Ultrafine Co3Se4 Nanoparticles in Nitrogen‐Doped 3D Carbon Matrix for High‐Stable and Long‐Cycle‐Life Lithium Sulfur Batteries

Lithium–sulfur batteries are a promising high energy output solution for substitution of traditional lithium ion batteries. In recent times research in this field has stepped into the exploration of practical applications. However, their applications are impeded by cycling stability and short life‐span mainly due to the notorious polysulfide shuttle effect. In this work, a multifunctional sulfur host fabricated by grafting highly conductive Co₃Se₄ nanoparticles onto the surface of an N‐doped 3D carbon matrix to inhibit the polysulfide shuttle and improve the sulfur utilization is proposed. By regulating the carbon matrix and the Co₃Se₄ distribution, N‐CN‐750@Co₃Se₄‐0.1 m with abundant polar sites is experimentally and theoretically shown to be a good LiPSs absorbent and a sulfur conversion accelerator. The S/N‐CN‐750@Co₃Se₄‐0.1 m cathode shows excellent sulfur utilization, rate performance, and cyclic durability. A prolonged cycling test of the as‐fabricated S/N‐CN‐750@Co₃Se₄‐0.1 m cathode is carried out at 0.2 C for more than 5 months which delivers a high initial capacity of 1150.3 mAh g^?1 and retains 531.0 mAh g^?1 after 800 cycles with an ultralow capacity reduction of 0.067% per cycle, maintaining Coulombic efficiency of more than 99.3%. The reaction details are characterized and analyzed by ex situ measurements. This work highly emphasizes the potential capabilities of transition‐metal selenides in lithium–sulfur batteries.     

Interfacial Charge Field in Hierarchical Yolk–Shell Nanocapsule Enables Efficient Immobilization and Catalysis of Polysulfides Conversion

Inhibiting the shuttle effect of lithium polysulfides and accelerating their conversion kinetics are crucial for the development of high‐performance lithium–sulfur (Li–S) batteries. Herein, a modified template method is proposed to synthesize the robust yolk–shell sulfur host that is constructed by enveloping dispersive Fe₂O₃ nanoparticles within Mn₃O₄ nanosheet‐grafted hollow N‐doped porous carbon capsules (Fe₂O₃@N‐PC/Mn₃O₄‐S). When applied as a cathode for Li–S batteries, the as‐prepared Fe₂O₃@N‐PC/Mn₃O₄‐S can deliver capacities as high as 1122 mAh g^?1 after 200 cycles at 0.5 C and 639 mAh g^?1 after 1500 cycles at 10 C, respectively. Remarkably, even as the areal sulfur loading is increased to 5.1 mg cm^?2, the cathode can still maintain a high areal specific capacity of 5.08 mAh cm^?2 with a fading rate of only 0.076% per cycle over 100 cycles at 0.1 C. By a further combination analysis of electron holography and electron energy loss spectroscopy, the outstanding performance is revealed to be mainly traced to the oxygen‐vacancy‐induced interfacial charge field, which immobilizes and catalyzes the conversion of lithium polysulfides, assuring low polarization, fleet redox reaction kinetics, and sufficient utilization of sulfur. These new findings may shed light on the dependence of electrochemical performance on the heterostructure of sulfur hosts.     

Sandwich‐Like Ultrathin TiS2 Nanosheets Confined within N,S Codoped Porous Carbon as an Effective Polysulfide Promoter in Lithium‐Sulfur Batteries

As the lightest member of transition metal dichalcogenides, 2D titanium disulfide (2D TiS₂) nanosheets are attractive for energy storage and conversion. However, reliable and controllable synthesis of single‐ to few‐layered TiS₂ nanosheets is challenging due to the strong tendency of stacking and oxidation of ultrathin TiS₂ nanosheets. This study reports for the first time the successful conversion of Ti₃C₂T_x MXene to sandwich‐like ultrathin TiS₂ nanosheets confined by N, S co‐doped porous carbon (TiS₂@NSC) via an in situ polydopamine‐assisted sulfuration process. When used as a sulfur host in lithium–sulfur batteries, TiS₂@NSC shows both high trapping capability for lithium polysulfides (LiPSs), and remarkable electrocatalytic activity for LiPSs reduction and lithium sulfide oxidation. A freestanding sulfur cathode integrating TiS₂@NSC with cotton‐derived carbon fibers delivers a high areal capacity of 5.9 mAh cm^?2 after 100 cycles at 0.1 C with a low electrolyte/sulfur ratio and a high sulfur loading of 7.7 mg cm^?2, placing TiS₂@NSC one of the best LiPSs adsorbents and sulfur conversion catalysts reported to date. The developed nanospace‐confined strategy will shed light on the rational design and structural engineering of metal sulfides based nanoarchitectures for diverse applications.     

Double‐Shelled NiO‐NiCo2O4 Heterostructure@Carbon Hollow Nanocages as an Efficient Sulfur Host for Advanced Lithium–Sulfur Batteries

Double‐shelled NiO‐NiCo₂O₄ heterostructure@carbon hollow nanocages as efficient sulfur hosts are synthesized to overcome the barriers of lithium–sulfur (Li–S) batteries simultaneously. The double‐shelled nanocages can prevent the diffusion of lithium polysulfides (LiPSs) effectively. NiO‐NiCo₂O₄ heterostructure is able to promote polysulfide conversion reactions. Furthermore, the thin carbon layer outside can improve the electrical conductivity during cycling. Besides, such unique double‐shelled hollow nanocage architecture can also accommodate the volumetric effect of sulfur upon cycling. As a result, the prepared S/NiO‐NiCo₂O₄@carbon (C) electrode exhibits good rate capacities and stable cycling life up to 500 cycles at 0.5 C with a very low capacity decay rate of only ≈0.059% per cycle.     

Rationalizing Electrocatalysis of Li–S Chemistry by Mediator Design: Progress and Prospects

The lithium–sulfur (Li–S) battery is regarded as a next‐generation energy storage system due to its conspicuous merits in high theoretical capacity (1672 mAh g^?1), overwhelming energy density (2600 Wh kg^?1), and the cost‐effectiveness of sulfur. However, the practical application of Li–S batteries is still handicapped by a multitude of key challenges, mainly pertaining to fatal lithium polysulfide (LiPS) shuttling and sluggish sulfur redox kinetics. In this respect, rationalizing electrocatalytic processes in Li–S chemistry to synergize the entrapment and conversion of LiPSs is of paramount significance. This review summarizes recent progress and well‐developed strategies of the mediator design toward promoted Li–S chemistry. The current advances, existing challenges, and future directions are accordingly highlighted, aiming at providing in‐depth understanding of the sulfur reaction mechanism and guiding the rational mediator design to realize high‐energy and long‐life Li–S batteries.     

Catalytic and Dual‐Conductive Matrix Regulating the Kinetic Behaviors of Polysulfides in Flexible Li–S Batteries

The main challenge in developing foldable Li–S batteries (LSB) lies in developing an electrode that is ultraflexible, conductive, and catalytic for dissolved lithium polysulfides (LiPSs). In this paper, lightweight macromolecule graphitic carbon nitride (g‐C₃N₄) film and a conductive polymer (CP) of poly(3,4‐ethylenedioxythiophene) shell are introduced into flexible LSBs by compositing with carbon cloth (CC). In the designed hybrid of CP/g‐C₃N₄@CC, 2D g‐C₃N₄ is used in the form of an effective trapper and functions as a continuous catalytic layer for LiPSs via the formation of pyridinic‐N‐Li bonds. This is revealed by both experimental investigations and theoretical analysis. The sandwich‐like CC and CP simultaneously bring an omnidirectional conductive network for fast interfacial reaction kinetics. With these benefits, the self‐supported CP/g‐C₃N₄@CC forms a powerful interaction system to fully in situ “lock” LiPSs in the commercial CC matrix. Thus, a substantially enhanced electrochemical performance is obtained at a high sulfur loading (4.7 mg cm^–2) even operating in a pouch cell. This work may provide a potential avenue for practical use of high‐performance LSBs toward flexible energy‐storage devices.     

MoN Supported on Graphene as a Bifunctional Interlayer for Advanced Li‐S Batteries

Rational design of effective polysulfide barriers is highly important for high‐performance lithium‐sulfur (Li‐S) batteries. A variety of adsorbents have been applied as interlayers to alleviate the shuttle effect. Nevertheless, the unsuccessful oxidation of Li₂S on interlayers leads to loss of active materials and blocks Li ion transport. In this work, a MoN‐based interlayer sandwiched between the C‐S cathode and the separator is developed. Such an interlayer not only strongly binds lithium polysulfides via Mo‐S bonding but also efficiently accelerates the decomposition of Li₂S. The acceleration mechanism toward Li₂S decomposition is determined to be a combination of contributions of catalytic cleavage of Li‐S bond in Li₂S based on the proposed covalence‐activation mechanism and rapid migration of the produced Li ions. As a result, the C–S cathodes with the as‐developed interlayer manifest a negligible charging potential barrier and outstanding cycling stability with a very low capacity fading rate of 0.023% per cycle during 1500 cycles at 1 C. High areal capacity of 6.02 mAh cm^?2 is achieved for high sulfur loading of 7.0 mg cm^?2 after cycling at 0.1 C. The material and strategy demonstrated in this work can open the door toward developing shuttle suppression interlayers without impairing cathode performance.     

Electrokinetic Phenomena Enhanced Lithium‐Ion Transport in Leaky Film for Stable Lithium Metal Anodes

The application of lithium (Li) metal anodes in Li metal batteries has been hindered by growth of Li dendrites, which lead to short cycling life. Here a Li‐ion‐affinity leaky film as a protection layer is reported to promote a dendrite‐free Li metal anode. The leaky film induces electrokinetic phenomena to enhance Li‐ion transport, leading to a reduced Li‐ion concentration polarization and homogeneous Li‐ion distribution. As a result, the dendrite‐free Li metal anode during Li plating/stripping is demonstrated even at an extremely high deposition capacity (6 mAh cm^?2) and current density (40 mA cm^?2) with improved Coulombic efficiencies. A full cell battery with the leaky‐film protected Li metal as the anode and high‐areal‐capacity LiNi_0.8Co_0.1Mn_0.1O₂ (NCM‐811) (≈4.2 mAh cm^?2) or LiFePO₄ (≈3.8 mAh cm^?2) as the cathode shows improved cycling stability and capacity retention, even at lean electrolyte conditions.     

High Capacity All‐Solid‐State Lithium Batteries Enabled by Pyrite‐Sulfur Composites

As the theoretical limit of intercalation material‐based lithium‐ion batteries is approached, alternative chemistries based on conversion reactions are presently considered. The conversion of sulfur is particularly appealing as it is associated with a theoretical gravimetric energy density up to 2510 Wh kg^?1. In this paper, three different carbon‐iron disulfide‐sulfur (C‐FeS₂‐S) composites are proposed as alternative positive electrode materials for all‐solid‐state lithium‐sulfur batteries. These are synthesized through a facile, low‐cost, single‐step ball‐milling procedure. It is found that the crystalline structure (evaluated by X‐ray diffraction) and the morphology of the composites (evaluated by scanning electron microscopy) are greatly influenced by the FeS₂:S ratio. Li/LiI‐Li₃PS₄/C‐FeS₂‐S solid‐state cells are tested under galvanostatic conditions, while differential capacity plots are used to discuss the peculiar electrochemical features of these novel materials. These cells deliver capacities as high as 1200 mAh g_(FeS2+S)^?1 at the intermediate loading of 1 mg cm^?2 (1.2 mAh cm^?2), and up to 3.55 mAh cm^?2 for active material loadings as high as 5 mg cm^?2 at 20 °C. Such an excellent performance, rarely reported for (sulfur/metal sulfide)‐based, all solid‐state cells, makes these composites highly promising for real application where high positive electrode loadings are required.     

A Hollow‐Shell Structured V2O5 Electrode‐Based Symmetric Full Li‐Ion Battery with Highest Capacity

The symmetric batteries with an electrode material possessing dual cathodic and anodic properties are regarded as an ideal battery configuration because of their distinctive advantages over the asymmetric batteries in terms of fabrication process, cost, and safety concerns. However, the development of high‐performance symmetric batteries is highly challenging due to the limited availability of suitable symmetric electrode materials with such properties of highly reversible capacity. Herein, a triple‐hollow‐shell structured V₂O₅ (THS‐V₂O₅) symmetric electrode material with a reversible capacity of >400 mAh g^?1 between 1.5 and 4.0 V and >600 mAh g^?1 between 0.1 and 3.0 V, respectively, when used as the cathode and anode, is reported. The THS‐V₂O₅ electrodes assembled symmetric full lithium‐ion battery (LIB) exhibits a reversible capacity of ≈290 mAh g^?1 between 2 and 4.0 V, the best performed symmetric energy storage systems reported to date. The unique triple‐shell structured electrode makes the symmetric LIB possessing very high initial coulombic efficiency (94.2%), outstanding cycling stability (with 94% capacity retained after 1000 cycles), and excellent rate performance (over 140 mAh g^?1 at 1000 mA g^?1). The demonstrated approach in this work leaps forward the symmetric LIB performance and paves a way to develop high‐performance symmetric battery electrode materials.     

An Efficient Separator with Low Li‐Ion Diffusion Energy Barrier Resolving Feeble Conductivity for Practical Lithium–Sulfur Batteries

Due to unprecedented features including high‐energy density, low cost, and light weight, lithium–sulfur batteries have been proposed as a promising successor of lithium‐ion batteries. However, unresolved detrimental low Li‐ion transport rates in traditional carbon materials lead to large energy barrier in high sulfur loading batteries, which prevents the lithium–sulfur batteries from commercialization. In this report, to overcome the challenge of increasing both the cycling stability and areal capacity, a metallic oxide composite (NiCo₂O₄@rGO) is designed to enable a robust separator with low energy barrier for Li‐ion diffusion and simultaneously provide abundant active sites for the catalytic conversion of the polar polysulfides. With a high sulfur‐loading of 6 mg cm^?2 and low sulfur/electrolyte ratio of 10, the assembled batteries deliver an initial capacity of 5.04 mAh cm^?2 as well as capacity retention of 92% after 400 cycles. The metallic oxide composite NiCo₂O₄@rGO/PP separator with low Li‐ion diffusion energy barrier opens up the opportunity for lithium–sulfur batteries to achieve long‐cycle, cost‐effective operation toward wide applications in electric vehicles and electronic devices.     

N‐Doped Graphene Modified 3D Porous Cu Current Collector toward Microscale Homogeneous Li Deposition for Li Metal Anodes

Lithium metal is the most promising anode material for high‐energy‐density batteries due to its high specific capacity of 3860 mAh g^?1 and low reduction potential of ?3.04 V versus standard hydrogen electrode. However, huge volume change, safety concerns, and low efficiency impede the practical applications of Li metal anodes. Herein, it is shown that the nitrogen‐doped graphene modified 3D porous Cu (3DCu@NG) current collector can mitigate the above problems. The N‐doped graphene, coating on the surface of 3D current collector, not only contributes to a uniform Li⁺ flux, but also leads to a scattered distribution of electrons throughout the surface, finally contributing to a uniform Li deposition and the improved electrochemical performance. In addition, the continuously porous structure of 3DCu@NG provides a space for the metallic Li deposition and could effectually accommodate the volume expansion during cycling. As a result, the Li‐3DCu@NG anode exhibits a high areal capacity of 4 mAh cm^?2, a high Li utilization of ≈98%, and an ultralow voltage hysteresis of ≈19 mV. The multifunctional N‐doped graphene modified 3D porous current collector promisingly provides a strategy for safe and high‐energy lithium metal anodes.     

Porphyrin‐Derived Graphene‐Based Nanosheets Enabling Strong Polysulfide Chemisorption and Rapid Kinetics in Lithium–Sulfur Batteries

Lithium–sulfur (Li–S) batteries hold great promise as a next‐generation battery system because of their extremely high theoretical energy density and low cost. However, ready lithium polysulfide (LiPS) diffusion and sluggish redox kinetics hamper their cyclability and rate capability. Herein, porphyrin‐derived graphene‐based nanosheets (PNG) are proposed for Li–S batteries, which are achieved by pyrolyzing a conformal and thin layer of 2D porphyrin organic framework on graphene to form carbon nanosheets with a spatially engineered nitrogen‐dopant‐enriched skin and a highly conductive skeleton. The atomic skin is decorated with fully exposed lithiophilic sites to afford strong chemisorption to LiPSs and improve electrolyte wettability, while graphene substrate provides speedy electron transport to facilitate redox kinetics of sulfur species. The use of PNG as a lightweight interlayer enables efficient operation of Li–S batteries in terms of superb cycle stability (cyclic decay rate of 0.099% during 300 cycles at 0.5 C), good rate capability (988 mAh g^?1 at 2.0 C), and impressive sulfur loading (areal capacity of 8.81 mAh cm^?2 at a sulfur loading of 8.9 mg cm^?2). The distinct interfacial strategy is expected to apply to other conversion reaction batteries relying on dissolution–precipitation mechanisms and requiring interfacial charge‐ and mass‐transport‐mediation concurrently.     

Synergistic Engineering of Defects and Architecture in Binary Metal Chalcogenide toward Fast and Reliable Lithium–Sulfur Batteries

Lithium–sulfur (Li–S) batteries have great promise to support the next‐generation energy storage if their sluggish redox kinetics and polysulfide shuttling can be addressed. The rational design of sulfur electrodes plays key roles in tacking these problems and achieving high‐efficiency sulfur electrochemistry. Herein, a synergetic defect and architecture engineering strategy to design highly disordered spinel Ni–Co oxide double‐shelled microspheres (NCO‐HS), which consist of defective spinel NiCo₂O_4–x (x = 0.9 if all nickel is Ni²⁺ and cobalt is Co^2.13+), as the multifunctional sulfur host material is reported. The in situ constructed cation and anion defects endow the NCO‐HS with significantly enhanced electronic conductivity and superior polysulfide adsorbability. Meanwhile, the delicate nanoconstruction offers abundant active interfaces and reduced ion diffusion pathways for efficient Li–S chemistry. Attributed to these synergistic features, the sulfur composite electrode achieves excellent rate performance up to 5 C, remarkable cycling stability over 800 cycles and good areal capacity of 6.3 mAh cm^?2 under high sulfur loading. This proposed strategy based on synergy engineering could also inform material engineering in related energy storage and conversion fields.     

Optimized Catalytic WS2–WO3 Heterostructure Design for Accelerated Polysulfide Conversion in Lithium–Sulfur Batteries

The lithium–sulfur (Li–S) battery is a next generation high energy density battery, but its practical application is hindered by the poor cycling stability derived from the severe shuttling of lithium polysulfides (LiPSs). Catalysis is a promising way to solve this problem, but the rational design of relevant catalysts is still hard to achieve. This paper reports the WS₂–WO₃ heterostructures prepared by in situ sulfurization of WO₃, and by controlling the sulfurization degree, the structure is controlled, which balances the trapping ability (by WO₃) and catalytic activity (by WS₂) toward LiPSs. As a result, the WS₂–WO₃ heterostructures effectively accelerate LiPS conversion and improve sulfur utilization. The Li–S battery with 5 wt% WS₂–WO₃ heterostructures as additives in the cathode shows an excellent rate performance and good cycling stability, revealing a 0.06% capacity decay each cycle over 500 cycles at 0.5 C. By building an interlayer with such heterostructure‐added graphenes, the battery with a high sulfur loading of 5 mg cm^?2 still shows a high capacity retention of 86.1% after 300 cycles at 0.5 C. This work provides a rational way to prepare the metal oxide–sulfide heterostructures with an optimized structure to enhance the performance of Li–S batteries.     

Metal Sulfide‐Decorated Carbon Sponge as a Highly Efficient Electrocatalyst and Absorbant for Polysulfide in High‐Loading Li2S Batteries

Owing to its high theoretical specific capacity (1166 mA h g^?1) and particularly its advantage to be paired with a lithium‐metal‐free anode, lithium sulfide (Li₂S) is regarded as a much safer cathode for next‐generation advanced lithium–sulfur (Li–S) batteries. However, the low conductivity of Li₂S and particularly the severe “polysulfide shuttle” of lithium polysulfide (LiPS) dramatically hinder their practical application in Li–S batteries. To address such issues, herein a bifuctional 3D metal sulfide‐decorated carbon sponge (3DTSC), which is constructed by 1D carbon nanowires cross‐linked with 2D graphene nanosheets with high conductivity and polar 0D metal sulfide nanodots with efficient electrocatalytic activity and strong chemical adsorption capability for LiPSs, is presented. Benefiting from the well‐designed multiscale, multidimensional 3D porous nanoarchitecture with high conductivity, and efficient electrocatalytic and absorption ability, the 3DTSC significantly mitigates LiPS shuttle, improves the utilization of Li₂S, and facilitates the transport of electrons and ions. As a result, even with a high Li₂S loading of 8 mg cm^?2, the freestanding 3DTSC‐Li₂S cathode without a polymer binder and metallic current collector delivers outstanding electrochemical performance with a high areal capacity of 8.44 mA h cm^?2.     

An Ion‐Exchange Promoted Phase Transition in a Li‐Excess Layered Cathode Material for High‐Performance Lithium Ion Batteries

A new approach to intentionally induce phase transition of Li‐excess layered cathode materials for high‐performance lithium ion batteries is reported. In high contrast to the limited layered‐to‐spinel phase transformation that occurred during in situ electrochemical cycles, a Li‐excess layered Li[Li_0.2Mn_0.54Ni_0.13Co_0.13]O₂ is completely converted to a Li₄Mn₅O₁₂‐type spinel product via ex situ ion‐exchanges and a post‐annealing process. Such a layered‐to‐spinel phase conversion is examined using in situ X‐ray diffraction and in situ high‐resolution transmission electron microscopy. It is found that generation of sufficient lithium ion vacancies within the Li‐excess layered oxide plays a critical role for realizing a complete phase transition. The newly formed spinel material exhibits initial discharge capacities of 313.6, 267.2, 204.0, and 126.3 mAh g^?1 when cycled at 0.1, 0.5, 1, and 5 C (1 C = 250 mA g^?1), respectively, and can retain a specific capacity of 197.5 mAh g^?1 at 1 C after 100 electrochemical cycles, demonstrating remarkably improved rate capability and cycling stability in comparison with the original Li‐excess layered cathode materials. This work sheds light on fundamental understanding of phase transitions within Li‐excess layered oxides. It also provides a novel route for tailoring electrochemical performance of Li‐excess layered cathode materials for high‐capacity lithium ion batteries.     

A Metal Organic Framework Derived Solid Electrolyte for Lithium–Sulfur Batteries

Lithium–sulfur batteries (LSBs) are currently considered as promising candidates for next‐generation energy storage technologies. However, their practical application is hindered by the critical issue of the polysulfide‐shuttle. Herein, a metal organic framework (MOF)‐derived solid electrolyte is presented to address it. The MOF solid electrolyte is developed based on a Universitetet i Oslo (UIO) structure. By grafting a lithium sulfonate (‐SO₃Li) group to the UIO ligand, both the ionic conductivity and the polysulfide‐suppression capability of the resulting ‐SO₃Li grafted UIO (UIOSLi) solid electrolyte are greatly improved. After integrating a Li‐based ionic liquid (Li‐IL), lithium bis(trifluoromethanesulfonyl)imide in 1‐ethyl‐3‐methylimidazolium bis(trifluoromethylsulfonyl)imide, the resulting Li‐IL/UIOSLi solid electrolyte exhibits an ionic conductivity of 3.3 × 10^?4 S cm^?1 at room temperature. Based on its unique structure, the Li‐IL/UIOSLi solid electrolyte effectively restrains the polysulfide shuttle and suppresses lithium dendritic growth. Lithium–sulfur cells with the Li‐IL/UIOSLi solid electrolyte and a Li₂S₆ catholyte show stable cycling performance that preserves 84% of the initial capacity after 250 cycles with a capacity‐fade rate of 0.06% per cycle.     

Capture and Catalytic Conversion of Polysulfides by In Situ Built TiO2‐MXene Heterostructures for Lithium–Sulfur Batteries

The detrimental shuttle effect in lithium–sulfur batteries mainly results from the mobility of soluble polysulfide intermediates and their sluggish conversion kinetics. Herein, presented is a multifunctional catalyst with the merits of strong polysulfides adsorption ability, superior polysulfides conversion activity, high specific surface area, and electron conductivity by in situ crafting of the TiO₂‐MXene (Ti₃C₂T_x) heterostructures. The uniformly distributed TiO₂ on MXene sheets act as capturing centers to immobilize polysulfides, the hetero‐interface ensures rapid diffusion of anchored polysulfides from TiO₂ to MXene, and the oxygen‐terminated MXene surface is endowed with high catalytic activity toward polysulfide conversion. The improved lithium–sulfur batteries deliver 800 mAh g^?1 at 2 C and an ultralow capacity decay of 0.028% per cycle over 1000 cycles at 2 C. Even with a high sulfur loading of 5.1 mg cm^?2, the capacity retention of 93% after 200 cycles is still maintained. This work sheds new insights into the design of high‐performance catalysts with manipulated chemical components and tailored surface chemistry to regulate polysulfides in Li–S batteries.     

Suppressed Shuttle via Inhibiting the Formation of Long‐Chain Lithium Polysulfides and Functional Separator for Greatly Improved Lithium–Organosulfur Batteries Performance

The development of lithium–sulfur batteries is limited by the poor conductivity of sulfur cathodes and soluble long‐chain lithium polysulfides (LPSs), which cause the low utilization of sulfur and the aversive shuttle effect, and further, give rise to self‐discharge, rapid reversible capacity fading, and low Coulombic efficiency. In this work, a novel configuration is built for high‐performance lithium–organosulfur batteries, in which the organosulfur hybrid material and lithium metal are used as the cathode and the anode, respectively, and are separated by a functional separator decorated with nitrogen and sulfur co‐doped reduced graphite oxide. The organosulfur in the cathode prevents the shuttle effect by inhibiting the formation of long‐chain LPSs. In addition, the functional separator effectively adsorbs LPSs escaping from the cathode by electrostatic interactions and further restrains the shuttle effect. These effects are confirmed by density‐functional theory calculations. As a result, this novel configuration provides a high initial discharge capacity of 1364 mAh g^?1 at 0.2 C and a high discharge capacity of 750 mAh g^?1 at 1 C after 700 cycles with a very low capacity decay rate of 0.037% per cycle.