A Robust,Freestanding MXene‐Sulfur Conductive Paper for Long‐Lifetime Li–S Batteries

Freestanding, robust electrodes with high capacity and long lifetime are of critical importance to the development of advanced lithium–sulfur (Li–S) batteries for next‐generation electronics, whose potential applications are greatly limited by the lithium polysulfide (LiPS) shuttle effect. Solutions to this issue have mostly focused on the design of cathode hosts with a polar, sulfurphilic, conductive network, or the introduction of an extra layer to suppress LiPS shuttling, which either results in complex fabrication procedures or compromises the mechanical flexibility of the device. A robust Ti₃C₂T_x/S conductive paper combining the excellent conductivity, mechanical strength, and unique chemisorption of LiPSs from MXene nanosheets is reported. Importantly, repeated cycling initiates the in situ formation of a thick sulfate complex layer on the MXene surface, which acts as a protective membrane, effectively suppressing the shuttling of LiPSs and improving the utilization of sulfur. Consequently, the Ti₃C₂T_x/S paper exhibits a high capacity and an ultralow capacity decay rate of 0.014% after 1500 cycles, the lowest value reported for Li–S batteries to date. A robust prototype pouch cell and full cell of Ti₃C₂T_x/S paper // lithium foil and prelithiated germanium are also demonstrated. The preliminary results show that Ti₃C₂T_x/S paper holds great promise for future flexible and wearable electronics.     

Enhanced Interfacial Stability of Hybrid‐Electrolyte Lithium‐Sulfur Batteries with a Layer of Multifunctional Polymer with Intrinsic Nanoporosity

The use of lithium‐ion conductive solid electrolytes offers a promising approach to address the polysulfide shuttle and the lithium‐dendrite problems in lithium‐sulfur (Li‐S) batteries. One critical issue with the development of solid‐electrolyte Li‐S batteries is the electrode–electrolyte interfaces. Herein, a strategic approach is presented by employing a thin layer of a polymer with intrinsic nanoporosity (PIN) on a Li⁺‐ion conductive solid electrolyte, which significantly enhances the ionic interfaces between the electrodes and the solid electrolyte. Among the various types of Li⁺‐ion solid electrolytes, NASICON‐type Li_1+xAl_xTi_2‐x(PO₄)₃ (LATP) offers advantages in terms of Li⁺‐ion conductivity, stability in ambient environment, and practical viability. However, LATP is susceptible to reaction with both the Li‐metal anode and polysulfides in Li‐S batteries due to the presence of easily reducible Ti⁴⁺ ions in it. The coating with a thin layer of PIN presented in this study overcomes the above issues. At the negative‐electrode side, the PIN layer prevents the direct contact of Li‐metal with the LATP solid electrolyte, circumventing the reduction of LATP by Li metal. At the positive electrode side, the PIN layer prevents the migration of polysulfides to the surface of LATP, preventing the reduction of LATP by polysulfides.     

Porous Ti4O7 Particles with Interconnected‐Pore Structure as a High‐Efficiency Polysulfide Mediator for Lithium–Sulfur Batteries

Multifunctional Ti₄O₇ particles with interconnected‐pore structure are designed and synthesized using porous poly(styrene‐b ‐2‐vinylpyridine) particles as a template. The particles can work efficiently as a sulfur‐host material for lithium–sulfur batteries. Specifically, the well‐defined porous Ti₄O₇ particles exhibit interconnected pores in the interior and have a high‐surface area of 592 m² g^?1; this shows the advantage of mesopores for encapsulating of sulfur and provides a polar surface for chemical binding with polysulfides to suppress their dissolution. Moreover, in order to improve the conductivity of the electrode, a thin layer of carbon is coated on the Ti₄O₇ surface without destroying its porous structure. The porous Ti₄O₇ and carbon‐coated Ti₄O₇ particles show significantly improved electrochemical performances as cathode materials for Li–S batteries as compared with those of TiO₂ particles.     

Facile Preparation of High‐Content N‐Doped CNT Microspheres for High‐Performance Lithium Storage

Herein, high‐content N‐doped carbon nanotube (CNT) microspheres (HNCMs) are successfully synthesized through simple spray drying and one‐step pyrolysis. HNCM possesses a hierarchically porous architecture and high‐content N‐doping. In particular, HNCM800 (HNCM pyrolyzed at 800 °C) shows high nitrogen content of 12.43 at%. The porous structure derived from well‐interconnected CNTs not only offers a highly conductive network and blocks diffusion of soluble lithium polysulfides (LiPSs) in physical adsorption, but also allows sufficient sulfur infiltration. The incorporation of N‐rich CNTs provides strong chemical immobilization for LiPSs. As a sulfur host for lithium–sulfur batteries, good rate capability and high cycling stability is achieved for HNCM/S cathodes. Particularly, the HNCM800/S cathode delivers a high capacity of 804 mA h g^?1 at 0.5 C after 1000 cycles corresponding to low fading rate (FR) of only 0.011% per cycle. Remarkably, the cathode with high sulfur loading of 6 mg cm^?2 still maintains high cyclic stability (capacity of 555 mA h g^?1 after 1000 cycles, FR 0.038%). Additionally, CNT/Co₃O₄ microspheres are obtained by the oxidation of CNTs/Co in the air. The as‐prepared CNT/Co₃O₄ microspheres are employed as an anode for lithium‐ion batteries and present excellent cycling performance.     

Rational Design of Multifunctional Integrated Host Configuration with Lithiophilicity-Sulfiphilicity toward High-Performance Li–S Full Batteries

High-energy-density Li–S batteries are considered one of the next-generation energy storage systems, but the uncontrolled Li-dendrite growth in Li metal anodes and the shuttling of polysulfides in S cathode severely impede the commercial development of Li–S batteries. Herein, a conductive composite architecture that is made up of bio-derived N-doped porous carbon fiber bundles (N-PCFs) with co-imbedded cobalt and niobium carbide nanoparticles is employed as a multifunctional integrated host for simultaneously addressing the challenges in both Li anodes and S cathodes. The implantation of Co and NbC nanoparticles bestows the N-PCFs matrix with synergistically enhanced degree of graphitization, electrical conductivity, hierarchical porosity, and surface polarization. Theoretical calculations and experimental results show that NbC with specific lithiophilic and sulfiphilic features can synchronously regulate the Li and S electrochemistry by realizing homogeneous lithium deposition with suppressed Li-dendrite growth and exerting catalytic effects for promoting the polysulfide conversion together with fast Li₂S nucleation. Hence, the assembled Li–S full batteries exhibit a superb rate capability (704 mAh g⁻¹ at 5 C) and cycling life (≈82.3% capacity retention after 500 cycles) at a sulfur loading over 3.0 mg cm⁻², as well as high reversible areal capacity (>6.0 mAh cm⁻²) even at a higher sulfur loading of 6.7 mg cm⁻².     

Electrode Design for Lithium–Sulfur Batteries: Problems and Solutions

Pursuit of advanced batteries with high‐energy density is one of the eternal goals for electrochemists. Over the past decades, lithium–sulfur batteries (LSBs) have gained world‐wide popularity due to their high theoretical energy density and cost effectiveness. However, their road to the market is still full of thorns. Apart from the poor electronic conductivity of sulfur‐based cathodes, LSBs involve special multielectron reaction mechanisms associated with active soluble lithium polysulfides intermediates. Accordingly, the electrode design and fabrication protocols of LSBs are different from those of traditional lithium ion batteries. This review is aimed at discussing the electrode design/fabrication protocols of LSBs, especially the current problems on various sulfur‐based cathodes (such as S, Li₂S, Li₂S_x catholyte, organopolysulfides) and corresponding solutions. Different fabrication methods of sulfur‐based cathodes are introduced and their corresponding bullet points to achieve high‐quality cathodes are highlighted. In addition, the challenges and solutions of sulfur‐based cathodes including active material content, mass loading, conductive agent/binder, compaction density, electrolyte/sulfur ratio, and current collector are summarized and rational strategies are refined to address these issues. Finally, the future prospects on sulfur‐based cathodes and LSBs are proposed.     

Highly Stable Lithium−Sulfur Batteries Promised by Siloxene: An Effective Cathode Material to Regulate the Adsorption and Conversion of Polysulfides

Designing an appropriate cathode is still a challenge for lithium–sulfur batteries (LSBs) to overcome the polysulfides shuttling and sluggish redox reactions. Herein, 2D siloxene nanosheets are developed by a rational wet‐chemistry exfoliation approach, from which S@siloxene@graphene (Si/G) hybrids are constructed as cathodes in Li‐S cells. The siloxene possesses corrugated 2D Si backbone with abundant O grafted in Si₆ rings and hydroxyl‐functionalized surface, which can effectively intercept polysulfides via synergistic effects of chemical trapping capability and kinetically enhanced polysulfides conversion. Theoretical analysis further reveals that siloxene can significantly elevate the adsorption energies and lower energy barrier for Li⁺ diffusion. The LSBs assembled with 2D Si/G hybrid cathodes exhibit greatly enhanced rate performance (919, 759, and 646 mAh g^?1 at 4 C with sulfur loading of 1, 2.9, and 4.2 mg cm^?2, respectively) and superb durability (demonstrated by 1000 cycles with an initial capacity of 951 mAh g^?1 and negligible 0.032% decay rate at 1 C with sulfur loading of 4.2 mg cm^?2). It is expected that the study presented here may open up a new vision toward developing high‐performance LSBs with siloxene for practical applications.     

Advanced Lithium–Sulfur Batteries Enabled by a Bio‐Inspired Polysulfide Adsorptive Brush

Issues with the dissolution and diffusion of polysulfides in liquid organic electrolytes hinder the advance of lithium–sulfur batteries for next‐generation energy storage. To trap and re‐utilize the polysulfides without hampering lithium ion conductivity, a bio‐inspired, brush‐like interlayer consisting of zinc oxide (ZnO) nanowires and interconnected conductive frameworks is proposed. The chemical effect of ZnO on capturing polysulfides has been conceptually confirmed, initially by using a commercially available macroporous nickel foam as a conductive backbone, which is then replaced by a free‐standing, ultra‐light micro/mesoporous carbon (C) nanofiber mat for practical application. Having a high sulfur loading of 3 mg cm^?2, the sulfur/multi‐walled carbon nanotube composite cathode with a ZnO/C interlayer exhibits a reversible capacity of 776 mA h g^?1 after 200 cycles at 1C with only 0.05% average capacity loss per cycle. A good cycle performance at a high rate can be mainly attributed to the strong chemical bonding between ZnO and polysulfides, fast electron transfer, and an optimized ion diffusion path arising from a well‐organized nanoarchitecture. These results herald a new approach to advanced lithium–sulfur batteries using brush‐like chemi‐functional interlayers.     

A 3D Hybrid of Chemically Coupled Nickel Sulfide and Hollow Carbon Spheres for High Performance Lithium–Sulfur Batteries

Lithium–sulfur batteries are a promising next‐generation energy storage device owing to their high theoretical capacity and the low cost and abundance of sulfur. However, the low conductivity and loss of active sulfur material during operation greatly limit the rating capabilities and cycling stability of lithium–sulfur batteries. In this work, a unique sulfur host hybrid material comprising nanosized nickel sulfide (NiS) uniformly distributed on 3D carbon hollow spheres (C‐HS) is fabricated using an in situ thermal reduction and sulfidation method. In the hybrid material, the nanosized NiS provides a high adsorption capability for polysulfides and the C‐HS serves as a physical confinement for polysulfides and also a 3D electron transfer pathway. Moreover, NiS has strong chemical coupling with the C‐HS, favoring fast charge transfer and redox kinetics of the sulfur electrode. With a sulfur loading of up to 2.3 mg cm^?2, the hybrid material‐based lithium–sulfur batteries offer a capacity decay as low as 0.013% per cycle and a capacity of 695 mA h g^?1 at 0.5 C after 300 cycles. This unique 3D hybrid material with strong chemical coupling provides a promising sulfur host for high performance lithium–sulfur batteries.     

A Flexible 3D Multifunctional MgO‐Decorated Carbon Foam@CNTs Hybrid as Self‐Supported Cathode for High‐Performance Lithium‐Sulfur Batteries

One of the critical challenges to develop advanced lithium‐sulfur (Li‐S) batteries lies in exploring a high efficient stable sulfur cathode with robust conductive framework and high sulfur loading. Herein, a 3D flexible multifunctional hybrid is rationally constructed consisting of nitrogen‐doped carbon foam@CNTs decorated with ultrafine MgO nanoparticles for the use as advanced current collector. The dense carbon nanotubes uniformly wrapped on the carbon foam skeletons enhance the flexibility and build an interconnected conductive network for rapid ionic/electronic transport. In particular, a synergistic action of MgO nanoparticles and in situ N‐doping significantly suppresses the shuttling effect via enhanced chemisorption of lithium polysulfides. Owing to these merits, the as‐built electrode with an ultrahigh sulfur loading of 14.4 mg cm^?2 manifests a high initial areal capacity of 10.4 mAh cm^?2, still retains 8.8 mAh cm^?2 (612 mAh g^?1 in gravimetric capacity) over 50 cycles. The best cycling performance is achieved upon 800 cycles with an extremely low decay rate of 0.06% at 2 C. Furthermore, a flexible soft‐packaged Li‐S battery is readily assembled, which highlights stable electrochemical characteristics under bending and even folding. This cathode structural design may open up a potential avenue for practical application of high‐sulfur‐loading Li‐S batteries toward flexible energy‐storage devices.     

Copper Sulfide (CuxS) Nanowire‐in‐Carbon Composites Formed from Direct Sulfurization of the Metal‐Organic Framework HKUST‐1 and Their Use as Li‐Ion Battery Cathodes

Li‐ion batteries containing cost‐effective, environmentally benign cathode materials with high specific capacities are in critical demand to deliver the energy density requirements of electric vehicles and next‐generation electronic devices. Here, the phase‐controlled synthesis of copper sulfide (Cu_xS) composites by the temperature‐controlled sulfurization of a prototypal Cu metal‐organic framework (MOF), HKUST‐1 is reported. The tunable formation of different Cu_xS phases within a carbon network represents a simple method for the production of effective composite cathode materials for Li‐ion batteries. A direct link between the sulfurization temperature of the MOF and the resultant Cu_xS phase formed with more Cu‐rich phases favored at higher temperatures is further shown. The Cu_xS/C samples are characterized through X‐ray diffraction (XRD), thermogravimetric analysis (TGA), transmission electron microscopy, and energy dispersive X‐ray spectroscopy (EDX) in addition to testing as Li‐ion cathodes. It is shown that the performance is dependent on both the Cu_xS phase and the crystal morphology with the Cu_1.8S/C‐500 material as a nanowire composite exhibiting the best performance, showing a specific capacity of 220 mAh g^?1 after 200 charge/discharge cycles.     

MXene-Based Anode-Free Magnesium Metal Battery

Rechargeable magnesium batteries (RMBs) are promising next-generation low-cost and high-energy devices. Among all RMBs, anode-free magnesium metal batteries that use in situ magnesium-plated current collectors as negative electrodes can afford optimal energy densities. However, anode-free magnesium metal batteries have remained elusive so far, as their practical application is plagued by low Mg plating/stripping efficiency due to nonuniform Mg deposition on conventional anode current collectors. Herein, for the first time, an anode-free Mg-metal battery is developed by employing a 3D MXene (Ti₃C₂T_x) film with horizontal Mg electrodeposition. The magnesiophilic oxygen and reactive fluorine terminations in MXene enable an enriched local magnesium-ion concentration and a durable magnesium fluoride-rich solid electrolyte interphase on the Ti₃C₂T_x film surface. Meanwhile, Ti₃C₂T_x MXene exhibits a high lattice geometrical fit with Mg (≈96%) to guide the horizontal electrodeposition of Mg. Consequently, the developed Ti₃C₂T_x film achieves reversible Mg plating/stripping with high Coulombic efficiencies (>99.4%) at high-current-density (5.0 mA cm⁻²) and high-Mg-utilization (50%) conditions. When this Ti₃C₂T_x film is coupled with a pre-magnesized Mo₆S₈ cathode, the anode-free Mg-metal full-cell prototype exhibits a volumetric energy density five times higher than its standard Mg-metal counterpart. This work provides insights into the rational design of anode current collectors to guide horizontal Mg electrodeposition for anode-free Mg metal batteries.     

Ferromagnetic Nanoparticle–Assisted Polysulfide Trapping for Enhanced Lithium–Sulfur Batteries

The lithium–sulfur (Li–S) battery is a promising candidate for next‐generation high‐density energy storage devices because of its ultrahigh theoretical energy density and the natural abundance of sulfur. However, the practical performance of the sulfur cathode is plagued by fast capacity decay and poor cycle life, both of which can be attributed to the intrinsic dissolution/shuttling of lithium polysulfides. Here, a new built‐in magnetic field–enhanced polysulfide trapping mechanism is discovered by introducing ferromagnetic iron/iron carbide (Fe/Fe₃C) nanoparticles with a graphene shell (Fe/Fe₃C/graphene) onto a flexible activated cotton textile (ACT) fiber to prepare the ACT@Fe/Fe₃C/graphene sulfur host. The novel trapping mechanism is demonstrated by significant differences in the diffusion behavior of polysulfides in a custom‐designed liquid cell compared to a pure ACT/S cathode. Furthermore, a cell assembled using the ACT@Fe/Fe₃C/S cathode exhibits a high initial discharge capacity of ≈764 mAh g^?1, excellent rate performance, and a remarkably long lifespan of 600 cycles using ACT@Fe/Fe₃C/S (whereas only 100 cycles can be achieved using pure ACT/S). The new magnetic field–enhanced trapping mechanism provides not only novel insight but unveils new possibilities for mitigating the “shuttle effect” of polysulfides thereby promoting the practical applications of Li–S batteries.     

Nitrogen‐Doped Mesoporous Carbon Promoted Chemical Adsorption of Sulfur and Fabrication of High‐Areal‐Capacity Sulfur Cathode with Exceptional Cycling Stability for Lithium‐Sulfur Batteries

As one important component of sulfur cathodes, the carbon host plays a key role in the electrochemical performance of lithium‐sulfur (Li‐S) batteries. In this paper, a mesoporous nitrogen‐doped carbon (MPNC)‐sulfur nanocomposite is reported as a novel cathode for advanced Li‐S batteries. The nitrogen doping in the MPNC material can effectively promote chemical adsorption between sulfur atoms and oxygen functional groups on the carbon, as verified by X‐ray absorption near edge structure spectroscopy, and the mechanism by which nitrogen enables the behavior is further revealed by density functional theory calculations. Based on the advantages of the porous structure and nitrogen doping, the MPNC‐sulfur cathodes show excellent cycling stability (95% retention within 100 cycles) at a high current density of 0.7 mAh cm^‐2 with a high sulfur loading (4.2 mg S cm^‐2) and a sulfur content (70 wt%). A high areal capacity (≈3.3 mAh cm^‐2) is demonstrated by using the novel cathode, which is crucial for the practical application of Li‐S batteries. It is believed that the important role of nitrogen doping promoted chemical adsorption can be extended for development of other high performance carbon‐sulfur composite cathodes for Li‐S batteries.     

Confined Sulfur in Microporous Carbon Renders Superior Cycling Stability in Li/S Batteries

The use of sulfur in the next generation Li‐ion batteries is currently precluded by its poor cycling stability caused by irreversible Li₂S formation and the dissolution of soluble polysulfides in organic electrolytes that leads to parasitic cell reactions. Here, a new C/S cathode material comprising short‐chain sulfur species (predominately S₂) confined in carbonaceous subnanometer and the unique charge mechanism for the subnano‐entrapped S₂ cathodes are reported. The first charge–discharge cycle of the C/S cathode in the carbonate electrolyte forms a new type of thiocarbonate‐like solid electrolyte interphase (SEI). The SEI coated C/S cathode stably delivers ≈600 mAh g^?1 capacity over 4020 cycles (0.0014% loss cycle^?1) at ≈100% Coulombic efficiency. Extensive X‐ray photoelectron spectroscopy analysis of the discharged cathodes shows a new type of S₂ species and a new carbide‐like species simultaneously, and both peaks disappear upon charging. These data suggest a new sulfur redox mechanism involving a separated Li⁺/S^2? ion couple that precludes Li₂S compound formation and prevents the dissolution of soluble sulfur anions. This new charge/discharge process leads to remarkable cycling stability and reversibility.     

Mechanisms of the Planar Growth of Lithium Metal Enabled by the 2D Lattice Confinement from a Ti3C2Tx MXene Intermediate Layer

The propensity of Li to form irregular and nonplanar electrodeposits has become a fundamental barrier for fabricating Li metal batteries. Here, a planar, dendrite-free Li metal growth on 2D Ti₃C₂T_x MXene is reported. Ab initio calculations suggest that Li forms a hexagonal close-packed (hcp) layer on the surface of Ti₃C₂T_x via ionic bonding and the lattice confinement. The ionic bonding weakens gradually after a few monolayers, resulting in a nanometers-thin transition region of hcp-Li. Above this transition region, the deposition is dominated by plating of body-centered cubic (bcc) Li via metallic bonding. Formation of a dense and planar Li metal anode with preferential growth along the (110) facet is explained by the lattice matching between Ti₃C₂T_x and hcp-Li and then with bcc-Li, as well as preferred thermodynamic factors including the large dendrite formation energy and small migration barrier for Li. The prepared Li metal anode shows stable cycling in a wide current density range from 0.5 to 10.0 mA cm^–2. The LiFePO₄‖Li full cell fabricated with this Li metal anode exhibits only 9.5% capacity fading after 500 charge–discharge cycles at 1 C rate.     

Lamellar MXene Composite Aerogels with Sandwiched Carbon Nanotubes Enable Stable Lithium–Sulfur Batteries with a High Sulfur Loading

Realizing long cycling stability under a high sulfur loading is an essential requirement for the practical use of lithium–sulfur (Li–S) batteries. Here, a lamellar aerogel composed of Ti₃C₂T_x MXene/carbon nanotube (CNT) sandwiches is prepared by unidirectional freeze-drying to boost the cycling stability of high sulfur loading batteries. The produced materials are denoted parallel-aligned MXene/CNT (PA-MXene/CNT) due to the unique parallel-aligned structure. The lamellae of MXene/CNT/MXene sandwich form multiple physical barriers, coupled with chemical trapping and catalytic activity of MXenes, effectively suppressing lithium polysulfide (LiPS) shuttling under high sulfur loading, and more importantly, substantially improving the LiPS confinement ability of 3D hosts free of micro- and mesopores. The assembled Li–S battery delivers a high capacity of 712 mAh g⁻¹ with a sulfur loading of 7 mg cm⁻², and a superior cycling stability with 0.025% capacity decay per cycle over 800 cycles at 0.5 C. Even with sulfur loading of 10 mg cm⁻², a high areal capacity of above 6 mAh cm⁻² is obtained after 300 cycles. This work presents a typical example for the rational design of a high sulfur loading host, which is critical for the practical use of Li–S batteries     

Natural Vermiculite Enables High‐Performance in Lithium–Sulfur Batteries via Electrical Double Layer Effects

Lithium–sulfur batteries with potentially high specific energy are viewed as very promising candidates for next‐generation lightweight and low‐cost rechargeable batteries. However, sulfur‐based cathodes suffer from dissolution of polysulfides causing shuttle effects. Here, in order to confine elemental sulfur and anchor the polysulfides, a novel host that is an inexpensive natural clay mineral, viz., vermiculite is proposed. When compared to regular carbon–sulfur composites, vermiculite–sulfur composites offer promising rate capability and much better cycling stabilities, displaying capacity retentions of ≈89 and ≈93% within 200 cycles at C/2 and 1 C, respectively, and ≈60 % at C/5 within 1000 cycles. Postmortem studies, advanced adsorption tests, density functional theory calculations, and zeta potential measurements in combination with intrinsic characteristics of the natural vermiculite provide insights into the new mechanism. The vermiculite contains naturally present surface cations which show a strong tendency to adsorb S_n^2? anions, hence protecting them from dissolution. The excess surface charge is most probably compensated by excess Li⁺ in the space charge zones which is beneficial for charge transfer and local conductivity. The reported results show that natural clay‐minerals are promising sulfur hosts being able to fixate sulfides via electrical double layer effects, thus enabling high‐performance in lithium–chalcogen batteries.     

Combined Defect and Heterojunction Engineering in ZnTe/CoTe2@NC Sulfur Hosts Toward Robust Lithium–Sulfur Batteries

Lithium–sulfur batteries (LSBs) are feasible candidates for the next generation of energy storage devices, but the shuttle effect of lithium polysulfides (LiPSs) and the poor electrical conductivity of sulfur and lithium sulfides limit their application. Herein, a sulfur host based on nitrogen-doped carbon (NC) coated with small amount of a transition metal telluride (TMT) catalyst is proposed to overcome these limitations. The properties of the sulfur redox catalyst are tuned by adjusting the anion vacancy concentration and engineering a ZnTe/CoTe₂ heterostructures. Theoretical calculations and experimental data demonstrate that tellurium vacancies enhance the adsorption of LiPSs, while the formed TMT/TMT and TMT/C heterostructures as well as the overall architecture of the composite simultaneously provide high Li⁺ diffusion and fast electron transport. As a result, v-ZnTe/CoTe₂@NC/S sulfur cathodes show excellent initial capacities up to 1608 mA h g⁻¹ at 0.1C and stable cycling with an average capacity decay rate of 0.022% per cycle at 1C during 500 cycles. Even at a high sulfur loading of 5.4 mg cm^–2, a high capacity of 1273 mA h g⁻¹ at 0.1C is retained, and when reducing the electrolyte to 7.5 µL mg⁻¹, v-ZnTe/CoTe₂@NC/S still maintains a capacity of 890.8 mA h g⁻¹ after 100 cycles at 0.1C.     

All‐Purpose Electrode Design of Flexible Conductive Scaffold toward High‐Performance Li–S Batteries

The main obstacles that hinder the development of efficient lithium sulfur (Li–S) batteries are the polysulfide shuttling effect in sulfur cathode and the uncontrollable growth of dendritic Li in the anode. An all‐purpose flexible electrode that can be used both in sulfur cathode and Li metal anode is reported, and its application in wearable and portable storage electronic devices is demonstrated. The flexible electrode consists of a bimetallic CoNi nanoparticle‐embedded porous conductive scaffold with multiple Co/Ni‐N active sites (CoNi@PNCFs). Both experimental and theoretical analysis show that, when used as the cathode, the CoNi and Co/Ni‐N active sites implanted on the porous CoNi@PNCFs significantly promote chemical immobilization toward soluble lithium polysulfides and their rapid conversion into insoluble Li₂S, and therefore effectively mitigates the polysulfide shuttling effect. Additionally, a 3D matrix constructed with porous carbonous skeleton and multiple active centers successfully induces homogenous Li growth, realizing a dendrite‐free Li metal anode. A Li–S battery assembled with S/CoNi@PNCFs cathode and Li/CoNi@PNCFs anode exhibits a high reversible specific capacity of 785 mAh g^?1 and long cycle performance at 5 C (capacity fading rate of 0.016% over 1500 cycles).