Performance Of Lithium-sulfur Batteries Research Articles

Multifunctional Asymmetric Separator Constructed by Polyacrylonitrile-Derived Nanofibers for Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries hold great promise as next-generation high-energy storage devices owing to the high theoretical specific capacity of sulfur, but polysulfide shuttling and lithium dendrite growth remain key challenges limiting cycling life. In this work, we propose a polyacrylonitrile-derived asymmetric (PDA) separator to enhance Li-S battery performance by accelerating sulfur redox kinetics and guiding lithium plating and stripping. A PDA separator was constructed from two layers: the cathode-facing side consists of polyacrylonitrile nanofibers carbonized at 800 °C and doped with titanium nitride, which can achieve rapid polysulfide conversion via electrocatalysis to suppress their shuttling; the anode-facing side consists of polyacrylonitrile oxidized at 280 °C, on which the abundant electronegative groups guide uniform lithium ion plating and stripping. Li-S batteries assembled with the PDA separator exhibited enhanced rate performance, cycling stability, and sulfur utilization, retaining 426 mA h g-1 capacity at 1 C over 1000 cycles and 632 mA h g-1 at 4 C over 200 cycles. Attractively, the PDA separator showed high thermal stability, which could mitigate the risk of internal short circuits and thermal runaway. This work demonstrates an original path to addressing the most critical issues with Li-S batteries.

PEI/Super P Cathode Coating: A Pathway to Superior Lithium–Sulfur Battery Performance

Lithium–sulfur batteries exhibit a high energy density of 2500–2600 Wh/kg with affordability and environmental advantages, positioning them as a promising next-generation energy source. However, the insulating nature of sulfur/Li2S and the rapid capacity fading due to the shuttle effect have hindered their commercialization. In this study, we propose a method to boost the performance of lithium–sulfur batteries by modifying the sulfur cathode with a coating layer composed of polyethyleneimine (PEI) and Super P conductive carbon. The PEI/Super P-modified electrode retained 73% of its discharge capacity after 300 cycles at the 2 C scan rate. The PEI/Super P coated layer effectively adsorbs lithium polysulfides, suppressing the shuttle effect and acting as an auxiliary electrode to facilitate the electrochemical reactions of sulfur/Li2S. We analyzed the PEI/Super P-modified electrodes using symmetric cells, electrochemical impedance spectroscopy, and cyclic voltammetry. The battery manufacturing method presented here is not only cost-effective but also industrially viable due to its compatibility with the roll-to-roll process.

Facile synthesis of MoS2 confined in yolk-shell hollow mesoporous carbon spheres with enhanced polysulfide binding for high-rate Li-S batteries

Lithium-sulfur (Li-S) batteries are one of the most potential energy storage systems because of their high theoretical density, environmental friendliness. However, the practical application of Li-S batteries is currently hampered by several intrinsic problems including the shuttle effects of polysulfides and sluggish electrode reaction kinetics. Herein, a flower-like MoS2 nanosheets confined and in situ grown inside yolk-shell hollow mesoporous carbon spheres (abbreviated as MoS2 @YHMCs) was fabricated as advanced sulfur immobilizer, which can effectively inhibit shuttle effect and conversion of polysulfides. The yolk-shell hollow mesoporous carbon spheres can restrain the volume variation during lithiation-delithiation processes, expose abundant active interfaces and furnish a shortened ion/electron transmission route for facilitated redox reactions. Furthermore, the few layered MoS2 nanosheets have strong LiPS adsorption and catalyzation, thereby achieving rapid redox conversion and enhanced reaction kinetics. Owing to these structural advantages, the delicately-designed MoS2 @S@YHMCs cathode shows good Li-S battery performance, i.e., high initial discharge capacity (1145 mAh g−1), desirable rate capability (770 mAh g−1 at 4 C), and superior cycling performance (583 mAh g−1 after 200 cycles at 1 C), suggesting great application prospects in the development of Li-S batteries.

Dual-atoms iron sites boost the kinetics of reversible conversion of polysulfide for high-performance lithium-sulfur batteries

Atomically dispersed metal catalysts have offered significant potential for accelerating sluggish kinetics of lithium polysulfides conversion and inhibiting the shuttle effect, so as to achieve the long-life cycle and high-rate performance of lithium sulfur batteries. However, the end-on adsorption structure between single metal site and polysulfide limits the adsorption capacity and catalytic activity of single atom catalysts. Here, we construct dual-atoms iron sites on nitrogen doped graphene to serve as highly efficient catalyst for lithium sulfur batteries. As expected, the dual-atoms sites can firmly bind polysulfides by forming double Fe-S bonds between polysulfides and the two adjacent iron atoms. Such double-bond adsorption structure is also favorable for electron transfer and polysulfides activation, resulting in reducing the energy barrier and accelerating the reaction kinetics. As a result, the as-obtained dual-atoms iron catalyst can effectively alleviate the shuttle effect and improve the utilization of active sulfur, thus the batteries present high initial capacity of 1615 mAh g−1 at 0.05 C and long-cycle life with a decay rate per cycle as low as 0.015% at 2C over 1000 cycles.

A Triptycene-Based Layered/Flower-Like 2D Conductive Metal-Organic Framework with 3D Extension as an Electrode for Efficient Li Storage.

2D metal-organic frameworks (2D MOFs) with π conjugation have attracted widespread attention in the field of lithium storage due to their unique electron transfer units and structural characteristics. However, the periodic 2D planar extension structure hides some active sites, which is not conducive to the utilization of its structural advantages. In this work, a series of triptycene-based 2D conductive MOFs (M-DBH, M = Ni, Mn, and Co) with 3D extension structures are constructed by coordinating 9,10-dihydro-9,10-[1,2]benzenoanthracene-2,3,6,7,14,15-hexaol with metal ions to explore their potential applications in lithium-ion and lithium-sulfur batteries. This is the first study in which 2D conductive MOFs with the 3D extended molecule are used as electrode materials for lithium storage. The designed material generates rich active sites through staggered stacking layers and shows excellent performance in lithium-ion and lithium-sulfur batteries. The capacity retention rate of Ni-DBH can reach over 70% after 500 cycles at 0.2 C in lithium-ion batteries, while the capacity of S@Mn-DBH exceeds 305 mAhg-1 after 480 cycles at 0.5 C in lithium-sulfur batteries. Compared with the materials with 2D planar extended structures, the M-DBH electrodes with 3D extended structures in this work exhibit better performance in terms of cycle time and lithium storage capacity.

Heterostructures Regulating Lithium Polysulfides for Advanced Lithium-Sulfur Batteries.

Sluggish reaction kinetics and severe shuttling effect of lithium polysulfides seriously hinder the development of lithium-sulfur batteries. Heterostructures, due to unique properties, have congenital advantages that are difficult to be achieved by single-component materials in regulating lithium polysulfides by efficient catalysis and strong adsorption to solve the problems of poor reaction kinetics and serious shuttling effect of lithium-sulfur batteries. In this review, the principles of heterostructures expediting lithium polysulfides conversion and anchoring lithium polysulfides are detailedly analyzed, and the application of heterostructures as sulfur host, interlayer, and separator modifier to improve the performance of lithium-sulfur batteries is systematically reviewed. Finally, the problems that need to be solved in the future study and application of heterostructures in lithium-sulfur batteries are prospected. This review will provide a valuable reference for the development of heterostructures in advanced lithium-sulfur batteries.

Size Effect for Inhibiting Polysulfides Shuttle in Lithium-Sulfur Batteries.

Itis undeniable that the dissolution of polysulfides is beneficial in speeding up the conversion rate of sulfur in electrochemical reactions. But it also brings the bothersome "shuttle effect".Therefore, if polysulfides can be retained on the cathode side, the efficient utilization of the polysulfides can be guaranteed to achieve the excellent performance of lithium-sulfur batteries. Based on this idea, considerable methods have been developed to inhibit the shuttling of polysulfides. It is necessary to emphasize that no matter which method is used, the solvation mechanism, and existence forms of polysulfides are essential to analyze. Especially, it is important to clarify the sizes of different forms of polysulfides when using the size effect to inhibit the shuttling of polysulfides. In this review, a comprehensive summary and in-depth discussion of the solvation mechanism, the existing forms of polysulfides, and the influencing factors affecting polysulfides species are presented. Meanwhile, the size of diverse polysulfide species is sorted out for the first time. Depending on the size of polysulfides, tactics of using size effect in cathode, separator, and interlayer parts are elaborated. Finally, a design idea of materials pore size is proposed to satisfy the use of size effect to inhibit polysulfides shuttle.

Enhancing performance of lithium-sulfur batteries through porous carbon network integration in carbonized cotton

A novel material, Cporous@CC, has been developed by incorporating a porous conductive network into carbonized cotton (CC). This modification significantly enhances the surface area of the material, increasing it from 29.1 to 163.0 m2 g−1. The introduction of the porous network significantly enhances the connection between carbon fibers, resulting in a substantial improvement in electronic conduction, up to 2–3 times greater than bare CC. To evaluate its potential, Cporous@CC was utilized as a conductive host for the cathode-active material in lithium-sulfur batteries. The battery utilizing Cporous@CC as the cathode host demonstrated a higher initial capacity of 1200 mAh g−1 at 0.2C and exhibited superior rate capability across the range of 0.1C to 1.0C, outperforming the CC-based battery. The factors contributing to the enhanced electrochemical performance of the Cporous@CC cell were further elucidated through the utilization of the galvanostatic intermittent titration technique.

Dual-functional chloropyrazine additives for enhanced performance of lithium-sulfur batteries

The commercialization of lithium-sulfur batteries (LSBs) faces challenges due to uncontrolled lithium deposition and lithium polysulfides (LiPSs) shuttling. In this study, a class of chloropyrazine-based electrolyte additives was introduced to address these issues. The results showed that the presence of chloropyrazine facilitated the formation of a robust and smooth organic-inorganic hybrid solid-electrolyte interface (SEI) enriched with LiCl. This SEI layer enabled reversible lithium plating/stripping, suppressed dendrite growth, and protected the lithium anode from detrimental side reactions with LiPSs. Furthermore, Density functional theory (DFT) results demonstrate that chloropyrazine additives effectively modulated the molecular orbital energy levels of LiPSs and promoted the kinetics of their conversion reactions. LSBs incorporating chloropyrazine additives demonstrated outstanding high-rate performance and long-term cycling stability, with over 800 cycles at 1 C rate and a capacity retention of 81.6 %. Even under challenging conditions of high sulfur loading (5.8 mg cm−2) and low electrolyte-to-sulfur ratio (5 μL mg−1), the battery demonstrated capacity decay rate of only 0.066 % per cycle after 500 cycles at 0.2 C rate. With the highlights of dual-functional chloropyrazine electrolyte additives in improving interfacial chemistry and modulating the orbital energy levels of LiPSs, this work offers a promising direction for advanced electrolyte design in LSBs.

Enhancing the Cycle Performance of Lithium-Sulfur Batteries by Coating the Separator with a Cation-Selective Polymer Layer.

Lithium-sulfur batteries are believed to possess the feasibility to power electric vehicles in the future ascribed to the competitive energy density. However, soluble polysulfides continuously shuttle between the sulfur electrode and lithium anode across the separator, which dramatically impairs the battery's capacity. Herein, the surface of a polypropylene separator (PP film) is successfully modified with a delicately designed cation-selective polymer layer to suppress the transport of polysulfides. In principle, since bis-sulfonimide anions groups on the backbone of the polymer are immobilized, only cations can pass through the polymer layer. Furthermore, plenty of ethoxy chains in the polymer can facilitate lithium-ion mobility. Consequently, in addition to obstructing the movement of negatively charged polysulfides by the electrostatic repulsive force of fixed anions, the coated multi-functional layer on the PP film also guarantees the smooth conduction of lithium ions. The investigations demonstrate that the battery with the pristine PP film only delivers 228.5 mAh g-1 after 300 cycles at 2 C with a high capacity fading rate of 60.9 %. By contrast, the polymer-coated sample can release 409.4 mAh g-1 under the identical test condition and the capacity fading rate sharply declines to 43.2 %, illustrating superior cycle performance.

Modification of separators with neodymium oxide/graphene composite to enhance lithium-sulfur battery performance

Lithium-sulfur (Li–S) batteries have generated significant attention due to their high theoretical specific capacity and energy density among a host of energy storage power devices. Nevertheless, the lithium polysulfide dissolution shuttle that occurs within Li–S batteries will lead to capacity deterioration and inadequate cycling stability. In the paper, we proposed a measure to deal with the above problems by modifying the separator with Nd2O3/graphene composite in Li–S batteries. Graphene's special chemical properties and structural qualities make it an excellent choice for Li–S batteries. Meanwhile, Nd2O3 has a strong binding affinity with lithium polysulfide due to its low electronegativity, which exhibits Lewis's acidity and forms strong interactions with lithium polysulfide, which is strongly Lewis basic. By utilizing these advantageous properties, Li–S batteries assembling Nd2O3-decorated reduced graphite oxide modified polypropylene separators (Nd2O3/RGO/PP) demonstrate outstanding electrochemical performance, including a mere 0.0525% capacity attenuation rate under 2C during 1000 cycles and with exceptional rate performance of 614 mAh/g even at 3C. This study presents valuable knowledge for effectively modifying separators using rare earth oxides to incorporate graphene, ultimately promoting the practical application of Li–S batteries.

High Entropy Sulfide Nanoparticles as Lithium Polysulfide Redox Catalysts.

The polysulfide shuttle contributes to capacity loss in lithium-sulfur batteries, which limits their practical utilization. Materials that catalyze the complex redox reactions responsible for the polysulfide shuttle are emerging, but foundational knowledge that enables catalyst development remains limited with only a small number of catalysts identified. Here, we employ a rigorous electrochemical approach to show quantitatively that the lithium polysulfide redox reaction is catalyzed by nanoparticles of a high entropy sulfide material, Zn0.30Co0.31Cu0.19In0.13Ga0.06S. When 2% by weight of the high entropy sulfide is added to the lithium sulfur cathode composite, the capacity and Coulombic efficiency of the resulting battery are improved at both moderate (0.2 C) and high (1 C) charge/discharge rates. Surface analysis of the high entropy sulfide nanoparticles using X-ray photoelectron spectroscopy provides important insights into how the material evolves during the cycling process. The Zn0.30Co0.31Cu0.19In0.13Ga0.06S nanoparticle catalyst outperformed the constituent metal sulfides, pointing to the role that the high-entropy "cocktail effect" can play in the development of advanced electrocatalytic materials for improved lithium sulfur battery performance.

Correlating Polysulfide Solvation Structure with Electrode Kinetics towards Long-Cycling Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries are promising due to ultrahigh theoretical energy density. However, their cycling lifespan is crucially affected by the electrode kinetics of lithium polysulfides. Herein, the polysulfide solvation structure is correlated with polysulfide electrode kinetics towards long-cycling Li-S batteries. The solvation structure derived from strong solvating power electrolyte induces fast anode kinetics and rapid anode failure, while that derived from weak solvating power electrolyte causes sluggish cathode kinetics and rapid capacity loss. By contrast, the solvation structure derived from medium solvating power electrolyte balances cathode and anode kinetics and improves the cycling performance of Li-S batteries. Li-S coin cells with ultra-thin Li anodes and high-S-loading cathodes deliver 146 cycles and a 338 Wh kg-1 pouch cell undergoes stable 30 cycles. This work clarifies the relationship between polysulfide solvation structure and electrode kinetics and inspires rational electrolyte design for long-cycling Li-S batteries.

Rational design of a functional interlayer to simultaneously suppress lithium polysulfides shuttling and facilitate Li-ion migration for high-performance Li-S battery

Lithium-sulfur (Li-S) battery has been considered to be the most promising next-generation secondary battery system, but the shuttle effect of lithium polysulfides (LiPSs) and sluggish redox kinetics of LiPSs conversion processes still hinder its commercial application. Herein, a honeycomb-like structured and dense layer coated interlayer with Co nanoparticles uniformly dispersed was fabricated via a modified phase inversion method followed by carbonization. This interlayer can suppress the LiPSs shuttling by physically blocking the diffusion of LiPSs and chemically capturing and accelerating the conversion of LiPSs due to the high catalytic activity of Co nanoparticles. Meanwhile, the abundant lithiophilic pyridinic N sites can also facilitate Li+ migration, which further promotes the reaction kinetics of LiPSs conversion. Consequently, the Li-S battery assembled with this interlayer can exhibit an excellent specific capacity of 586.6 mAh/g after 400 cycles at 4.0 C with a low decay rate of 0.10 %. Even when the sulfur loading is elevated to 5.1 mg cm−2, this battery can still maintain the specific capacity of 646.0 mAh/g after 100 cycles at 0.2 C. This work demonstrates the importance and potential of the rational design of interlayer structure and composition in improving the overall Li-S battery performance.

Introduction of UV-cured interpenetrating polymer network in PEO-based all-solid-state Li-S battery

Lithium–sulfur (Li-S) battery attracts numerous study due to its high theoretical specific capacity. Unfortunately, the notorious shuttle effect and the safety issue of lithium anode limit the development. The application of solid-state electrolyte is regarded as one of the solutions. Herein, a UV-cured polymer network is introduced in poly(ethylene oxide) (PEO)-based solid polymer electrolyte (SPE) to enhance the performance of Li-S battery. Poly(ethylene glycol) dimethacrylate (PEGDMA) was used as the main crosslinking monomer. The abundant -C-C-O- long chain can provide a fast channel for Li+ transfer. Trimethylolpropane ethoxylate triacrylate (TMPETA) is used as the crosslinker, which made the linear copolymer formed by single monomer transform into interpenetrating polymer network. Hence, an interpenetrating UV-cured network was synthesized and combined with PEO. This elaborately designed structure enhances the ionic conductivity and the mechanical properties of PEO SPE as well as hinder the lithium polysulfides (LiPSs) migration. As a result, the symmetric Li cells with this SPE can stably cycle for >1600 h at the current density of 0.1 mA cm−2. Moreover, the Li-S cells can deliver an initial capacity of 1131 mAh g−1 at 0.1C. It provides a thread to design the polymer network of SPE.

Investigation of the corrosion behavior influence of carbon interlayer on aluminum collector in lithium-sulfur battery system

Due to the shuttle effect brought by polysulfides, the commercialization of lithium-sulfur batteries still faces significant difficulties. Carbon interlayer is introduced to enhance the electrochemical performance of lithium-sulfur batteries, while the drawback that the interlayer will reversely affect the performance of the current collector was ignored. The current collector has a significant influence and contribution to the cycle stability of lithium-sulfur batteries. In this study, we looked into the electrochemical stability and corrosion situation of standard aluminum foil collectors in lithium-sulfur batteries with carbon interlayer. The results show that the introduction of carbon interlayer into the lithium-sulfur batteries will make aluminum foil and carbon paper form an electronic conduction path and galvanic corrosion occurs, accelerating the corrosion of aluminum foil. Therefore, we propose a new corrosion model. During the cycle, the surface of the aluminum collector becomes a non-dense passivation film and lithium polysulfide terminal (ST−1). Then, under the action of the carbon interlayer, the passivation film peels off and the oxide film is attacked by the electrolyte, thiosulfate and polythionate, resulting in pitting holes and ultimately accelerating the corrosion of the aluminum foil collector. This research has some guiding significance for the commercial application of lithium-sulfur batteries.

Beaded CoSe2-C Nanofibers for High-Performance Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries are regarded as highly promising energy storage devices due to their high theoretical specific capacity and high energy density. Nevertheless, the commercial application of Li-S batteries is still restricted by poor electrochemical performance. Herein, beaded nanofibers (BNFs) consisting of carbon and CoSe2 nanoparticles (CoSe2/C BNFs) were prepared by electrospinning combined with carbonization and selenization. Benefitting from the synergistic effect of physical adsorption and chemical catalysis, the CoSe2/C BNFs can effectively inhibit the shuttle effect of lithium polysulfides and improve the rate performance and cycle stability of Li-S batteries. The three-dimensional conductive network provides a fast electron and ion transport pathway as well as sufficient space for alleviating the volume change. CoSe2 can not only effectively adsorb the lithium polysulfides but also accelerate their conversion reaction. The CoSe2/C BNFs-S cathode has a high reversible discharge specific capacity of 919.2 mAh g-1 at 0.1 C and presents excellent cycle stability with a low-capacity decay rate of 0.05% per cycle for 600 cycles at 1 C. The combination of the beaded carbon nanofibers and polar metal selenides sheds light on designing high-performance sulfur-based cathodes.

(Invited) Modeling the Dependence of the Lithium-Sulfur Battery Performance on the Materials and Cell Design Factors

Lithium-sulfur (Li-S) batteries have attracted significant research interest in the last couple of decades due to their significantly high theoretical specific capacity in addition to the fact that the cathode active material sulfur is abundant and inexpensive and has a high capacity. However, several mechanisms hinder the Li-S battery performance; the depletion of the lithium metal or the electrolyte in the cell with cycling, the polysulfide shuttle mechanism due to the transport of the soluble reaction intermediates between the cathode and the anode, and the passivation of the cathode surface due to the precipitation of the insoluble product Li2S are some examples of these mechanisms that lead to fast capacity fade and thus limited cycle life of the Li-S batteries. As a result of the highly complicated reaction and degradation mechanisms in the cell, the performance of the Li-S battery significantly depends on the materials and cell design. Consequently, it is of significant importance to study this key relation. Herein, we develop electrochemical models to predict the impact of critical materials and cell design parameters: electrolyte-to-sulfur (E/S) ratio, carbon-to-sulfur (C/S) ratio, sulfur loading, and carbon and electrolyte properties, on the Li-S battery performance. We use zero-dimensional (concentration-independent) and one-dimensional (concentration-dependent) models to project the isothermal, constant-current discharge behavior of the Li-S cell. In our models, a novel definition for the electrochemically active area is proposed, which describes the cathode area as a function of the carbon amount and the porosity in the cathode. Experimental trends on the influence of cathode design parameters on the discharge performance are captured successfully. A mechanistic explanation of these trends is offered with the presented model by introducing the proposed electrochemically active area.

MOF-Derived Nitrogen-Doped Porous Carbon Polyhedrons/Carbon Nanotubes Nanocomposite for High-Performance Lithium-Sulfur Batteries.

Nanocomposites that combine porous materials and a continuous conductive skeleton as a sulfur host can improve the performance of lithium-sulfur (Li-S) batteries. Herein, carbon nanotubes (CNTs) anchoring small-size (~40 nm) N-doped porous carbon polyhedrons (S-NCPs/CNTs) are designed and synthesized via annealing the precursor of zeolitic imidazolate framework-8 grown in situ on CNTs (ZIF-8/CNTs). In the nanocomposite, the S-NCPs serve as an efficient host for immobilizing polysulfides through physical adsorption and chemical bonding, while the interleaved CNT networks offer an efficient charge transport environment. Moreover, the S-NCP/CNT composite with great features of a large specific surface area, high pore volume, and short electronic/ion diffusion depth not only demonstrates a high trapping capacity for soluble lithium polysulfides but also offers an efficient charge/mass transport environment, and an effective buffering of volume changes during charge and discharge. As a result, the Li-S batteries based on a S/S-NCP/CNT cathode deliver a high initial capacity of 1213.8 mAh g-1 at a current rate of 0.2 C and a substantial capacity of 1114.2 mAh g-1 after 100 cycles, corresponding to a high-capacity retention of 91.7%. This approach provides a practical research direction for the design of MOF-derived carbon materials in the application of high-performance Li-S batteries.

First‐principles Screening of Transition‐Metal Doped FeS2 As Sulfur Cathode Host for Sulfur Redox Chemistry

AbstractThe sulfur cathode host Fe1‐xMxS2 (M=transition‐metal; x=0, 0.125, and 0.25) for the sulfur redox chemistry is essential to facilitate the fast charge‐discharge kinetics of lithium‐sulfur‐batteries (LSBs). Applying first‐principles calculations, the formation energy, conductivity, work function, charge redistribution, chemical adsorption, and catalytic performance of Fe1‐xMxS2 are systematically investigated. Ti/V‐doped FeS2 has low lattice distortion and formation energy, and facilitates the Li+ diffusion due to charge redistribution. Chemical adsorption for polysulfides (LiPSs) is closely related to d‐band center of Fe1‐xMxS2. Li2S's activation begins with the transfer of electrons from the electron‐rich metal center to the empty orbitals of Li2S. Gibbs free energy change of Li2S4 to Li2S determines the catalytic efficiency. Li2S deposition and decomposition affects the redox kinetics of sulfur. Ti/V‐doped FeS2 has superior conductivity, chemical adsorption, and has low thermodynamic barrier of Li2S deposition. Li2S decomposition tends to occur on Fe0.875Ti0.125S2(001) surface. In general, Ti/V‐doped FeS2, as the host material of the sulfur cathode, is more beneficial to the cycle performance of LSBs. The electrochemical properties of sulfur cathode host materials can be controlled by doping, and can be manipulated and optimized in a certain range through electronic structure and chemical composition design in LSBs.