Lychee-like TiO2@TiN dual-function composite material for lithium–sulfur batteries

Lithium–sulfur (Li–S) batteries are promising candidates for next generation rechargeable batteries because of their high energy density of 2600 W h kg⁻¹. However, the insulating nature of sulfur and Li₂S, the “shuttle effect” of lithium polysulfides (LiPSs), and the volumetric change of sulfur electrodes limit the practical application of Li–S batteries. Here, lychee-like TiO₂@TiN hollow spheres (LTTHS) have been developed that combine the advantages of high adsorption TiO₂ and high conductivity TiN to achieve smooth adsorption/spread/conversion of LiPSs and use them as a sulfur host material in Li–S batteries for the first time. The cathode exhibits an initial specific capacity of 1254 mA h g⁻¹ and a reversible capacity of 533 mA h g⁻¹ after 500 cycles at 0.2C, which corresponds to an average coulombic efficiency up to 99%. The cell with the LTTHS@S cathode achieved an extended lifespan of over 1000 cycles. Such good performance can be assigned to the good adsorption and catalysis of the dual-function TiO₂@TiN composite. This work proved that the TiO₂@TiN composite can be an attractive matrix for sulfur cathodes.

Lithium–sulfur (Li–S) batteries are promising candidates for next generation rechargeable batteries because of their high energy density of 2600 W h kg⁻¹.     

Bagasse as a carbon structure with high sulfur content for lithium–sulfur batteries

A bagasse-based 3D carbon matrix (BC) with high specific surface area and high conductivity was obtained by carbonization and pore-forming processes with bagasse as the carbon precursor and K₂FeO₄ as the pore-former. The microporous structure and nitrogenous functional groups were determined in the prepared carbon matrix, which could allow high sulfur loading and improve the polysulfide absorption capacity during cycling. After sulfur infusion, the S/BC composite with 68.8% sulfur content was obtained. The lithium–sulfur (Li–S) battery with the S/BC cathode shows high specific capacity and good cycling performance. It delivers a specific capacity of 1360 mA h g⁻¹ at 0.2C and remains at 790 mA h g⁻¹ after 200 cycles. At 1C, the Li–S with this composite cathode exhibits 601 mA h g⁻¹ after 150 cycles. This work offers a new kind of green material and a new method for Li–S batteries.

Bagasse-based carbon matrix with microporous structure and nitrogenous functional groups could have high sulfur loading and excellent polysulfide absorption capacity.     

Self-assembled layer-by-layer partially reduced graphene oxide–sulfur composites as lithium–sulfur battery cathodes

Constructing a reliable conductive carbon matrix is essential for the sulfur-containing cathode materials of lithium–sulfur batteries. A ready-made conductive matrix infiltrated with sulfur as the cathode is the usual solution. Here, a partially reduced graphene oxide–sulfur composite (prGO/S) with an ordered self-assembled layer-by-layer structure is introduced as a Li–S battery cathode. The prGO/S composites are synthesized through a facile one-step self-assembly liquid route. An appropriate amount of sulfur is in situ deposited on the surface of the prGO nanosheets by adjusting the reduction degree of the GO nanosheets. The combined effect of the electrostatic repulsions and surface energy makes the sulfur wrapped prGO nanosheets self-assemble to form an ordered layer-by-layer structure, which not only ensures the uniform distribution of sulfur but also accommodates the volume change of the sulfur species during cycling. Moreover, the conductivity of the prGO/S composites improves when the reduction time increases. XPS spectra confirm that sulfur is still chemically bonded to the prGO. After applying the prGO coating of the prGO/S composite particle and as an interlayer in a lithium–sulfur battery configuration, a high initial discharge capacity of 1275.8 mA h g⁻¹ is achieved and the discharge capacity of the 100th cycle is 1013.8 mA h g⁻¹ at 0.1C rate.

The general procedures for the synthesis of the self-assembled layer-by-layer prGO/S composites.     

Low cost bio-derived carbon-sprinkled manganese dioxide as an efficient sulfur host for lithium–sulfur batteries

Realization of the lithium-sulfur battery system is of major concern because a theoretical cell capacity of 1675 mA h g⁻¹ can be obtained at an average voltage of 2.1 V. The primary issues that hinder the practical applications of this system include its poor utilization of sulfur, limited cycle life and retarded rate performance. In the present study, hemp-derived carbon (C-hemp) is made into a composite with room temperature-synthesized MnO₂, which acts as a host for sulfur in the lithium-sulfur battery system. The composite material is characterized physico-chemically and electrochemically using various techniques. This composite exhibits better electrochemical performance as a sulfur carrier compared to pristine carbon. An initial specific capacity of 926 mA h g⁻¹ is obtained at 0.1 C for C-hemp/MnO₂-sulfur, which surpasses that of the C-hemp-sulfur sample. C-hemp provides a conductive matrix as well as porous sites for the accommodation of sulfur, while MnO₂ exhibits the ability to absorb polysulfide chemically. Thus, this composite is established as a potential cathode for lithium-sulfur batteries.

MnO₂-biomass (hemp) derived carbon composite is used as an effective cathode in Li–S cell. MnO₂ acted as polysulfide scuffolding in the composite enhancing Li–S cell performance. New carbon source (hemp-fibre) was utilised successfully in Li–S.     

A new metallic π-conjugated carbon sheet used for the cathode of Li–S batteries

Lithium–sulfur (Li–S) batteries are considered as the most promising next generation high density energy storage devices. However, the commercialization of Li–S batteries is hindered by the shuttle effect of polysulfides, the low electronic conductivity of the sulfur cathode and a large volume expansion during lithiation. Herein, we predict a new two dimensional sp² hybridized carbon allotrope (PHE-graphene) and prove its thermodynamic and kinetic stability. If it is utilized to encapsulate the cathode of Li–S batteries, not only will the shuttle effect be avoided but also the electronic conductivity of the sulfur cathode will be improved significantly owing to its metallic electronic band structure. The thermal conductivity of PHE-graphene was found to be very high and even comparable with graphene, which is helpful for the heat dissipation of cathodes. In addition, PHE-graphene also exhibited superior mechanical properties including ideal tensile strength and in-plane stiffness.

A metallic carbon sheet was used for the cathode of Li–S batteries to eliminate the shuttle effect and improve cathode electric conductivity.     

Mesoporous TiO2 coating on carbon–sulfur cathode for high capacity Li–sulfur battery

In this paper, a meso-porous TiO₂ (titania) coating is shown to effectively protect a carbon–sulfur composite cathode from polysulfide dissolution. The cathode consisted of a sulfur impregnated carbon support coated with a few microns thick mesoporous titania layer. The carbon–sulfur cathode is made using activated carbon powder (ACP) derived from biomass. The mesoporous titania coated carbon–sulfur cathodes exhibit a retention capacity after 100 cycles at C/3 rate (433 mA g ⁻¹) and stabilized at a capacity around 980 mA h g⁻¹. The electrochemical impedance spectroscopy (EIS) of the sulfur cathodes suggests that the charge transfer resistance at the anode, (R_act) is stable for the titania coated sulfur electrode in comparison to a continuous increase in R_act for the uncoated electrode implying mitigation of polysulfide shuttling for the protected cathode. Stability in the cyclic voltammetry (CV) data for the first 5 cycles further confirms the polysulfide containment in the titania coated cathode while the uncoated sulfur electrode shows significant irreversibility in the CV with considerable shifting of the voltage peak positions. Raman spectroscopy and X-ray photoelectron spectroscopy (XPS) studies confirm the adsorption of soluble polysulfides by mesoporous titania.

Mesoporous TiO₂ coating on carbon–sulfur cathode with simple electrical contact for high capacity Li–S battery.     

Stabilizing cathode structure via the binder material with high resilience for lithium–sulfur batteries

Lithium–sulfur (Li–S) batteries have been considered as one of the most promising next-generation energy storage systems with high-energy density. The huge volumetric change of sulfur (ca. 80% increase in volume) in the cathode during discharge is one of the factors affecting the battery performance, which can be remedied with a binder. Herein, a self-crosslinking polyacrylate latex (PAL) is synthesized and used as a binder for the sulfur cathode of a Li–S battery to keep the cathode structure stable. The synthesized PAL has nano-sized latex particles and a low glass transition temperature (T_g), which will ensure a uniform dispersion and good adhesion in the cathode. This crosslinking structure can provide fine elasticity to recover from the deformation due to volumetric change. The stable cathode structure, stemming from the fine elasticity of the PAL binder, can facilitate ion migration and diffusion to decrease the polarization. Therefore, the Li–S batteries with the PAL binder can function well with excellent cycling stability and superior C-rate performance.

A self-crosslinking polyacrylate binder with fine elasticity stabilizing the sulfur cathode and endowing Li–S batteries with excellent performance.     

The phase transfer effect of sulfur in lithium–sulfur batteries

Lithium–sulfur (Li–S) batteries are considered to be among the most promising energy storage technologies owing to their high theoretical capacity (1675 mA h g⁻¹). At present, however, discharge mechanisms are complicated and remain a controversial issue. In this work, elemental sulfur, used as an electrical insulator for the cathode, was introduced into batteries for its potential chemical reactions in the electrolyte. A film, prepared by loading elemental sulfur onto glass fiber, was introduced as an interlayer in a Li–S battery. The results demonstrate that elemental sulfur may be reduced to polysulfides even when it functions as an electrical insulator for the cathode. Furthermore, it can improve the overall capacity of the Li–S battery and cycle life. This was verified by simulating the phase equilibrium of the chemical system in Li–S batteries using HSC Chemistry software. We hypothesize that the insulating elemental sulfur could be reduced by polysulfides generated on the cathode, after which they are dissolved in the electrolyte and participate in cathode reactions. This phase transfer effect of sulfur in Li–S batteries revealed a chemical equilibrium in the electrolyte of the Li–S battery, which may form a chemical path embedded into the discharge process of Li–S batteries.

The insulating elemental sulfur in a Li–S battery could be reduced to high-grade polysulfides by low-grade polysulfides from the cathode, after which they could participate in the discharging process of the Li–S battery.     

Ultradispersed titanium dioxide nanoparticles embedded in a three-dimensional graphene aerogel for high performance sulfur cathodes

Lithium–sulfur (Li–S) batteries are regarded as one of the most promising energy storage technologies, however, their practical application is greatly limited by a series of sulfur cathode challenges such as the notorious “shuttle effect”, low conductivity and large volume change. Here, we develop a facile hydrothermal method for the large scale synthesis of sulfur hosts consisting of three-dimensional graphene aerogel with tiny TiO₂ nanoparticles (5–10 nm) uniformly dispersed on the graphene sheet (GA–TiO₂). The obtained GA–TiO₂ composites have a high surface area of ∼360 m² g⁻¹ and a hierarchical porous structure, which facilitates the encapsulation of sulfur in the carbon matrix. The resultant GA–TiO₂/S composites exhibit a high initial discharge capacity of 810 mA h g⁻¹ with an ultralow capacity fading of 0.054% per cycle over 700 cycles at 2C, and a high rate (5C) performance (396 mA h g⁻¹). Such architecture design paves a new way to synthesize well-defined sulfur hosts to tackle the challenges for high performance Li–S batteries.

GA–TiO₂ composites as a cathode material realize an excellent electrochemical performance in Li–S batteries.     

Interaction between functionalized graphene and sulfur compounds in a lithium–sulfur battery – a density functional theory investigation

Lithium–sulfur (Li–S) batteries are emerging as one of the promising candidates for next generation rechargeable batteries. However, dissolution of lithium polysulfides in the liquid electrolyte, low electrical conductivity of sulfur and large volume change during electrochemical cycling are the main technical challenges for practical applications. In this study, a systematic first-principles density functional theory calculation is adopted to understand the interactions between graphene and graphene with oxygen containing functional groups (hydroxyl, epoxy and carboxyl groups) and sulphur (S₈) and long chain lithium polysulfides (Li₂S₈ and Li₂S₄). We find the adsorption is dominated by different mechanisms in sulphur and lithium polysulfides, i.e. van der Waals attraction and formation of coordinate covalent Li–O bonds. The adsorption strength is dependent on the inter-layer distance and electron rich functional groups. Through these mechanisms, sulphur and lithium polysulfides can be successfully retained in porous graphene, leading to improved conductivity and charge transfer in the cathode of Li–S batteries.

Functionalized graphene can successfully anchor sulfur compounds via moderate interactions, leading to improved conductivity and charge transfer in the cathode of Li–S batteries.     

Polyvinylchloride-derived N,S co-doped carbon as an efficient sulfur host for high-performance Li–S batteries

The intrinsic polysulfide shuttle in lithium–sulfur (Li–S) batteries have significantly limited their practical applications. Conductive carbon materials with heteroatom doping and rich porosity is the most common strategy for the effective prevention of polysulfide shuttle, but are usually obtained with high costs and tedious procedures. Herein, we managed to obtain highly porous N, S-codoped carbon materials (NS-C) through treating waste plastic of polyvinylchloride (PVC) with KOH. The resulting NS-C was revealed to be highly efficient hosts for sulfur cathode, achieving large reversible capacities of 1205 mA h g⁻¹ and 836 mA h g⁻¹ at 0.1C and 1.0C, respectively, and remaining at 550 mA h g⁻¹ after 500 cycles at 1C rate, showing an outstanding cycling stability. The significantly enhanced cycling performance was mainly ascribed to both the hierarchically porous structure and heavy N, S co-dopants, which respectively provided physical blocks and chemical affinity for the efficient immobilization of intermediate lithium polysulfides. The results provide an effective paradigm in the surface chemistry and sulfur cathode materials design for high-performance Li–S batteries and a new application for recycled plastic waste.

The intrinsic polysulfide shuttle in lithium–sulfur (Li–S) batteries have significantly limited their practical applications.     

A defective MOF architecture threaded by interlaced carbon nanotubes for high-cycling lithium–sulfur batteries

Metal organic frameworks (MOFs) have been deemed among the most promising sulfur hosts for lithium–sulfur (Li–S) batteries owing to their high specific surface areas, novel pore structures and open metal sites. However, their highly coordinated, electronically insulating and structurally unstable nature overshadows the merits of MOFs to a great extent. In this work, a novel UiO-66/carbon nanotube (UC) composite was initially synthesized via a facile one-pot synthesis strategy, in which abundant linker-missing defects were caused by introduced competitive coordination. Meanwhile, flexible and interlaced carbon nanotubes (CNTs) throughout mechanically stable UiO-66 nanoparticles constructed a reliable conductive network. Because of its superior structural stability, high electronic conductivity and strong polysulfide chemisorption, the UC architecture as the sulfur cathode in Li–S batteries shows stable cycling, delivering an initial capacity of 925 mA h g⁻¹ at 0.5 A g⁻¹ and a very low fading rate over 800 cycles of 0.071% per cycle at 1 A g⁻¹. A strong chemical affinity between coordination defects and LiPSs was revealed by first principles calculations and apparent absorption, which indicates significant entrapment of soluble polysulfides by the UC composite, thus leading to the outstanding cycling performance of S@UC electrodes.

Abundant artificial linker-missing defects as active sites display superior chemisorption of LiPSs, which contribute to outstanding cycling performance in Li–S cells.     

A N-doped graphene–cobalt nickel sulfide aerogel as a sulfur host for lithium–sulfur batteries

Herein, three-dimensional (3D) N-doped reduced graphene oxide (N-rGO) nanosheets were decorated with a uniform distribution of Co–Ni–S (CNS) nanoparticles to form the CNS/N-rGO composite as a sulfur host material for lithium–sulfur batteries. The CNS nanoparticles and N in CNS/N-rGO strongly interact with polysulfides, whereas graphene, as a conductive network, can improve its electrical conductivity. A CNS/N-rGO/sulfur composite cathode was prepared via the sulfur melting diffusion method. The electrochemical study showed that the CNS/N-rGO/sulfur cathode delivered an initial discharge capacity of 1430 mA h g⁻¹ at a current density of 0.1C. Moreover, it retained a specific capacity of 685 mA h g⁻¹ after 300 cycles at 0.5C with a coulombic efficiency of 98%, which was better than that of commercial rGO. This composite was used as a sulfur cathode for a lithium–sulfur battery, exhibiting excellent rate capability and remarkable performance in terms of long cycling stability.

Herein, three-dimensional (3D) N-doped reduced graphene oxide (N-rGO) nanosheets were decorated with a uniform distribution of Co–Ni–S (CNS) nanoparticles to form the CNS/N-rGO composite as a sulfur host material for lithium–sulfur batteries.     

Sulfur encapsulated in thermally reduced graphite oxide as a cathode for Li–S batteries

Rechargeable Li–S batteries are receiving ever-increasing attention due to their high theoretical energy density and inexpensive raw sulfur materials. However, their practical applications have been hindered by short cycle life and limited power density owing to the poor electronic conductivity of sulfur species, diffusion of soluble polysulfide intermediates (Li₂S_n, n = 4–8) and the large volume change of the S cathode during charge/discharge. Optimizing the carbon framework is considered as an effective approach for constructing high performance S/carbon cathodes because the microstructure of the carbon host plays an important role in stabilizing S and restricting the “shuttle reaction” of polysulfides in Li–S batteries. In this work, reduced graphite oxide (rGO) materials with different oxidation degree were investigated as the matrix to load the active material by an in situ thermally reducing graphite oxide (GO) and intercalation strategy under vacuum at 600 °C. It has been found that the loaded amount of S embedded in the rGO layer for the S/carbon cathode and its electrochemical performance strongly depended on the oxidation degree of GO. In particular, on undergoing CS₂ treatment, the rGO–S cathode exhibits extraordinary performances in Li–S batteries. For instance, at a current density of 0.2 A g⁻¹, the optimized rGO–S cathode shows a columbic efficiency close to 100% and retains a capacity of around 750 mA h g⁻¹ with progressive cycling up to over 250 cycles.

Reduced graphite oxide materials with different oxidation degree were investigated as the matrix to load sulfur by an in situ thermal-reduction and intercalation strategy. The C/S composite cathode exhibits a superior electrochemical properties.     

TiO2-decorated porous carbon nanofiber interlayer for Li–S batteries

Lithium–sulfur (Li–S) batteries are the most promising energy storage systems owing to their high energy density. However, shuttling of polysulfides detracts the electrochemical performance of Li–S batteries and thus prevents the commercialization of Li–S batteries. Here, TiO₂@porous carbon nanofibers (TiO₂@PCNFs) are fabricated via combining electrospinning and electrospraying techniques and the resultant TiO₂@PCNFs are evaluated for use as an interlayer in Li–S batteries. TiO₂ nanoparticles on PCNFs are observed from SEM and TEM images. A high initial discharge capacity of 1510 mA h g⁻¹ is achieved owing to the novel approach of electrospinning the carbon precursor and electrospraying TiO₂ nanoparticles simultaneously. In this approach TiO₂ nanoparticles capture polysulfides with strong interaction and the PCNFs with high conductivity recycle and re-use the adsorbed polysulfides, thus leading to high reversible capacity and stable cycling performance. A high reversible capacity of 967 mA h g⁻¹ is reached after 200 cycles at 0.2C. The cell with the TiO₂@PCNF interlayer also delivers a reversible capacity of around 1100 mA h g⁻¹ at 1C, while the cell without the interlayer exhibits a lower capacity of 400 mA h g⁻¹. Therefore, this work presents a novel approach for designing interlayer materials with exceptional electrochemical performance for high performance Li–S batteries.

Lithium–sulfur (Li–S) batteries are the most promising energy storage systems owing to their high energy density.     

Cationic polymer-grafted graphene oxide/CNT cathode-coating material for lithium–sulfur batteries

A cathode-coating material composed of cationic polymer-grafted graphene oxide (CPGO) and carbon nanotube (CNT) was prepared, where the CPGO was synthesized by grafting quaternized 2-(dimethylamino)ethyl methacrylate (QDMAEMA) onto graphene oxide (GO) via atom transfer radical polymerization (ATRP). GO has good compatibility with carbon black, the main component of the cathode in lithium–sulfur (Li–S) batteries. Here, the cationic polymer having the QDMAEMA unit was intentionally grafted onto GO to decrease the shuttle effect by increasing the chemical adsorption of polysulfide (PS). In addition, when CNT was mixed with CPGO, the compatibility with carbon black was found to be further increased. The lithium–sulfur (Li–S) battery with a sulfur-deposited Super P® carbon black (S/C) cathode coated with a mixture of CPGO and CNT was found to have much improved cell performance compared to those coated without any coating material, with only CPGO, with the mixture of GO and CNT, and with the mixture of PQDMAEMA and CNT. For example, the Li–S battery with the cathode coated using the mixture of CPGO and CNT retained a discharge capacity of 744 mA h g⁻¹ after 50 cycles at 0.2C-rate, while those of the Li–S batteries with bare S/C and CPGO-S/C cathodes were found to be much smaller, i.e., 488 mA h g⁻¹ and 641 mA h g⁻¹, respectively, under the same conditions. Therefore, the mixture of CPGO with CNT as the cathode-coating material showed a synergetic effect to enhance the cell performance of the Li–S battery system.

A cathode-coating material composed of cationic polymer-grafted graphene oxide (CPGO) and carbon nanotube (CNT) was prepared and used as a cathode-coating material for lithium sulfur batteries.     

Nitrogen–sulfur dual-doped porous carbon spheres/sulfur composites for high-performance lithium–sulfur batteries

A nitrogen–sulfur dual-doped porous carbon spheres/sulfur composite (PCS-NS/S) sample was prepared by a simple hydrothermal method with starch and l-methionine as carbon and nitrogen–sulfur resources, respectively. XRD, XPS, and N₂ adsorption–desorption tests were used to characterize the crystal and pore structure of the PCS-NS/S sample. The morphology and weight ratio of sulfur were investigated by SEM, TEM, and TG analyses. The sample was used as the positive electrode for lithium–sulfur batteries and found to exhibit excellent electrochemical performance.

Simultaneously introduced nitrogen–sulfur through one reagent. The as-prepared PCS-NS/S composites exhibited excellent electrochemical performance as positive electrode for Li–S battery.     

Influence of morphology of monolithic sulfur–poly(acrylonitrile) composites used as cathode materials in lithium–sulfur batteries on electrochemical performance

Solvent-induced phase separation (SIPS) and thermally-induced phase separation (TIPS) derived poly(acrylonitrile) (PAN) based monoliths with different morphology and specific surface area were prepared and thermally converted into monolithic sulfur–poly(acrylonitrile) (SPAN) materials for use as active cathode materials in lithium–sulfur batteries. During thermal processing, the macroscopic monolithic structure fully prevailed while significant changes in porosity were observed. Both the monomer content in the precursor PAN-based monoliths and the tortuosity of the final monolithic SPAN materials correlate with the electrochemical performance of the SPAN-based cathodes. Overall, percolation issues predominate. In percolating SPAN-based cathode materials, the specific capacity of the SPAN-based cells increases with decreasing tortuosity. All monolithic SPAN materials provided highly reversible and cycle stable cathodes reaching reversible discharge capacities up to 1330 mA h g_sulfur⁻¹ @ 0.25C, 900 mA h g_sulfur⁻¹ @ 2C and 420 mA h g_sulfur⁻¹ @ 8C.

Influence of SPAN-based cathode materials with a defined morphology on the electrochemical behavior of Li–S-cells.     

In situ template synthesis of hierarchical porous carbon used for high performance lithium–sulfur batteries

Hierarchical porous carbon (HPC) consists of micropores, mesopores and macrospores which are synthesized by in situ formation of template followed by acid etching. The obtained pores are three-dimensional and interconnected, and evenly distributed in the carbon matrix. By adjusting the ratio of the raw materials, the high specific surface area and large pore volume is afforded. The obtained HPC-3 samples possess graphite flakes and locally graphited-carbon walls, which provide good electrical conductivity. These unique characteristics make these materials suitable cathode scaffolds for Li–S batteries. After encapsulating 61% sulfur into HPC-3 host, the S/HPC-3 composite exhibits excellent cycling stability, high columbic efficiency, and superior rate cycling as a cathode material. The S/HPC-3 composite cathode displays an initial discharge capacity of 1059 mA h g⁻¹, and a reversible capacity of 797 mA h g⁻¹ after 200 cycles at 0.2C. The discharge capacities of the S/HPC-3 composite cathode after every 10 cycles at 0.1, 0.2, 0.5, 1, and 2C are 1119, 1056, 982, 921, and 829 mA h g⁻¹, respectively.

In situ template synthesis of HPCs used for lithium–sulfur batteries, which exhibits excellent cycling stability and superior rate cycling.     

Enhanced performance of lithium–sulfur batteries based on single-sided chemical tailoring,and organosiloxane grafted PP separator

Even after a decade of research and rapid development of lithium–sulfur (Li–S) batteries, the infamous shuttle effect of lithium polysulfide is still the major challenge hindering the commercialization of Li–S batteries. In order to further address this issue, a functionalized PP separator is obtained through selective single-sided chemical tailoring, and then organosiloxane fumigation grafting. During the charge–discharge process, the grafted functional groups can effectively block the transportation of the dissolved polysulfides through strong chemical anchoring, inhibit the shuttle effect and greatly enhance the cycle stability of the Li–S battery. Interestingly, the specially designed single-sided enlarged channel structure formed by chemical tailoring can well accommodate the deposition with intermediate polysulfides on the separator surface toward the cathode chamber, resulting in enhanced initial discharge capacity and rate performance. Compared to the battery assembled with PP, the Li–S battery employing the separator grafted with a 3-ureidopropyltrimethoxysilane (PP–O^x−–U) displays better electrochemical performance. Even at 2C, it can still deliver a high capacity of 786 mA h g⁻¹, and retain a capacity of 410 mA h g⁻¹ with a low capacity fading of 0.095% per cycle over 500 cycles. This work provides a very promising and feasible strategy for the development of a special functionalization PP separator for Li–S batteries with high electrochemical performance.

Even after a decade of research and rapid development of lithium–sulfur (Li–S) batteries, the infamous shuttle effect of lithium polysulfide is still the major challenge hindering the commercialization of Li–S batteries.