Lithium Polysulfides Research Articles

Defect-riched prussian blue analogues with superior adsorption-catalysis toward lithium polysulfides for high performance lithium-sulfur batteries

Lithium‑sulfur batteries (LiS) garner significant interest within the energy storage industry, because of their exceptional theoretical energy density coupled with employment of environmental materials. Nevertheless, the broader implementation of LiS batteries faces challenges, primarily due to the lithium polysulfide (LiPSs) shuttle effect and the sluggish conversion kinetics associated with LiPSs. In this work, we introduce a reduction-induced dissolution process to fabricate a mesoporous CoFePB rich in crystal defects via a facile solvothermal method. The experimental results indicate that the abundance of crystal defects originate from the phase transition from Co3[FeIII(CN)6]2 to Co2[FeII(CN)6]. The subsequent adsorption tests and electrochemical evaluations have shown that the defect-rich CoFePB possesses enhanced LiPSs absorption capacity and improved cycling performance in contrast to the pristine CoFePB, which is primarily ascribed to proliferation of active sites emerging as a result of the crystal defects. Consequently, the D-CoFePB-S cathode demonstrates remarkable rate performance with 583 mAh g−1 at a substantial 5C current rate, superior long-term stability with capacity retention of 64.3 % over 2000 cycles at current rate of 2C and outstanding areal capacity of 4.9 mAh cm−2 at 0.1C, even under a substantial sulfur loading of 5.0 mg cm−2.

A Review of Advances in Heterostructured Catalysts for Li-S Batteries: Structural Design and Mechanism Analysis.

Lithium-sulfur (Li-S) batteries, acclaimed for their high energy density, cost-effectiveness, and environmental benefits, are widely considered as a leading candidate for the next-generation energy storage systems. However, their commercialization is impeded by critical challenges, such as the shuttle effect of lithium polysulfides and sluggish reaction kinetics. These issues can be effectively mitigated through the design of heterojunction catalysts. Despite the remarkable advancements in this field, a comprehensive elucidation of the underlying mechanisms and structure-performance relationships of heterojunction catalysts in sulfur electrocatalysis systems remains conspicuously absent. Here, it is expounded upon the mechanisms underlying heterostructure engineering in Li-S batteries and the latest advancements in heterostructure catalysts guided by these multifarious mechanisms are examined. Furthermore, it illuminates groundbreaking paradigms in heterostructure design, encompassing the realms of composition, structure, function, and application. Finally, the research trends and future development directions for the novel heterojunction materials are extensively deliberated. This study not only provides a comprehensive and profound understanding of heterostructure catalysts in Li-S batteries but also facilitates the exploration of new electrocatalyst systems.

Multifunctional Ultrathin Ti3C2Tx MXene@CuCo2O4 /PE Separator for Ultra-High-Energy-Density and Large-Capacity Lithium-Sulfur Pouch Cells.

The shuttling of lithium polysulfides (LiPSs), sluggish reaction kinetics, and uncontrolled lithium deposition/stripping remain the main challenges in lithium-sulfur batteries (LSBs), which are aggravated under practical working conditions, i.e., high sulfur loading and lean electrolyte in large-capacity pouch cells. This study introduces a Ti3C2Tx MXene@CuCo2O4 (MCC) composite on a polyethylene (PE) separator to construct an ultrathin MXene@CuCo2O4/PE (MCCP) film. The MCCP functional separator can deliver superior LiPSs adsorption/catalysis capabilities via the MCC composite and regulate the Li+ deposition through a conductive Ti3C2Tx MXene framework, enhancing redox kinetics and cycling lifetime. When paired with sulfur/carbon (S/C) cathode and lithium metal anode, the resultant 10 Ah-level pouch cell with the ultrathin MCCP separator achieves an energy density of 417Wh kg-1 based on the whole cell and a stable running of 100 cycles under practical operation conditions (cathode loading = 10.0 mg cm-2, negative/positive areal capacity ratio (N/P ratio) = 2, and electrolyte/sulfur weight ratio (E/S ratio) = 2.6 µL mg-1). Furthermore, through a systematic evaluation of the as-prepared Li-S pouch cell, the study unveils the operational and failure mechanisms of LSBs under practical conditions. The achievement of ultrahigh energy density in such a large-capacity lithium-sulfur pouch cell will accelerate the commercialization of LSBs.

Hierarchical van der Waals heterostructure with dual-defect sites for bidirectionally catalyzing Li2S nucleation and decomposition in lithium-sulfur batteries

The lithium‑sulfur batteries hold a promising option for the next generation of energy storage systems. Nevertheless, the shuttle effect of soluble lithium polysulfides and their slow reaction kinetics lead to extremely low efficiency and poor stability, thereby limiting the commercial viability of lithium‑sulfur batteries. Herein, MoSe2/Ti3C2 van der Waals heterostructure is synthesized with a dual-defect strategy, and its electrocatalytic performance is further improved through solution coating treatment (SCT), which involves the addition of glucose during the hydrothermal process. The conductive Ti3C2 scaffold effectively inhibits the aggregation of MoSe2 nanoflakes, thereby validating a larger active surface area. Meanwhile, the nitrogen dopant and selenium vacancy dual-defects in MoSe2 provide abundant active sites for anchoring polysulfides and catalyzing their conversion. As a result, the synergistic interaction between MoSe2 and Ti3C2 bidirectionally catalyzes the Li2S nucleation and decomposition through a heterointerface effect. The lithium‑sulfur battery equipped with MoSe2/Ti3C2-SCT heterostructure modified separator exhibits outstanding discharge specific capacity of 1496.9 mAh g−1 at 0.1C, and a low decay rate per cycle of 0.059 % after 500 cycles at 1C. The discharge specific capacity recovers to 89.3 % of the initial capacity when the current density is decreased from 5C to 0.1C. This work highlights the potential of defect engineering in transition metal selenides to enhance the performance of lithium‑sulfur batteries. It offers a new approach to designing composite electrocatalysts for high-performance lithium‑sulfur batteries.

Regulating the electronic modulation configuration of MnxFeCoNiCu high entropy alloy for reliable sulfur redox kinetics

Current research on sulfur redox catalysis primarily focuses on the adsorption and catalytic conversion of lithium polysulfides (LiPSs). However, it often neglecting the modulation of the catalysts' electronic structure, which includes charge transfer and orbital interactions that significantly affect adsorption and catalytic properties. In this work, multi-channel carbon nanotubes modified with high entropy alloy nanoparticles (MnxFeCoNiCu/MCCFs) are elaborately synthesized as hosts to reveal the relationship between the catalytic activity and surface electronic configuration for reliable sulfur electrochemistry. Combining density functional theory (DFT) calculations with detailed experimental investigations, we demonstrate that modulating the electron consumption center of this intrinsic electron transfer-replenishment mechanism, the surface charge distribution is reestablished, thereby improving the performance of multi-electron reactions. Achieving a balance between adsorption and desorption significantly enhance the catalytic efficiency for LiPSs conversion. Consequently, the as-prepared Mn1.00/MCCFs with an optimized electronic structure as sulfur host can deliver a high capacity of 938 mAh g−1, corresponding to an ultralow capacity decay of 0.013 % per cycle over 500 cycles at 1.0 C.

Cyclodextrin Metal-Organic Framework Functionalized Carbon Materials with Optimized Interface Electronics and Selective Supramolecular Channels for High-Performance Lithium-Sulfur Batteries.

During the reaction process in lithium-sulfur batteries, Lewis acidic lithium polysulfides (LiPSs) affect ion distribution and overall electrolyte stability, degrading battery performance and product distribution (e.g., Li2S). Here, a microenvironment regulation strategy with optimized interface electronics and selective supramolecular channels, is proposed to enhance LiPS reaction kinetics through Lewis basic γ-cyclodextrin metal-organic framework (γ-CDMOF). To validate this concept, γ-CDMOF is rapidly synthesized on 3D graphene foam (GF) via a microwave-assisted method, resulting in a γ-CDMOF/GF cathode for high-performance Li-S batteries. A range of analytical techniques combined with density functional theory (DFT) calculations confirm that introducing a Lewis basic supramolecular microenvironment mitigates the LiPSs shuttle effect, enhances polysulfide capture, and improves sulfur redox conversion. Additionally, COMSOL simulations reveal that the γ-CDMOF framework and oxygen sites significantly reduce volumetric expansion stress during the LiPS solid-liquid phase transition. Impressively, the γ-CDMOF/GF cathode exhibits exceptional performance, including a high specific capacity (1253.01 mAh g⁻¹ at 0.1C), excellent rate performance (589.68 mAh g⁻¹ at 5C), and long cycle life (over 1200 cycles). This study introduces a new concept of supramolecular microenvironment regulation and interfacial interaction strategy, offering a unique approach for the development of multifunctional electrode materials.

Incorporation of Fe/FeOx Nanoparticles into Interlinked N-Doped Porous Carbon Nanofiber Networks to Realizing Sequential Catalytic Conversion of Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries (LSBs) with energy density (2600 Wh/kg) much higher than typical Li-ion batteries (150-300 Wh/kg) have received considerable attention. However, the insulation nature of solid sulfur species and the high activation barrier of lithium polysulfides (LiPSs) lead to slow sulfur redox kinetics. By the introduction of catalytic materials, the effective adsorption of LiPSs, and significantly reduced conversion, energy barriers are expected to be achieved, thereby sharpening electrochemical reaction kinetics and fundamentally addressing these challenges. In this work, a multifunctional catalyst consisting of highly dispersed heterostructure Fe-Fe2O3 nanoparticles was synthesized and introduced to the LSB. Experimental and theoretical analyses revealed that the spontaneous interfacial charge redistribution, resulting in moderate polysulfide adsorption, facilitates the transfer of polysulfides and diffusion of electrons at heterogeneous interfaces. This catalyst achieves sequential catalytic processes on polysulfides with different components. Furthermore, the reduced conversion energy barriers enhanced the catalytic activity of Fe/Fe2O3-NG for expediting LiPS conversion. Consequently, the battery exhibited long-term stability for 300 cycles with 0.03% capacity decay per cycle at 5C. This work provides in-depth insight into the fundamental design principles of effective catalysts for LSBs.

Rational Design of Two-Dimensional MA2Z4 Monolayers as Effective Anchoring Materials for Lithium-Sulfur Batteries.

Advances in lithium-sulfur batteries (LSBs) are impeded by the inefficiency of anchoring materials in facilitating long-term cycling and rate performance. To address this challenge, an exploration of two-dimensional MA2Z4 monolayers as potential anchoring materials for LSBs is proposed based on density functional theory calculations and machine learning (ML) techniques. Adsorption features, sulfur reduction reaction behaviors, and solvent interactions are assessed and analyzed; and MoGe2N4 and WGe2N4 are identified as the most promising candidates because they have optimal adsorption energies for lithium polysulfides to suppress the shuttle effect and exhibit enhanced catalytic activity. Meanwhile, ML analysis highlights the critical influence of the electronegativity of element Z in MA2Z4 on anchoring properties, providing valuable insights into future anchoring material design for high-performance LSBs.

Doped germanene as anchoring material for lithium polysulfides for Li-S batteries: A DFT study

Lithium-sulfur batteries face significant challenges due to the dissolution of lithium polysulfides (LiPSs), commonly known as the shuttle effect, which leads to a loss in charge capacity. This study uses density functional theory (DFT) calculations, with van der Waals corrections, to investigate the polysulfide anchoring potential of a boron-doped germanene monolayer (B-2DGe). The results show that the adsorption energies of LiPSs on B-2DGe range from 1.46 to 3.39 eV. Furthermore, all LiPSs on B-2DGe exhibit conductive behavior. These findings suggest that B-2DGe, as a LiPS substrate, reduces the shuttle effect and prevents polysulfide agglomeration at electrodes, improving the performance of Li-S batteries.

NiCo alloy-decorated nitrogen-doped carbon double-shelled hollow polyhedrons with abundant catalytic active sites to accelerate lithium polysulfides conversion

Lithium-sulfur (Li-S) batteries have received significant attention due to their high theoretical energy density. However, the inherent poor conductivity of S and lithium sulfide (Li2S), coupled with the detrimental shuttle effect induced by lithium polysulfides (LiPSs), impedes their commercialization. In this study, we develop NiCo alloy-decorated nitrogen-doped carbon double-shelled hollow polyhedrons (NC/NiCo DSHPs) as highly efficient catalysts for Li-S batteries. The distribution of NiCo alloy on both the inner and outer shells provides abundant catalytic active sites, effectively adsorbing LiPSs, mitigating the shuttle effect, and promoting the conversion between LiPSs and Li2S, even at high sulfur loadings. This results in enhanced redox kinetics within the Li-S system. Moreover, the highly conductive carbon material framework, enriched with carbon nanotubes and graphitic carbon layers, can greatly promote the efficient electron transportation. Additionally, the improved ion diffusion rates benefiting from the hollow structure can also be realized. By harnessing these synergistic effects, Li-S batteries incorporating the double-shelled NC/NiCo DSHP catalysts achieved a high specific capacity of 1310 mAh/g at 0.2C and a superior rate performance of 621 mAh/g at 4C. Furthermore, excellent cycling performance with ultralow capacity fading rate of only 0.045 % per cycle after 800 cycles at 1C was achieved. When sulfur loading reaches 6 mg cm−2, a high capacity of 4.6 mAh cm−2 at 0.1C after 100 cycles further validates the practical potential of this design. This study presents an innovative approach to alloy catalyst design, offering valuable insights for future research of Li-S batteries.

Dual-Functional SnO2-CNT-PANI||PP||SnO2 Separator for Enhanced Lithium-Sulfur Battery Stability and Capacity

Lithium-sulfur batteries (LSBs) provide high capacity and energy density for advanced energy storage but encounter performance and safety issues due to lithium polysulfides (LiPSs) dissolution and dendrite formation. This study introduces a dual-functional SnO2-CNT-PANI||PP||SnO2 separator (DF-SNCPS) aimed at improving the stability and safety of LSBs. The separator includes a SnO2-CNT-PANI layer on the sulfur cathode side for enhanced electrical conductivity and polysulfide adsorption and a SnO2 nanoparticle (nano-SnO2) layer on the lithium anode side to regulate lithium-ion concentration and inhibit dendrite growth. Density functional theory (DFT) and the phase field method have verified the relevant material's catalytic performance and dendrite suppression ability. These methods have provided a comprehensive understanding of the underlying mechanisms, providing auxiliary explanations for their role in catalyzing polysulfide conversion and suppressing lithium dendrite growth. This innovative design mitigates the shuttle effect and enhances cyclic stability and sulfur utilization, achieving a notable cyclic performance with a capacity retention of 0.05% per cycle over 800 cycles at 1C. The synergistic effects of the modified separator present a viable pathway for LSB commercialization.

Enhanced lithium-sulfur battery eilectrochemistry via Se-doped MoS2/rGO ultrathin sheets as sulfur hosts

In the pursuit of advancing lithium-sulfur (Li-S) battery technology, the intrinsic challenges of sulfur conductivity and the shuttle effect during charge-discharge cycles have posed significant barriers. Despite many efforts made through physical and chemical methodologies, the development of host materials with more active sites and good catalytic activities might still remain a challenging problem in Li-S batteries. This study presents a novel selenium-doped molybdenum disulfide (Se-MoS2) nanosheet, synthesized on reduced graphene oxide (rGO), which would address these issues. The Se-MoS2/rGO composite enhances conductivity and catalytic activity through the creation of anionic vacancies, facilitating lithium polysulfide adsorption. As a sulfur host, this material delivers an impressive initial capacity of 1008.1 mAh g−1 at 1C, maintaining 620.7 mAh g−1 after 500 cycles with a minimal capacity fade of 0.077 % per cycle, demonstrating superior coulombic efficiency and stability. The findings underscore the impact of heteroatom doping on the electrochemical performance of graphene-based materials for Li-S batteries.

High-entropy sulfides enhancing adsorption and catalytic conversion of lithium polysulfides for lithium-sulfur batteries

High-entropy sulfides enhancing adsorption and catalytic conversion of lithium polysulfides for lithium-sulfur batteries

Copper-nickel MOF-coated electrospun polyacrylonitrile membranes for Li–S batteries: Mitigating the shuttle effect and enhancing stability

Cu–Ni MOF nanoparticles were synthesized as coating materials for lithium–sulfur battery membranes, and the performance of batteries employing Cu–Ni MOF/PAN (CNMP) electrospinning membranes were examined. The modified membrane efficiently suppresses the shuttle effect, leveraging the synergistic catalysis and adsorption capabilities of the Cu–Ni MOF nanoparticles. The modified membrane exhibited relatively high porosity and outstanding electrolyte absorption capacity. The CNMP membrane battery demonstrated a remarkable first-cycle discharge capacity of 1529 mA h g⁻¹. The battery maintained an exceptional discharge capacity with 85.2 % retention and a minimal capacity decay rate of just 0.074 % per cycle after 200 cycles at 0.5 C. The capacity retention of the modified membrane battery remained at 74.6 % even after 2000 cycles at 2 C. The excellent performance of the modified membrane battery was due to the physical entrapment and strong chemical adsorption of lithium polysulfides by Cu–Ni MOF nanoparticles, significantly preventing the shuttle effect and facilitating rapid oxidation–reduction kinetics based on strong catalytic conversion.

Synergistic Interaction of Strongly Polar Zinc Selenide and Highly Conductive Carbon Nanoframeworks Accelerates Redox Kinetics of Polysulfides.

Lithium-sulfur batteries (LSBs) have become strong competitors in secondary battery systems because of their superior theoretical capacity and energy density. However, due to the serious shuttle effect of soluble long-chain lithium polysulfides (LiPSs) and the slow solid-solid reaction kinetics, LSBs face some specific challenges, such as a short cycle life and low rate performance. The introduction of selenide/carbon composites derived from zeolite imidazolate frameworks (ZIFs) into separator coatings is a direct and effective solution to the aforementioned problems. Here, a zinc selenide/carbon catalyst material (ZnSe@C) was constructed and employed to modify commercial polypropylene (PP) separators to accelerate the conversion of intermediates. The highly polar ZnSe effectively fixes the active material on the cathode side by transferring electrons between elements with LiPSs and improves the utilization rate of sulfur. Concurrently, the highly conductive carbon nanoskeleton generated following the pyrolysis of ZIF-8 ensures the rapid transfer of charges during the catalytic reaction. The prepared ZnSe@C has a large specific surface area (250.07 m2 g-1) and mesoporous ratio (78.03%), which not only enhances adsorption and catalysis but also promotes the penetration of the electrolyte and the transport of Li+. Based on this, ZnSe@C/PP separator cells exhibit a low average capacity decay rate of 0.051% per cycle after 500 cycles at 1 C.

Review on polymer electrolytes for lithium‐sulfurized polyacrylonitrile batteries

AbstractLithium‐sulfur (Li‐S) batteries are deemed as the next generation of energy storage devices due to high theoretical specific capacity (1675 mAh g−1) and energy density (2600 Wh kg−1). However, the commercial application has always been constrained by lithium polysulfide (LiPSs) shuttling effects and still has a long way to go. Sulfurized polyacrylonitrile (SPAN) is a promising alternative candidate to replace traditional sulfur cathode and is conducive to eliminating LiPSs by realizing “solid‐solid” direct conversion in conventional carbonate electrolytes. However, an over 25% irreversible capacity loss is exhibited inevitably in the first discharge process, the inherent structure of SPAN and the related reaction mechanism remain unclear. In this review, the structure characteristics and electrochemical behaviors of SPAN are summarized for better interpreting current knowledge and favoring the design of high performance materials. In the past few decades, many problems in traditional Li‐S batteries have been solved by improving electrolytes. Polymer electrolytes (PEs) have been widely used due to structural designability, multi‐functionality, exceptional chemical stability, and excellent processability. Surprisingly, the relevant researches on PEs compatible with SPAN remains limited currently. Therefore, the recent modification strategies of gel polymer electrolytes and solid polymer electrolytes in Li‐SPAN batteries are introduced in terms of Li+ transfer and interface engineering, the design principles are concluded, the specific challenges encountered by polymer‐based electrolytes are summarized and the instructive directions for future research on PEs are demonstrated, facilitating the commercialization of Li‐SPAN batteries.

Modification and Functionalization of Separators for High Performance Lithium-Sulfur Batteries.

Lithium-sulfur batteries (LSB) have been recognized as a prominent potential next-generation energy storage system, owing to their substantial theoretical specific capacity (1675 mAh g-1) and high energy density (2600 Wh kg-1). In addition, sulfur's abundance, low cost, and environmental friendliness make commercializing LSB feasible. However, challenges such as poor cycling stability and reduced capacity, stemming from the formation and diffusion of lithium polysulfides (LiPSs), hinder LSB's practical application. Introducing functional separators represents an effective strategy to surmount these obstacles and enhance the electrochemical performance of LSBs. Here, we have conducted a comprehensive review of recent advancements in functional separators for LSBs about various (i) carbon and metal compound materials, (ii) polymer materials, and (iii) novel separators in recent years. The detailed preparation process, morphology and performance characterization, and advantages and disadvantages are summarized, aiming to fundamentally understand the mechanisms of improving battery performance. Additionally, the development potential and future prospects of advanced separators are also discussed.

Application of Y-MOF-CNT-Derived Y2O3-C@CNT Composites in Lithium-Sulfur Battery Separators.

In order to mitigate the shuttle effect of lithium polysulfides in lithium-sulfur batteries, we propose a yttrium-metal-organic framework-carbon nanotube (Y-MOF-CNT)-derived Y2O3-C@CNT composite for modifying the separator in this study. The Y-MOFs, comprising yttrium (Y) rare earth metal and terephthalic acid, exemplify a prototypical category of metal-organic framework (MOF) materials. They manifest the advantageous attributes associated with MOFs while concurrently possessing distinctive catalytic traits ascribed to rare earth elements. In this study, Y-MOF nanoparticles were synthesized on carbon nanotube (CNT) substrates via a facile aqueous solution method, succeeded by high-temperature carbonization to yield Y2O3-C@CNT composite materials. These composites were subsequently employed as coatings on one side of polyethylene (PE) separators. The resultant Y2O3-C@CNT composite inherits the particle-like morphology and porosity from its precursor Y-MOF, alongside the inherent conductivity in carbon-based materials. This amalgamation is conducive to polysulfide capture and catalytic conversion processes within lithium-sulfur batteries. The application of the Y2O3-C@CNT-coated PE separator effectively mitigated polysulfide shuttle effects and significantly enhanced the battery electrochemical performance. At a sulfur loading level of 3 mg cm-2 under a 0.5 C rate, an initial discharge specific capacity of 900 mAh g-1 was achieved. After 400 cycles, the discharge specific capacity remained at 483.85 mAh g-1 with a capacity retention rate of 53.7%. Upon increasing sulfur loading to 5 mg cm-2, the discharge specific capacity at a lower rate (0.1 C) reached 817.8 mAh g-1; even after 100 cycles, it maintained a value of 700 mAh g-1 with a capacity retention rate of 85.6%. Notably, our modified Y2O3-C@CNT separator demonstrated exceptional cycling stability, even under conditions involving high sulfur loading.

Dynamically Regulating Polysulfide Degradation via Organic Sulfur Electrolyte Additives in Lithium‐Sulfur Batteries

AbstractLithium‐sulfur (Li‐S) batteries offer promising prospects due to their high energy density and cost‐effectiveness. However, the sluggish kinetics of lithium polysulfides (LiPSs) conversion, particularly the crucial stage from LiPSs to lithium sulfide (Li2S), hampers their development. Herein, a novel strategy for dynamically regulating LiPSs conversion by incorporating 4‐mercaptopyridine (4Mpy), as a LiPSs Redox Regulator (RR) in the electrolyte is introduced. This organic sulfur additive actively interacts with LiPSs during discharge, facilitating rapid conversion and promoting the formation of a three‐dimensional (3D) Li2S structure, thereby enhancing reaction kinetics. Both theoretical and experimental results reveal that the redox conversion mechanism with the 4Mpy additive differs from traditional electrolytes. Upon lithiation, 4Mpy forms lithium‐pyridinethiolate (Li‐pyS), which reversibly engages in the LiPSs conversion during the charging/discharging cycles, significantly improving the redox process. As a result, the Li‐S battery with 4Mpy additive demonstrates superior performances, achieving 10.05 mAh cm−2 under a high sulfur loading of 10.88 mg cm−2, surpassing industrial benchmarks. This study not only presents an approach to mitigating the shuttle effect in Li‐S batteries but also offers valuable insights into electrolyte design for other metal batteries.

ZIF‐67/ZIF‐8 and its Derivatives for Lithium Sulfur Batteries

AbstractLithium–sulfur batteries (LSBs), renowned for their superior energy density and the plentiful availability of sulfur resources, are progressively emerging as the focal point of forthcoming energy storage technology. Nevertheless, they presently confront fundamental challenges including insulation of sulfur and its discharge product, the lithium polysulfides (LiPSs) shuttle phenomenon, and the growth of lithium dendrites. Zeolite imidazole framework materials (ZIFs), particularly ZIF‐8 and ZIF‐67, are significant members of the metal–organic frameworks (MOFs) family. Owing to their high porosity, exceptional adsorption capacity, high structural tunability, and straightforward synthesis process, these materials have demonstrated unique application potential in the field of LSBs. This review initially provides a comprehensive summary of the developmental status and challenges associated with LSBs. Subsequently, it delves into an in‐depth analysis of the distinctive properties and synthesis strategies of ZIFs, with a particular emphasis on ZIF‐8 and ZIF‐67, as well as their composites and derivatives. The review systematically categorizes innovative application examples of these materials in the design of cathode structures and optimization of separators in LSBs. It also presents a forward‐looking perspective and insights on the potential future trajectory of ZIF‐67 materials, informed by the latest research advancements in the field.