanoporous ANF separators with thicknesses ranging from 1.6 ± 0.1 µm to 2.7 ± 0.1 µm. Thanks to the double-side solvent diffusion, the separators exhibit controllably uniform pore sizes with a narrow distribution, spanning from 40 ± 5 nm to 105 ± 9 nm, and a high modulus of 3.3 ± 0.5 GPa. These nanoporous ANF separators effectively inhibit lithium dendrite formation, resulting in a high-capacity retention rate for the LIBs (80% after 240 cycles). Most notably, their robust structural and mechanical stability at elevated temperatures significantly enhances LIB safety under transient thermal abuse conditions, thus addressing critical safety concerns associated with LIBs.

Dual-Modified Electrospun Fiber Membrane as Separator with Excellent Safety Performance and High Operating Temperature for Lithium-Ion Batteries.

Polyacrylonitrile/Boric acid/Melamine/the delaminated BN nanosheets electrospun fiber membrane (PB3N1BN) with excellent mechanical property, high thermal stability, superior flame-retardant performance, and good wettability are fabricated by electrospinning PAN/DMF/H3BO3/C3H6N6/ the delaminated BN nanosheets (BNNSs) homogeneous viscous suspension and followed by a heating treatment. BNNSs are obtained by delaminating the bulk h-BN in isopropyl alcohol (IPA) with an assistance of Polyvinylpyrrolidone (PVP). Benefiting from the cross-linked pore structure and high-temperature stability of BNNSs, PB3N1BN electrospun fiber membrane delivers high thermal dimensional stability (almost no size contraction at 200 °C), excellent mechanical property (19.1 MPa), good electrolyte wettability (contact angle about 0°), and excellent flame retardancy (minimum total heat release of 3.2 MJ m-2). Moreover, the assembled LiFePO4/PB3N1BN/Li asymmetrical battery using LiFePO4 as the cathode and Li as the anode has a high capacity (169 mAh g-1 at 0.5 C), exceptional rate capability (129 mAh g-1 at 5 C), the prominent cycling stability without obvious decay after 400 cycles, and a good discharge capacity of 152 mAh g-1 at a high temperature of 80 °C. This work offers a new structural design strategy toward separators with excellent mechanical performance, good wettability, and high thermal stability for lithium-ion batteries.

Built-in Electric Field Within CoSe2-FeSe2 Heterostructure for Enhanced Sulfur Reduction Reaction in Li-S Batteries.

The conversion of Li2S4 to Li2S is the most important and slowest rate-limiting step in the complex sulfur reduction reaction (SRR) for Li-S batteries, the adjustment of which can effectively inhibit the notorious "shuttle effect". Herein, a CoSe2-FeSe2 heterostructure embedded in 3D N-doped nanocage as a modified layer on commercial separator is designed (CoSe2-FeSe2@NC//PP). The CoSe2-FeSe2 heterostructure forms a built-in electric field at the two-phase interface, which leads to the optimized adsorption force on polysulfides and the accelerated reaction kinetics for Li2S4-Li2S evolution. Density functional theory (DFT) calculations and experimental results combine to show that the liquid-solid reaction (Li2S4-Li2S2/Li2S) is significantly enhanced in terms of thermodynamics and electrodynamics. Consequently, the batteries assembled with CoSe2-FeSe2@NC//PP delivered an excellent rate capability (606 mAh g-1 under 8.0 C) and a long cycling lifespan (only 0.056% at 1.0 C after 1000 cycles). In addition, the cells can provide high initial capacity of 887 mAh g-1 at sulfur loading of 5.8 mg cm-2 and 0.1 C. This work would provide valuable insights into binary metal selenide heterostructures for liquid-solid conversion in Li-S batteries.

In Situ Polymerization of Ultra-Thin and Defect-Free Polyamide Layer for Effectively Impeding the Polysulfides Shuttle.

Lithium-sulfur (Li-S) batteries present significant potential for next-generation high-energy-density devices. Nevertheless, obstacles such as the polysulfide shuttle and Li-dendrite growth severely impede their commercial production. It is still hard to eliminate gaps between individual particles on separators that serve as potential conduits for polysulfide shuttling. Herein, the synthesis of a nanoscale thickness and defect-free cross-linked polyamide (PA) layer on a polypropylene (PP) separator is presented through in situ polymerization. The PA modification layer can effectively impede the diffusion of polysulfides with a thickness of only 1.5 nm, as evidenced by the results of cyclic voltammetry (CV) and time-of-flight (TOF) testing. Therefore, the Li/Li symmetric battery assembled with the functional separator exhibits an overpotential of merely 12 mV after 1000 h of cycling under test conditions of 1 mA cm-2-1 mAh cm-2. Furthermore, the capacity degradation rate of the Li-S battery is only 0.06% per cycle over 450 cycles at 1 C, while the Li-S pouch cell retains 87.63% of its capacity after 50 cycles. This work will significantly advance the preparation and application of molecules in Li-S batteries, and it will also stimulate further research on defect-free modification of separators.

Cobalt Nitride Nanoparticles Encapsulated in N-Doped Carbon Nanotubes Modified Separator of Li-S Battery Achieving the Synergistic Effect of Restriction-Adsorption-Catalysis of Polysulfides.

Although lithium-sulfur (Li-S) batteries have broad market prospects due to their high theoretical energy density and potential cost-effectiveness, the practical applications still face serious shuttle effects of polysulfides (LiPSs) and slow redox reactions. Therefore, in this paper, cobalt nitride nanoparticles encapsulated in nitrogen-doped carbon nanotube (CoN@NCNT) are prepared as a functional layer for the separator of high-performance Li-S batteries. Carbon nanotubes with large specific surface areas not only promote the transport of ions and electrons but also weaken the migration of LiPSs and confine the dissolution of LiPSs in electrolytes. The lithiophilic heteroatom N adsorbs LiPSs by strong chemical adsorption, and the CoN particles with high catalytic activity greatly improve the kinetics of the conversion between LiPSs and Li2S2/Li2S during the charge-discharge process. Due to these advantages, the battery with CoN@NCNT modified separator has superior rate performance (initial discharge capacity of 834.7 mAh g-1 after activation at 1 C) and excellent cycle performance (capacity remains 729.7 mAh g-1 after 200 cycles at 0.2 C). This work proposes a strategy that can give the separator a strong ability to confinement-adsorption-catalysis of LiPSs in order to provide more possibilities for the development of Li-S batteries.

Mediating Triple Ions Migration Behavior via a Fluorinated Separator Interface toward Highly Reversible Aqueous Zn Batteries.

Rampant dendrite growth, electrode passivation and severe corrosion originate from the uncontrolled ions migration behavior of Zn2+ , SO4 2- , and H+ , which are largely compromising the aqueous zinc ion batteries (AZIBs) performance. Exploring the ultimate strategy to eliminate all the Zn anode issues is challenging but urgent at present. Herein, a fluorinated separator interface (PVDF@GF) is constructed simply by grafting the polyvinylidene difluoride (PVDF) on the GF surface to realize high-performance AZIBs. Experimental and theoretical studies reveal that the strong interaction between C─F bonds in the PVDF and Zn2+ ions enables evenly redistributed Zn2+ ions concentration at the electrode interface and accelerates the Zn transportation kinetics, leading to homogeneous and fast Zn deposition. Furthermore, the electronegative separator interface can spontaneously repel the SO4 2- and anchor H+ ions to alleviate the passivation and corrosion. Accordingly, the Zn|Zn symmetric cell with PVDF@GF harvests a superior cycling stability of 500 h at 10 mAh cm-2 , and the Zn|VOX full cell delivers 76.8% capacity retention after 1000 cycles at 2 A g-1 . This work offers an all-round solution and provides new insights for the design of advanced separators with ionic sieve function toward stable and reversible Zn metal anode chemistry.

ZnO@C Coated Cellulose-Based Separators Control Lithium Deposition Direction to Stable Lithium Metal Batteries.

Li metal anodes have attracted attention due to their high specific capacity and low electrochemical potential. Nevertheless, the uncontrolled growth of Li dendrites hinders the practical application of Li metal batteries. Although the various approaches have made performance improvements, safety hazards still exist since Li dendrites are still growing along the anode to the separator during the continuous plating/stripping process. Herein, a straightforward method is proposed to achieve stable Li metal batteries with directional growth control by using a functional ZnO@C/cellulose membrane as a separator. The abundant pore structure and functional groups of biomass cellulose enhance the Li-ion transport and interface compatibility. The ZnO transforms in situ to form a Li-Zn alloy layer which is uniformly coated to the separator to direct uniform ion concentration polarization and charge distribution polarization, control the growth direction of Li, significantly improve the cycling stability, and promote the reversibility of the Li plating/exfoliation process. As a result, the symmetric cell exhibits an extreme lifetime of more than 4500 h and low polarization at 3 mA cm-2 . The cycling performance of the Li||LiFePO4 full cell reaches a capacity retention of 98% after 270 cycles at a mass loading of 10 mg cm-2 .

Boosting Polysulfide Redox Kinetics by Temperature-Induced Metal-Insulator Transition Effect of Tungsten-Doped Vanadium Dioxide for High-Temperature Lithium-Sulfur Batteries.

The practical application of Li-S batteries is still severely restricted by poor cyclic performance caused by the intrinsic polysulfides shuttle effect, which is even more severe under the high-temperature condition owing to the inevitable increase of polysulfides' solubility and diffusion rate. Herein, tungsten-doped vanadium dioxide (W-VO2) micro-flowers are employed with first-order metal-insulator phase transition (MIT) property as a robust and multifunctional modification layer to hamper the shuttle effect and simultaneously improve the thermotolerance of the common separator. Tungsten doping significantly reduces the transition temperature from 68 to 35 °C of vanadium dioxide, which renders the W-VO2 easier to turn from the insulating monoclinic phase into the metallic rutile phase. The systematic experiments and theoretical analysis demonstrate that the temperature-induced in-suit MIT property endows the W-VO2 catalyst with strong chemisorption against polysulfides, low energy barrier for liquid-to-solid conversion, and outstanding diffusion kinetics of Li-ion under high temperatures. Benefiting from these advantages, the Li-S batteries with W-VO2 modified separator exhibit significantly improved rate and long-term cyclic performance under 50 °C. Remarkably, even at an elevated temperature (80 °C), they still exhibit superior electrochemical performance. This work opens a rewarding avenue to use phase-changing materials for high-temperature Li-S batteries.

Zinc Tellurium with Anionic Vacancies Anchored on Ordered Macroporous Carbon Skeleton Enabling Accelerated Polysulfide Conversion for Lithium-Sulfur Batteries.

Lithium-sulfur batteries (LSBs) showcase great promise for large-scale energy storage systems, however, their practical commercialization is seriously hindered by the sluggish redox reaction kinetics and detrimental shuttle effect of soluble polysulfides. Herein, small ZnTe1- x nanoparticles with anionic vacancies firmly anchored on 3D ordered macroporous N-doped carbon skeleton (3DOM-ZnTe1- x@NC) are elaborately constructed as a high-efficiency electrocatalyst for LSBs. The ordered macroporous carbon skeleton not only greatly increases the external surface area to expose sufficient active sites but also facilitates the electrolyte penetration. Additionally, the experimental studies combined with theoretical calculations confirm the presence of Te vacancies optimizes the electronic structure to enhance the intrinsic catalytic activity and chemical absorption. Consequently, LSBs assembled with the 3DOM-ZnTe1- x@NC modified separators exhibit high specific discharge capacity, as well as superior rate performance and good long-term cycling stability. Even under a high sulfur loading of 6.5 mg cm-2 and lean electrolyte, an impressive areal capacity of 5.28 mAh cm-2 is achieved at 0.1 C after 100 cycles. More significantly, the 3DOM-ZnTe1- x@NC based pouch cells are also fabricated to demonstrate its potential for practical applications. This work highlights that the rational combination of 3DOM architecture and vacancy engineering is important for designing advanced Li-S electrocatalysts.

Porous Organic Framework Materials (MOF, COF, and HOF) as the Multifunctional Separator for Rechargeable Lithium Metal Batteries.

The separator is an important component in batteries, with the primary function of separating the positive and negative electrodes and allowing the free passage of ions. Porous organic framework materials have a stable connection structure, large specific surface area, and ordered pores, which are natural places to store electrolytes. And these materials with specific functions can be designed according to the needs of researchers. The performance of porous organic framework-based separators used in rechargeable lithium metal batteries is much better than that of polyethylene/propylene separators. In this paper, the three most classic organic framework materials (MOF, COF, and HOF) are analyzed and summarized. The applications of MOF, COF, and HOF separators in lithium-sulfur batteries, lithium metal anode, and solid electrolytes are reviewed. Meanwhile, the research progress of these three materials in different fields is discussed based on time. Finally, in the conclusion, the problems encountered by MOF, COF, and HOF in different fields as well as their future research priorities are presented. This review will provide theoretical guidance for the design of porous framework materials with specific functions and further stimulate researchers to conduct research on porous framework materials.

Tuning the D-Band Center of Bi2S3─MoS2 Heterostructure Towards Superior Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries are one of the most promising energy storage devices due to their environmental friendliness, low cost, and high specific capacity. However, the slow electrochemical kinetics and the "shuttle effect" have seriously hindered their commercialization. Herein, the nanoflower Bi2S3─MoS2 (BMS) heterostructure is synthesized by a two-step hydrothermal method, and then the Bi2S3─MoS2-Polypropylene (BMS-PP) interlayer is constructed. The heterostructure is rich in active sites, in which BMS has strong adsorption to lithium polysulfides (LiPSs) and can effectively anchor LiPSs while catalyzing LiPSs and promote the redox of Li2S at the same time, which can improve the utilization of active substances. More importantly, the d-band center can be tuned by the formation of Bi2S3─MoS2 heterostructure. Thus, Li-S batteries containing the BMS-PP interlayer show excellent rate performance (841.6 mAh g-1 at 5 C) and cycling performance (70.3% capacity retention after 500 cycles at 3 C). This work provides a new route for high-performance lithium-sulfur batteries.