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Monocomponent catalysts exhibit the limited catalytic conversion of polysulfides due to their intrinsic electronic structure, but their catalytic activity can be improved by introducing heteroatoms to regulate its electronic structure. However, the rational selection principles of doping elements remain unclear. Here, we are guided by theoretical calculations to select the suitable doping elements based on the balanced relationship between the adsorption strength of lithium polysulfides (LiPSs) and catalytic activity of lithium sulfide. We apply the screening method to develop a new catalyst of phosphorus doped RuSe2, manifesting the further enhanced conductivity compared with original RuSe2, facilitating charge transfer and further modulating the d‐band center of RuSe2, thereby augmenting its effectiveness in interacting with LiPSs. Consequently, the assembled cell exhibits an areal capacity of 7.7 mAh cm−2, even under high sulfur loading of 8.0 mg cm−2 and a lean electrolyte condition (5.0 μL mg−1). This rational screening strategy offers a robust solution for the design of advanced catalysts in the field of lithium‐sulfur batteries and potentially other domains as well. [ABSTRACT FROM AUTHOR]

Lithium–sulfur batteries with liquid electrolytes are discussed as the most promising post‐lithium‐ion‐battery technology in literature due to their high theoretical specific energy and first prototype cells delivering >470 Wh kg−1. Although several electrolyte and material concepts are developed that partially solve the issue of the so‐called shuttle mechanism, the most promising concept to genuinely confine sulfur species in the cathode is all‐solid‐state argyrodite–sulfur cathodes leading to almost theoretical active material utilization by maintaining reasonable sulfur loadings and electrolyte to sulfur ratios. However, this battery concept has so far not achieved reversible cycling against metallic lithium anodes as it requires high pressures for manufacturing, and ductile lithium metal creeps along the grain boundaries of the solid electrolyte particles leading to short cuts of the cells. Recent findings show that metallic lithium, however, can be stably cycled with dimethoxyethane/lithium‐bis(fluorosulfonyl)imide (DME/LiFSI)‐based electrolytes. Herein, for the first time, a semisolid concept is presented combining the benefits of an argyrodite‐based solid‐state cathode and a DME/LiFSI/hydrofluoroether‐based anolyte concept – in coin cells and first pouch cells. This disruptive approach enables projected specific energies higher than 600 Wh kg−1 at cell stack level. [ABSTRACT FROM AUTHOR]

[Display omitted] Despite the bright fortune of lithium-sulfur (Li-S) batteries as one of the next-generation energy storage systems owing to the ultrahigh theoretical energy density and earth-abundance of sulfur, crucial challenges including polysulfide shuttling and low sulfur content of sulfur cathodes need to be overcome before the commercial survival of sulfur cathodes. Herein, cobalt/carbon spheres embedded CNTs (Co-C-CNTs) are rationally designed as multifunctional hosts to synergistically address the drawbacks of sulfur cathodes. The host is synthesized by a facile pyrolysis using Co(OH) 2 template and followed with the controllable etching process. The hierarchical porous structure owning high pore volume and surface area can buffer the volume change, physically confine polysulfides, and provide conductive networks. Besides, partially remained metallic cobalt nanoparticles are favorable for chemical adsorption and conversion of polysulfides, as validated by density functional theory simulations. With the combination of above merits, the S@Co-C-CNTs cathodes with a high sulfur content of 80 wt% present a superior initial capacity (1568 mAh g−1 at 0.1C) with ultrahigh 93.6% active material utilization, and excellent rate performance (649 mAh g−1 at 2C), providing feasible strategies for the optimization of cathodes in metal-sulfur batteries. [ABSTRACT FROM AUTHOR]

Though polyvinylidene fluoride (PVDF) is widely‐used binder for conventional lithium‐sulfur (Li–S) batteries, it still encounters challenges of severe electrode fracture involved by drastic volume change upon repeating cycling, and lack of extended‐functions like trapping dissolved polysulfides and smoothing Li+ transfer. Herein, a methodology of grafting sulfophilic hydrogen‐bond donor and lithiophilic hydrogen‐bond acceptor to the polymer binder (named as PIL), function as gear teethes and tooth spaces, is reported. When cracks occur, the engaged gears driven by dynamic hydrogen bonds are separated, which are spontaneously reformed owing to the automatic meshing of gears, and thus accelerate the healing of cracks. At the molecular level, the synergetic effect of sulfophilic hydrogen‐bond donor and lithiophilic hydrogen‐bond acceptor enables polysulfides immobilization through "push‐pull effect", facilitating the subsequent redox kinetics. Accordingly, the cross‐link network of hydrogen bonds endows the elaborated designed polymer binder with strong adhesive strength and rapid Li+ migration. Attributed to these beneficial properties, the PIL‐based sulfur cathode exhibits excellent rate performance and superior cycling durability (an ultralow capacity fading rate of 0.062% per cycle over 800 cycles at 2 C). Even with high sulfur loading of 9.27 mg cm−2, a high areal capacity of 8.71 mAh cm−2 can be achieved, verifying its potential application. [ABSTRACT FROM AUTHOR]

Lithium‐sulfur (Li‐S) battery shows promising development potential in secondary lithium‐ion batteries. However, the shuttle effect of polysulfides, uncontrollable lithium dendrite growth, and safety hazards in conventional liquid electrolytes limit the popularity of Li‐S batteries in the future commercial market. In this work, a high‐performance gel electrolyte (GPE) was prepared in situ by initiating the ring‐opening polymerization of 1,3‐dioxolane (DOL) with aluminum trifluoromethanesulfonate (Al(OTf)3) and using diethylene glycol dimethyl ether (DME) as a plasticizer, which can effectively improve the interfacial compatibility between sulfur cathode and the electrolyte, as well as the stability of lithium anode. The electrochemical performance of the poly‐DOL (PDOL) GPE was optimized by adjusting the concentration ratio of the initiator. When the concentration of Al(OTf)3 is 4 mM, the PDOL GPE has a high ionic conductivity up to 3.81 × 10−4 S cm−1 and a lithium ion migration number of 0.57. The assembled quasi‐solid‐state Li‐S batteries shows an initial discharge specific capacity of 908.1 mAh g−1 at 0.1 C with a capacity retention of 68% after 240 cycles, and its average Coulombic efficiency is maintained at 96.1%. This gel electrolyte design provides a feasible practical idea in quasi‐solid‐state Li‐S batteries. [ABSTRACT FROM AUTHOR]

Lithium‐sulfur batteries (LSBs) have recently gained extensive attention due to their high energy density, low cost, and environmental friendliness. However, serious shuttle effect and uncontrolled growth of lithium dendrites restrict them from further commercial applications. As "the third electrode", functional separators are of equal significance as both anodes and cathodes in LSBs. The challenges mentioned above are effectively addressed with rational design and optimization in separators, thereby enhancing their reversible capacities and cycle stability. The review discusses the status/operation mechanism of functional separators, then primarily focuses on recent research progress in versatile separators with purposeful modifications for LSBs, and summarizes the methods and characteristics of separator modification, including heterojunction engineering, single atoms, quantum dots, and defect engineering. From the perspective of the anodes, distinct methods to inhibit the growth of lithium dendrites by modifying the separator are discussed. Modifying the separators with flame retardant materials or choosing a solid electrolyte is expected to improve the safety of LSBs. Besides, in‐situ techniques and theoretical simulation calculations are proposed to advance LSBs. Finally, future challenges and prospects of separator modifications for next‐generation LSBs are highlighted. We believe that the review will be enormously essential to the practical development of advanced LSBs. [ABSTRACT FROM AUTHOR]

The spin state of transition‐metal compounds in lithium‐sulfur batteries (LSBs) significantly impacts the electronic properties and the kinetics of sulfur redox reactions (SRR). However, accurately designing the spin state remains challenging, which is crucial for understanding the structure‐performance relationship and developing high‐performance electrocatalysts. Herein, the CoF2, specifically the Co2+ with 3d7 electrons in a high‐spin state distribution (t2g5eg2), were tailored predictably for the first time through the weak coordination field effect of the F element. Both DFT calculations and experimental results confirm that the spin state of Co2+ transitions from low‐ to high‐spin configurations and strongly interacts with sulfur species through Co−S and Li−F bonds during the SRR process. This interaction weakens the S−S bond, promoting its facile cleavage from both ends while also facilitating the rapid and uniform nucleation of Li2S2/Li2S, thus resulting in LSBs with a capacity of 447.7 mAh g−1 at 10 C rates and stable cycling for 1000 cycles, with an acceptable practical capacity of 585 mAh g−1 at a high sulfur loading mass of 10 mg cm−2. This work achieves rational control of the active Co2+ d electron state through the field effect and enriches the application of spin control to accelerate SRR in LSBs. [ABSTRACT FROM AUTHOR]

Lithium‐sulfur batteries, despite being a promising solution for next‐generation secondary batteries, require substantial efforts to overcome the challenges of sluggish sulfur redox kinetics, polysulfides shuttling, and Li metal instability before achieving practical viability. Conventional strategies that utilize metal catalysts or soluble redox mediators (RMs) are limited by either impractical producing processes or unsatisfactory service life. Herein, an electrochemically active organic material, phloroglucinol – 2,6‐diaminoanthraquinone (PG‐DAAQ) is synthesized through a green and facile polymerization process to better resolve these issues. Serving as an RM at the cathode, PG‐DAAQ exhibits enduring redox activity within the sulfur operating potential window, leading to enhanced redox kinetics and sulfur utilization. Remarkably, even without any metal elements, PG‐DAAQ exhibits an excellent affinity to polysulfides, thereby suppressing the shuttling and facilitating the formation of a more favorable solid‐electrolyte interface to stabilize Li deposition at the anode. As a result, Li‐S cells employing PG‐DAAQ show significantly enhanced cycling and rate performances than the control cells. Even with a low electrolyte‐to‐sulfur ratio of 6, pouch cells with PG‐DAAQ deliver a reversible discharge capacity of 821 mA h g−1 after 100 cycles at a C/10 rate. [ABSTRACT FROM AUTHOR]

Both the sluggish sulfur redox reaction (SRR) kinetics and lithium polysulfides (LiPSs) shuttle effect limit the practical application of Li‐S batteries. Designing heterostructure sulfur hosts has emerged as an effective way to address these two issues with one material. However, the principles of heterostructures reinforced Li‐S batteries remain inadequately understood. Here, it is demonstrated for the first time that increasing the entropy of heterostructure can promote its SRR catalytic activity and alleviate the LiPSs shuttling. By a simple solution‐based strategy, a highly chaotic MXene‐based heterostructure (HCMH, TiS2/TiN/TiO2/Ti3C2Tx) is fabricated. The smart integration of "high entropy", heterostructure, and MXene endow the HCMH catalyst with significantly improved performance, demonstrated by a much smaller Tafel slope of 62.9 mV dec−1 and a higher electron transfer number of 7.10, compared with the moderately chaotic MXene‐based heterostructure (MCMH, TiO2/TiN/Ti3C2Tx) and MXene. DFT theoretical calculations reveal that introducing new phases lowers the Gibbs energy barriers of both rate‐limiting Li2S2/Li2S reduction and Li2S decomposition. Upon the addition of only 5 wt.% HCMH to the sulfur cathode, both the reversible capacity and rate capability of Li‐S cells are greatly improved, which further highlights the importance of the high entropy "cocktail effect" in the design of SRR electrocatalysts in the future. [ABSTRACT FROM AUTHOR]

Lithium–sulfur batteries (Li-S batteries) have attracted wide attention due to their high theoretical energy density and the low cost of sulfur cathode material. However, the poor conductivity of the sulfur cathode, the polysulfide shuttle effect, and the slow redox kinetics severely affect their cycling performance and Coulombic efficiencies, especially under low-temperature conditions, where these effects are more exacerbated. To address these issues, this study designs and synthesizes a microspherical cobalt molybdate@reduced graphene oxide (CoMoO4@rGO) composite material as the cathode material for Li-S batteries. By growing CoMoO4 nanoparticles on the rGO surface, the composite material not only provides a good conductive network but also significantly enhances the adsorption capacity to polysulfides, effectively suppressing the shuttle effect. After 100 cycles at room temperature with a current density of 1 C, the reversible specific capacity of the battery stabilizes at 805 mAh g−1. Notably, at −20 °C, the S/CoMoO4@rGO composite achieves a reversible specific capacity of 840 mAh g−1. This study demonstrates that the CoMoO4@rGO composite has significant advantages in suppressing polysulfide diffusion and expanding the working temperature range of Li-S batteries, showing great potential for applications in next-generation high-performance Li-S batteries. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

[Display omitted] • N doped carbon coating CoP hollow nanofibers was successfully fabricated. • Multifunctional materials N/C@CoP-HNFs are used for PIBs and Li-S batteries. • N/C@CoP-HNFs with unique structures show good performance in PIBs and Li-S batteries. • Phase variations of electrodes at different states are studied. • DFT are used to understand electrochemical properties at the atomic level. Herein, a composite of N -doped carbon coated phosphating cobalt hollow nanofibers (N/C@CoP-HNFs) was synthesized by electrospinning, phosphating, and carbon coating processes. When employed as multifunctional electrode materials for potassium-ion batteries (PIBs) and lithium-sulfur (Li-S) batteries, the N/C@CoP-HNFs demonstrated notable electrochemical properties. Specifically, it delivered an initial specific capacity of 420.4 mA h g−1 at a current density of 100 mA g−1, with a sustained capacity of 190.8 mA h g−1 after 200 cycles in PIBs, and a specific capacity of 1448 mA h g−1 at a current density of 0.5C in Li-S batteries, which is considered relatively high for these types of battery technology. This good performance may due to the combination of the carbon nitrogen layer and cobalt phosphide bilayer hollow tube structure, which is conducive to telescoping the diffusion length of ions and electrons and buffer volume variation, and effectively inhibits the shuttle effect. Density functional theory (DFT) calculations were also used to explore the energy storage mechanism of the material. The possible adsorption sites and corresponding adsorption energy of K+ were analyzed, and the advantages of the material were explored by calculating the diffusion barrier and state density. The theoretical simulations further validated the strong adsorption capability of CoP for polysulfides. This work is expected to provide new ideas for new energy storage materials. [ABSTRACT FROM AUTHOR]

Lithium–sulfur batteries are widely regarded as one of the most promising new types of batteries, and the sulfur-based cathode with high-performance is the key to promoting the success of lithium–sulfur batteries. In this work, the sulfur (S)/activated carbon (AC)/carbon nanotube (CNT) composite cathode materials for lithium–sulfur batteries are prepared by simple mixing and heating fusion. It is observed that the S/AC/CNT composites have obvious structural properties of S and consist of many irregular small-sized particles and some large-sized ellipsoids with rough surfaces. The electrochemical properties of the S/AC/CNT composite cathode are evaluated by matching the lithium metal anode and liquid electrolyte (LE). The cell delivers a high initial discharge capacity of 1077.0 mAh g−1 at 0.1 mA cm−2, and when the current density increases to 0.5 mA cm−2, the cell has a discharge capacity of 712.8 mAh g−1. In addition, the cell can retain the discharge capacities of 437.6 mAh g−1 after 200 cycles and 273.6 mAh g−1 after 500 cycles at 0.5 mA cm-2, showing good cycling stability. This work provides promising S/AC/CNT composite cathode materials with high capacity and good electrochemical stability for lithium–sulfur batteries. [ABSTRACT FROM AUTHOR]

The development of electrocatalysts with high catalytic activity is conducive to enhancing polysulfides adsorption and reducing activation energy of polysulfides conversion, which can effectively reduce polysulfide shuttling in Li-S batteries. Herein, a novel catalyst NiCo-MoOx/rGO (rGO = reduced graphene oxides) with ultra-nanometer scale and high dispersity is derived from the Anderson-type polyoxometalate precursors, which are electrostatically assembled on the multilayer rGO. The catalyst material possesses dual active sites, in which Ni-doped MoOx exhibits strong polysulfide anchoring ability, while Co-doped MoOx facilitates the polysulfides conversion reaction kinetics, thus breaking the Sabatier effect in the conventional electrocatalytic process. In addition, the prepared NiCo-MoOx/rGO modified PP separator (NiCo-MoOx/rGO@PP) can serve as a physical barrier to further inhibit the polysulfide shuttling effect and realize the rapid Li+ migration. The results demonstrate that Li-S coin cell with NiCo-MoOx/rGO@PP separator shows excellent cycling performance with the discharge capacity of 680 mAh·g−1 after 600 cycles at 1 C and the capacity fading of 0.064% per cycle. The rate performance is also impressive with the remained capacity of 640 mAh·g−1 after 200 cycles even at 4 C. When the sulfur loading is 4.0 mg·cm−2 and electrolyte volume/sulfur mass ratio (E/S) ratio is 6.0 μL·mg−1, a specific capacity of 830 mAh·g−1 is achieved after 200 cycles with a capacity decay of 0.049% per cycle. More importantly, the cell with NiCo-MoOx/rGO@PP separator exhibits cycling performance under wide operating temperature with the reversible capacities of 518, 715, and 915 mAh·g−1 after 100 cycles at −20, 0, and 60 °C, respectively. This study provides a new design approach of highly efficient catalysts for sulfur conversion reaction in Li-S batteries. [ABSTRACT FROM AUTHOR]

Ion‐selective separators are promising to inhibit soluble intermediates shuttle in practical lithium‐sulfur (Li−S) batteries. However, designing and fabricating such high‐performance ion‐selective separators using cost‐effective, eco‐friendly, and versatile methods remains a formidable challenge. Here we present ion‐selective separators fabricated via the spontaneous deposition of green tea‐derived polyphenols onto a polypropylene separator, aimed at enhancing the stability of Li−S batteries. The resulting natural polyphenol‐reinforced ion‐selective (NPRIS24) separators exhibit rapid Li ion transport and high soluble intermediates inhibition capability with an ultralow shuttle rate of 0.67 % for Li2S4, 0.19 % for Li2S6 and 0.10 % for Li2S8. This superior ion‐selectivity arises from the high electronegativity and strong lithiophilic nature of the phenolic compounds. Consequently, we have achieved high‐performance Li−S batteries that are steadily cyclable under the challenging conditions of an S loading of 5.7 mg cm−2, an electrolyte‐to‐S ratio of 5.1 μL mg−1, and a 50 μm Li foil anode. Furthermore, the NPRIS24 separator enhances the performance of other Li metal batteries utilizing commercial LiFePO4 (5.3 mg cm−2) and LiNi0.5Co0.2Mn0.3O2 (9.9 mg cm−2) cathodes. This work underscores the potential of utilizing natural polyphenols for the design of advanced ion‐selective separators in energy storage systems. [ABSTRACT FROM AUTHOR]

Lithium‐sulfur (Li−S) batteries are considered as a most promising rechargeable lithium metal batteries because of their high energy density and low cost. However, the Li−S batteries mainly suffer the capacity decay issue caused by the shutting effect of lithium polysulfides and the safety issues arising from the Li dendrites formation. This review outlines the current issues of Li−S batteries. Furthermore, we comprehensively summarized the challenges encountered by Li anode in Li−S batteries, such as the heterogeneous deposition of the Li anode, the unstable solid electrolyte interface (SEI) layer, and volume expansion. Moreover, research progresses in the stabilization strategies of Li anodes (physical approaches, optimization of electrolyte, surface protection layer, and design of current collector) is discussed in detail. Lastly, the remaining challenges and future research directions of Li metal anode stabilization in Li−S batteries are also present. [ABSTRACT FROM AUTHOR]

Alloy catalyst is considered to be an important strategy to solve the shuttle effect and sluggish kinetics of lithium‐sulfur batteries (LSBs). However, the effect of the electronic structure of the alloy catalyst on the sulfur conversion process has not been effectively analyzed. In this paper, based on alloying strategy, the electronic structure of such a FeCoNi catalyst is regulated and optimized, and the sulfur adsorption configuration and catalytic conversion process are defined. The in situ Raman spectroscopy and the density functional theory (DFT) are employed to deeply understand the catalytic mechanism of such a sulfur conversion. A cell with FeCoNi modified separator delivers an ultra‐low capacity attenuation of 0.056% per cycle over 1000 cycles at 3 C. The outstanding anti‐self‐discharge performance of 8.1% over 7 days is also achieved. Furthermore, the obtained cell with a high sulfur loading of 9.7 mg cm−2 and lean electrolyte of 5.6 µL mgs−1 exhibits 81% capacity retention after 100 cycles, providing a research prospect for the practical application of lithium‐sulfur batteries. [ABSTRACT FROM AUTHOR]

Sulfurized polyacrylonitrile (SPAN) cathodes in high energy‐density Li‐metal batteries have garnered widespread interest owing to their good cycling stability and moderately high capacities. However, their application is hindered by the low prevalence of advanced electrolytes that can simultaneously mitigate polysulfide generation at the cathode and stabilize the Li‐metal anode. Here, a weakly solvating electrolyte is presented, employing a single solvent tetrahydropyran (THP). The solvation structure is effectively tuned by adjusting the salt concentration to stabilize both the Li‐metal anode and SPAN cathode. This approach enables stable cycling with high SPAN loadings (≈5 mg cm−2) and lean electrolyte contents (≈5 µL mgSPAN−1) across a wide temperature range: 0 °C, room temperature, and 50 °C. A pouch cell with a high SPAN loading and a low electrolyte‐to‐SPAN (E/SPAN) ratio of 3 µL mg−1 shows a stable 79.1% capacity retention after 40 cycles. Additionally, THP can be effectively employed in localized high‐concentration electrolyte (LHCE) systems to reduce the diluent‐to‐solvent ratio for greater LHCE viability. The study demonstrates the potential of weakly solvating solvents in Li‐SPAN batteries, offering a pathway for their practical application. [ABSTRACT FROM AUTHOR]

Recently, research on polyoxometalates (POMs) has gained significant momentum. Owing to their properties as electronic sponges, POMs catalyst harbor substantial potential in lithium‐sulfur battery research. However, POMs undergo a transformation into reduced heteropoly blue (HPB) during electrochemical reactions, which then dissolve into the electrolyte, resulting in catalyst loss. In this research, we amalgamated 18‐crown‐6 (CR6) with K3PW12O40, (KPW), synthesized a novel POM‐based supramolecular compound, and integrated it with graphene oxide (GO) to fabricate a multi‐functional composite polypropylene (PP) separator KPW‐CR6/GO/PP. The crown ether array was employed to immobilize POM and construct ion transport channels, thereby enhancing the Li+ migration rate and capturing polysulfides. Subsequently, leveraging the stable structure and redox properties of POM, the polysulfide is catalyzed to transform and inhibit the shuttle effect, thereby protecting the Li anode. The lithium‐sulfur batteries with the Crown ether‐POM supramolecular compound separators, exhibit enhanced capacity and stability (1073.3 mAh g−1 at 1.0 C, and 81.5 % retention rate after 250 cycles). The battery (S loading: 3.2 mg cm−2) presents an initial specific discharge capacity of 543.4 mAh g−1 at 0.5 C, with 89.8 % of the capacity retained after 160 cycles. This underlines the practical application potential of Crown ether‐POM supramolecular materials in Li−S batteries. [ABSTRACT FROM AUTHOR]

The performance of high‐energy‐density lithium–sulfur (Li–S) batteries is limited by the unmanageable deposition/dissolution kinetics of lithium anode and sulfur cathode, leading to subpar electrochemical efficiency. Prior to being deposited on the electrolyte/electrode interface or within the interior, the solvated lithium‐ion (Li+) must undergo de‐solvation to produce free Li+ ions. These ions then participate in subsequent Redox reactions. The sulfur cathode faces challenges related to solid–liquid transformation and polysulfide conversion/shuttle, which impact the deposition/dissolution process. These issues collectively create insurmountable electrochemical barriers in lithium–sulfur batteries. Atom‐level 2D catalysts, contributing to the consummate atomic efficiency (≈100 at%), play an important role in accelerating deposition/dissolution kinetics in lithium–sulfur batteries. In the review, the preparation of atom‐level 2D catalysts and catalytic kinetic process on accelerating Li+ de‐solvation, Li0 stripping/dissolution, Li0 nucleation/deposition of lithium anode, polysulfide conversion, and LixS deposition of sulfur cathode are summarized, and the outlook of high‐performance single‐atom, multiple atoms modified 2D catalysts in lithium, sodium, and zinc‐based batteries is putting forward. [ABSTRACT FROM AUTHOR]

Lithium‐sulfur (Li−S) batteries display promise as redox‐based batteries, where separators are an essential part of preventing short‐circuiting of the positive and negative electrodes, while the shuttle effect is a critical issue of separators. Currently, commercial PP separators are weak in inhibiting the polysulfides shuttling, so modified separators are needed to inhibit it to improve the battery performance. This paper reports that CeVO4/KB composites act as separator materials. CeVO4/KB modified PP separators enhanced the adsorption of LiPSs, accelerated the rate of Li+ migration, and catalyzed the conversion of LiPSs. These bring about the effect that CeVO4/KB/PP batteries reach 1200.9 mAh g−1 in the first cycle with a capacity retention rate of 86.5 % after 100 cycles at 0.2 C and reach 882.7 mAh g−1 of the initial cycle with a capacity decay rate of 0.063 % after 1000 cycles at 3 C. This work introduces rare earth metal vanadates to modify the separator, adding new ideas for designing separators for good‐performance batteries. [ABSTRACT FROM AUTHOR]

Lithium–sulfur (Li-S) batteries offer a high theoretical energy density but suffer from poor cycling stability and polysulfide shuttling, which limits their practical application. To address these challenges, we developed a PANI-modified MoS2-NG composite, where MoS2 nanoflowers were uniformly grown on graphene oxide (GO) through PANI modification, resulting in an increased interlayer spacing of MoS2. This expanded spacing exposed more active sites, enhancing polysulfide adsorption and catalytic conversion. The composite was used to prepare MoS2-NG/PP separators for Li-S batteries, which achieved a high specific capacity of 714 mAh g−1 at a 3 C rate and maintained a low capacity decay rate of 0.085% per cycle after 500 cycles at 0.5 C. The larger MoS2 interlayer spacing was key to improving redox reaction kinetics and suppressing the shuttle effect, making the MoS2-NG composite a promising material for enhancing the performance and stability of Li-S batteries. [ABSTRACT FROM AUTHOR]

High‐specific energy sulfur‐based cathodes have attracted considerable interest in lithium batteries. Organosulfur cathodes offer inherent advantages of high element abundance and an extended cycling life, aligning with the evolving requirements of future energy storage devices. Over the past decade, research efforts have been devoted to optimizing electrochemical performance through the rich and tunable molecular structures of organosulfur compounds. To further advance the fundamental research and practical application of lithium‐organosulfur batteries, a systematical analysis of the correlation between the molecular structures and electrochemical mechanisms of organosulfur cathodes is imperative. This involves deriving the key parameters at the cell level and investigating the feasibility. In this review, the thermodynamics, reaction processes, and electrochemical kinetics of organosulfur cathodes, grounded in fundamental theories of electrochemistry and materials science are discussed. Expanding the insights, comparisons among elemental sulfur, organosulfur, and n‐type organic cathodes (e.g., carbonyl cathodes) are drawn. The gap between fundamentals and practical applications targeting 500 Wh kg−1 lithium organosulfur batteries is highlighted through energy density calculations and identification of key factors affecting pouch cells. Finally, potential strategies and prospects for the overall design of advanced lithium‐organosulfur batteries are proposed, considering both theoretical foundations and practical implementations. [ABSTRACT FROM AUTHOR]

Lithium‐sulfur batteries (LSBs) are regarded as one of the most promising candidates for next‐generation energy storage systems. However, the commercialization of LSBs is still hindered by several technical issues, including the notorious polysulfide migration from the cathode to the anode and the sluggish sulfur conversion kinetics. Herein, a quasi‐1D hexagonal chalcogenide perovskite, Sr8Ti7S21, is demonstrated as an efficient sulfur host able to overcome these limitations. Experimental results and density functional theory calculations show Sr8Ti7S21 to offer strong lithium polysulfides (LiPS) binding through multiple bond formation. Besides, Sr8Ti7S21 effectively facilitates the kinetics of the LiPS redox reaction. As a result, S@Sr8Ti7S21‐based cathodes exhibit excellent initial capacities up to 1315 mAh g−1 at 0.2C, impressive cycling stability with an average capacity decay rate of 0.08% per cycle over 400 cycles at 1C, and a high areal capacity of 6.58 mAh cm−2 under a high sulfur loading of 6.5 mg cm−2. This work reveals the potential capabilities and promising prospects of chalcogenide perovskites in advancing LSBs technology. [ABSTRACT FROM AUTHOR]

The step‐order or disproportionation conversion of lithium polysulfides (LiPSs) is still a blind box in LiS batteries (LSBs) system. The cation‐doped electrocatalyst (Fe‐CoS2@HCNF) is designed through modulating electron‐surrounding situation of the central atomic d‐band to promote regional electron‐directed LiPSs reduced‐order‐transformation (especially, Li2S4Li2S). Fe‐CoS2@HCNF satisfies the requirement of mass (electron/ion) transfer reaction, quantizing as multi‐osmosis‐connected transportation channels and an all‐encompassing interior space for sulfur reduction occurring. Based on experiments and DFT calculations, the introduced Fe presents a local electron deficiency state toward regulating regional electron delocalization between Fe and Co matrix, which induces the d‐band state of the metal site, strengthening the metal 3d orbital coupling interaction with S2−of LiPSs, further guiding the order‐transformation of intermediate LiPSs. Consequently, the Fe‐CoS2@HCNF electrode has excellent electrochemical properties, performing at 3.0 C with 0.064 % capacity decay per cycle, and even maintaining super cycle stability at a high sulfur loadings. In addition, the pouch cell assembled can also reach an initial specific capacity of 1070.3 mAh g−1 at 0.1 C, which can still show good long‐term cycle stability. This work provides a valuable prospect for analyzing SRR intermediate state by regional electron flow regulation of electrocatalyst in practical LSBs. [ABSTRACT FROM AUTHOR]

Improving the slow redox kinetics of sulfur species and shuttling issues of soluble intermediates induced from the multiphase sulfur redox reactions are crucial factors for developing the next‐generation high‐energy‐density lithium‐sulfur (Li−S) batteries. In this study, we successfully constructed a novel molecular electrocatalyst through in situ polymerization of bis(3,4‐dibromobenzene)‐18‐crown‐6 (BD18C6) with polysulfide anions on the cathode interface. The crown ether (CE)‐based polymer acts as a spatial "fence" to precisely control the unique redox characteristics of sulfur species, which could confine sulfur substance within its interior and interact with lithium polysulfides (LiPSs) to optimize the reaction barrier of sulfur species. The "fence" structure and the double‐sided Li+ penetrability of the CE molecule may also prevent the CE catalytic sites from being covered by sulfur during cycling. This new fence‐type electrocatalyst mitigates the "shuttle effect", enhances the redox activity of sulfur species, and promotes the formation of three‐dimensional stacked lithium sulfide (Li2S) simultaneously. It thus enables lithium‐sulfur batteries to exhibit superior rate performance and cycle stability, which may also inspire development facing analogous multiphase electrochemical energy‐efficient conversion process. [ABSTRACT FROM AUTHOR]

[Display omitted] • I-CNT with enhanced electronic conductivity is reported as a multifunctional sulfur skeleton material. • I-CNT skeleton boosts adsorption effect and conversion reaction kinetics of LiPSs. • DFT calculation, quasi in-situ EIS and in-situ Raman spectroscopy reveal the polysulfides conversion mechanism. • The Li 2 S potentiostatic deposition i - t curves also confirm the improved liquid–solid reaction kinetics. • I-CNT@S exhibits satisfactory cycle stability of 528.9 mAh g−1 at 2C after 700 cycles. Compared with lithium-ion batteries (LIBs), lithium-sulfur batteries (LSBs), based on electrochemical reactions involving multi-step 16-electron transformations provide higher specific capacity (1672 mAh g−1) and specific energy (2600 Wh kg−1), exhibiting great potential in the field of energy storage. However, the inherent insulation of sulfur, slow electrochemical reaction kinetics and detrimental shuttle-effect of lithium polysulfides (LiPSs) restrict the development of LSBs in practical applications. Herein, the iodine-doped carbon nanotubes (I-CNTs) is firstly reported as sulfur host material to the enhance the adsorption-conversion kinetics of LSBs. Iodine doping can significantly improve the polarity of I-CNTs. Iodine atoms with lone pair electrons (Lewis base) in iodine-doped CNTs can interact with lithium cations (Lewis acidic) in LiPSs, thereby anchoring polysulfides and suppressing subsequent shuttling behavior. Moreover, the charge transfer between iodine species (electron acceptor) and CNTs (electron donor) decreases the gap band and subsequently improves the conductivity of I-CNTs. The enhanced adsorption effect and conductivity are beneficial for accelerating reaction kinetics and enhancing electrocatalytic activity. The in-situ Raman spectroscopy, quasi in-situ electrochemical impedance spectroscopy (EIS) and Li 2 S potentiostatic deposition current–time (i-t) curves were conducted to verify mechanism of complex sulfur reduction reaction (SRR). Owing to above advantages, the I-CNTs@S composite cathode exhibits an ultrahigh initial capacity of 1326 mAh g−1 as well as outstanding cyclicability and rate performance. Our research results provide inspirations for the design of multifunctional host material for sulfur/carbon composite cathodes in LSBs. [ABSTRACT FROM AUTHOR]

The intrinsically sluggish sulfur reduction reaction kinetics and serious shuttle effect of soluble lithium polysulfides (LiPSs) severely impede the practical commercialization of lithium‐sulfur (Li‐S) batteries. Herein, self‐supported tungsten nitride and carbide heterostructures with vanadium doping that are directly grown on carbon cloth substrate (CC@V‐W2N/WC1‐x) are creatively designed for Li‐S batteries, which can tandemly catalyze the liquid–liquid conversion and liquid–solid conversion of polysulfide intermediate free of any interference from polymer binders and conductive additives. Noteworthy, the rich heterointerfaces and vanadium doping are beneficial for rapid charge transfer, strong chemical adsorption toward LiPSs, massive exposed catalytically active sites, and remarkable catalytic activities. Consequently, Li‐S batteries assembled with the CC@V‐W2N/WC1‐x/S cathodes exhibit high sulfur utilization, superior rate capability, and decent long‐term cycling stability. Furthermore, experimental analyses and theoretical calculations jointly substantiate that the V‐W2N component is more effective in catalyzing the conversion of long‐chain LiPSs, while the V‐WC1‐x benefits the favorable Li2S deposition kinetics. More importantly, the Li‐S pouch cells are also fabricated to demonstrate their feasibility for practical applications. This work not only highlights the significance of tandem catalysis on the consecutive conversion of LiPSs but also provides a feasible avenue for developing highly efficient electrocatalysts toward high‐performance Li‐S batteries. [ABSTRACT FROM AUTHOR]

It is of great importance to develop the high-performance energy storage systems that modern society needs for innovative technologies such as electric vehicles, consumer electronics, and grid-scale storage. Today, the unit cost of energy produced from renewable solar and wind sources has reached levels competitive with fossil fuels. Unit costs of energy storage systems have not yet reached the desired levels and are still very expensive. Therefore, there is a need to develop high-performance energy storage systems using sustainable and economical methods. In this study, the fabrication and characterization of S/c-ZIF-8/Ti3C2 cathodes were done, and the structural and electrochemical stability of high-capacity lithium-sulfur batteries (LSBs) was improved. After the structural and chemical characterization of the produced materials and cathodes, they were used in Li-S batteries and their performancerelated properties were examined. The fabricated Li-S batteries have a specific capacity of approximately 1000 mAh/g. With the fabricated S/c-ZIF-8/Ti3C2 cathodes, the adverse effects caused by the insulating nature of sulfur and lithium polysulfide are eliminated. [ABSTRACT FROM AUTHOR]

Developing high‐performance lithium‐sulfur batteries is a promising way to attain higher energy density at a lower cost beyond the state‐of‐the‐art lithium‐ion battery technology. However, the major issues impeding their practical applications are the sluggish kinetics and the parasitic shuttling reactions of sulfur and polysulfides. Here, pillaring the multilayer graphene membrane with a metal–organic framework (MOF) demonstrates the substantial impact of a versatile interlayer design in tackling these issues. Unlike regular composite separators reported so far, the participation of tri‐metallic Ni−Co−Mn MOF as pillars supports the construction of an ion‐channel interconnected interlayer structure, unexpectedly balancing the interfacial concentration polarization, spatially confining the soluble polysulfides, and vastly affording the lithiophilic sites for highly efficient polysulfide sieving/conversion. As a demonstration, we show that the MOF‐pillared interlayer structure enables outstanding capacity (1634 mAh g−1 at 0.1 C) and longevity (average capacity decay of 0.034 % per cycle in 2000 cycles) for lithium‐sulfur batteries. Besides, the multilayer separator can be readily integrated into the high‐nickel cathode (LiNi0.91Mn0.03Co0.06O2)‐based lithium‐ion batteries, which efficiently suppresses the undesired phase evolution upon cycling. These findings suggest the potential of “gap‐filling” materials in fabricating multi‐functional separators, bringing forward the pillared interlayer structure for energy‐storage applications. [ABSTRACT FROM AUTHOR]

The development of new energy storage technology has played a crucial role in advancing the green and lowcarbon energy revolution. This has led to significant progress, spanning from fundamental research to its practical application in industry over the past decade. Nevertheless, the constrained performance of crucial materials poses a significant challenge, as current electrochemical energy storage systems may struggle to meet the growing market demand. In recent years, carbon derived from biomass has garnered significant attention because of its customizable physicochemical properties, environmentally friendly nature, and considerable economic value. This review aims to provide a comprehensive overview of the production-application chain for biomass-derived carbon. It provides a comprehensive analysis of morphology design, structural regulation, and heteroatom-doping modification, and explores the operational mechanisms in different energy storage devices. Moreover, considering recent research progress, the potential uses of biomass-derived carbon in alkali metal-ion batteries, lithium-sulfur batteries, and supercapacitors are thoroughly assessed, offering a broader outlook on the emerging energy sector. Finally, based on the technical challenges that need to be addressed, potential research directions and development objectives are suggested for achieving large-scale production of biomass-derived carbon in the field of energy storage. [ABSTRACT FROM AUTHOR]

Sulfur redox reactions render lithium-sulfur (Li-S) batteries with an energy density of > 500 Wh kg-1 but suffer a low practical capacity and fast capacity fade due to sluggish sulfur redox reaction (SRR) kinetics, which lies in the complex reaction process that involves a series of reaction intermediates and proceeds via a cascade reaction. Here, we present a Pt-Cu dual-atom catalyst (Pt/Cu-NG) as an electrocatalyst for sulfur redox reactions. Pt/Cu-NG enabled the rapid conversion of soluble polysulfide intermediates into insoluble Li2S2/Li2S, and consequently, it prevented the accumulation and shuttling of lithium polysulfides, thus outperforming the corresponding singleatom catalysts (SACs) with individual Pt or Cu sites. Operando X-ray absorption spectroscopy and density functional theory calculations revealed that a synergistic effect between the paired Pt and Cu atoms modifies the electronic structure of the Pt site through d-orbital interactions, resulting in an optimal moderate interaction of the metal atom with the different sulfide species. This optimal interaction enhanced charge transfer kinetics and promoted sulfur redox reactions. Our work thus provides important insights on the atomic scale into the synergistic effects operative in dual-atom catalysts and will thus pave the way to electrocatalysts with enhanced efficiency for high-performance Li-S batteries. [ABSTRACT FROM AUTHOR]

Lithium–sulfur (Li–S) batteries promise high theoretical energy density and cost‐effectiveness but grapple with challenges like the polysulfide shuttle effect and sluggish kinetics. Metal–organic framework (MOF) catalysts emerge as a leading solution, despite limited conductivity and high steric hindrance. This study employs undercoordination chemistry to modify Zn–Co bimetallic MOFs (D‐ZIF L), removing organic ligands from active centers. This process mitigates spatial hindrance, thereby promoting comprehensive contact between sulfur species and metal active centers, consequently enhancing the catalytic efficiency of MOFs. Moreover, undercoordination treatment of the metal active centers induces electron redistribution, augmenting electron density at the Fermi level of the metal elements, thereby ameliorating the intrinsic conductivity. Leveraging these advantages, fabricated Li–S batteries employing D‐ZIF L catalysts exhibited markedly mitigated shuttling effects and accelerated sulfur species conversion kinetics. Notably, a substantial reverse areal capacity of 5.0 mAh cm⁻2 is achieved after 100 cycles with an evaluated sulfur loading of 5.5 mg cm⁻2. Furthermore, a practical pouch cell demonstrated an initial capacity of 1.8 Ah at 85.8 mA with stable cycling for 50 cycles. This study underscores the potential of undercoordination chemistry in the development of highly conductive MOF catalysts with minimized steric hindrance, thereby advancing the prospects of Li–S battery technology. [ABSTRACT FROM AUTHOR]

With the rising demand for electricity storage devices, the performance requirements for such equipment have become increasingly stringent. Lithium-sulfur (Li-S) batteries are poised to be among the next generation of energy storage systems. However, before they can be commercially viable, several challenges must be addressed, including low sulfur conductivity and the shuttle effect. Herein, polypyrrole based sulfur composite was prepared by simple method in hydrothermal teflon lined autoclave for Li-S battery. The S/SP/ppy/PVDF electrode exhibited the initial discharge capacity of 662 mAh g− 1 at 0.5 C and 637 mAh g− 1 after 100 cycles. The Coulombic efficiency was 96% all along charge/discharge cycling. Moreover, Li-S coin cells were assembled and tested to demonstrate the potential application and scale-up of the polypyrrole-sulfur composite. [ABSTRACT FROM AUTHOR]

Few-layered N -doped rGO nanosheets covered with defective TiO 2- x nanoparticles form an enriched 2D/0D Schottky heterojunction through interfacial N -Ti and C-Ti bonds, serving as a bipolar cathode host for lithium-sulfur batteries with enhanced electrochemical properties. [Display omitted] The shuttling and sluggish conversion kinetics of lithium polysulfides (LiPSs) lead to poor cycling performance and low energy efficiency in lithium-sulfur batteries (LSBs). In this work, a hierarchically structured nanocomposite, synthesized through a surfactant-directed hydrothermal growth following dopamine-protected pyrolysis, serves as a bidirectional catalyst for LSBs. This nanocomposite comprises N -doped reduced graphene oxide (rGO) nanosheets anchored with uniformly distributed TiO 2- x nanoparticles via interfacial N -Ti and C-Ti bonding, resulting in the formation of abundant 2D/0D Schottky heterojunctions (rGO/TiO 2- x). Density functional theory (DFT) calculations and in situ Raman characterizations demonstrate that rGO/TiO 2- x effectively inhibits the shuttling of LiPSs with enhanced redox kinetics, achieving high utilization of the sulfur cathode and improving the overall reversibility. A high areal capacity is attained at a high sulfur loading and a low electrolyte/sulfur ratio. The initial specific capacity reaches 1010 mA h g−1 at a current density of 0.2C (1C = 1675 mA g−1), and a retention of 86.4 % is attained over 100 cycles. A light-emitting diode (LED) screen using two LSBs with rGO/TiO 2- x demonstrates their high potential for practical applications. [ABSTRACT FROM AUTHOR]

The 1T-rich MoS 2 @PC materials were rationally constructed and evaluated as an efficient polysulfide promotor for high-performance Li-S batteries. The constructed 1T-rich MoS 2 nanosheets not only have strong adsorption capacity for polysulfide, but also can catalyze the conversion of polysulfide rapidly. [Display omitted] The practical applications of lithium-sulfur (Li-S) batteries have severely been hindered by notorious shuttle effect and sluggish redox kinetics of lithium polysulfide intermediates (LiPSs), which bring about rapid capacity degradation, low coulombic efficiency and poor cycling stability. In this work, 1T-rich MoS 2 nanosheets are in-situ developed onto the conductive porous carbon matrix (1T-rich MoS 2 @PC) as efficient polysulfide promotors for high-performance Li-S batteries. The porous carbon skeleton tightly anchors MoS 2 nanosheets to prevent their reaggregation and ensures accessible electrical channels, and at the same time provides a favorable confined space that promotes the generation of 1T-rich MoS 2 structure. More importantly, the uniformly distributed metallic 1T-rich MoS 2 nanosheets not only affords rich sulfphilic sites and high binding energy for immobilizing LiPSs, but also favors rapid electron transfer and LiPSs conversation kinetics, substantially regulating sulfur chemistry in working cells. Consequently, the Li-S cell assembled with 1T-rich MoS 2 @PC modified separator delivers a remarkable cycling stability with ultralow capacity decay rate of 0.067% over 500 cycles at 1C. Encouragingly, under harsh conditions (high sulfur loading of 4.78 mg cm−2 and low E/S ratio of 8 μL mg−1), a favorable electrochemical performance can still be demonstrated. This study highlights the profitable design of 1T-rich MoS 2 /carbon based electrocatalyst for suppressing shuttle effect and promoting catalytic conversation of LiPSs, and has the potential to be applied to in other energy storage systems. [ABSTRACT FROM AUTHOR]

A two-dimensional porous g-C 3 N 4 /MXene heterostructure (CN-MX) with intrinsic defects was designed as the desolvation promoter to accelerate the dissociation of solvated Li+ and propel the sulfur redox conversion. The Li-S cells with g-C 3 N 4 /MXene heterostructure demonstrated satisfactory areal capacity (5.5 mAh cm−2 at 0.2 C) and impressive low-temperature performance at 0 °C (91.6% capacity retention after 100 cycles at 0.5 C). [Display omitted] Lithium-sulfur (Li-S) batteries exhibit superior theoretical capacity and energy density but are still hindered by the sluggish redox conversion kinetic of lithium polysulfides arising from the significant desolvation barrier, especially under high current density or low-temperature environments. Herein, a two-dimensional (2D) porous graphitic phase carbon nitride/MXene (CN-MX) heterostructure with intrinsic defects was designed via electrostatic adherence and in-situ thermal polycondensation. In the design, the defect-rich CN with abundant catalytic activity and porous structure could efficiently facilitate the lithium polysulfides capture, the dissociation of solvated lithium-ion (Li+), and fast Li+ diffusion. Concurrently, 2D MXene nanosheets with high electronic conductivity could act as charge transport channels and provide electrochemical active sites for sulfur redox reactions. The Li-S cells with CN-MX heterostructure modified separator demonstrated uncommon rate performance (945 mAh/g at 4.0 C) and satisfactory areal capacity (5.5 mAh cm−2 at 0.2 C). Most remarkably, even at 0 °C, the assembled Li-S batteries performed favorable cycle stability (91.6% capacity retention after 100 cycles at 0.5 C) and outstanding rate performance (695 mAh/g at 2.0 C), and superior high loading performance (5.1 mAh cm−2 at 0.1 C). This work offers exciting new insights to enable Li-S batteries to operate in extreme environments. [ABSTRACT FROM AUTHOR]

To improve the sulfur reaction kinetics and inhibit the notorious shuttle effects, a tube‐in‐tube structure decorated by carbon nanotubes (CNT) and Fe3C nanoparticles (TIT/Fe3C‐CNT) is designed as sulfur host for lithium‐sulfur batteries (LSBs) in this work. The construction of tube‐in‐tube structure increases the active sites and the specific surface area of the material. Additionally, Fe3C nanoparticles can effectively adsorb the soluble lithium polysulfides and promote their catalytic conversion, thus greatly alleviating the shuttle effects. As a result of these advantages, the TIT/Fe3C‐CNT‐based cathode exhibits a high reversible capacity of 841 mAh g−1 after 200 cycles with a low decay of 0.056 % per cycle at 0.5 C. This work provides a promising and reasonable approach to the rational design of sulfur host for LSBs. [ABSTRACT FROM AUTHOR]

The high energy density and low cost of sulfur make lithium–sulfur batteries one of the most promising candidates for the next generation of energy storage. Nevertheless, the application is still hampered by the shuttle effect of soluble lithium polysulfides (LiPSs) intermediates and slow redox kinetics, resulting in irreversible loss of the active material, severe self‐discharge and poor cycle stability of the electrode. Therefore, in this work, a novel Mo,N co‐doped porous carbon (Mo,N−C) was successfully synthesized by simply calcining a mixture of ramie degumming waste with cost‐effective molybdenum salt, and then employed as the LiPSs anchor. Due to the conductive carbon matrix, abundant porous structures as well as the doping Mo and N heteroatoms, the sluggish redox kinetic of the cathode has been significantly improved and the shuttle phenomenon of LiPSs has been effectively inhibited, consequently, the as‐prepared Mo,N−C/S‐0.4 composite cathode could demonstrate a good initial capacity of 1379.2 mAh g−1 at 0.2 C, and the reversible capacity could remain at 997.5 mAh g−1 after 100 cycles. Even at a high discharge rate of 1.0 C, the capacity could remain at 700.2 mAh g−1 after 400 cycles. This work provides a new avenue for utilizing waste biomass in clean energy storage. [ABSTRACT FROM AUTHOR]

Lithium–sulfur (Li–S) battery is a promising next‐generation energy storage system. However, the poor cyclability caused by the shuttle effect is still a key challenge for its practical application. Here, a polypropylene separator modified with α‐MnO2/RuO2 heterostructure is presented to facilitate the transformation of lithium polysulfides (LiPSs) and optimize the rate‐determining step in both the reduction and oxidation processes of the sulfur electrode. The unique separator effectively suppresses the dissolution and shuttling of soluble LiPSs in Li–S batteries. The α‐MnO2/RuO2 heterostructure modified separator with a Ru content of ≈8 wt% enables a high areal capacity of over 5.0 mAh cm−2 after 55 cycles at 0.2C in a Li–S coin cell, and the resultant pouch cell retains 78.2% of its initial capacity after 200 cycles at 0.1C, suggesting considerable potential for commercial applications. This work provides new insights into the regulation of electrochemical reactions in Li–S batteries. [ABSTRACT FROM AUTHOR]

Established in 1962, lithium–sulfur (Li–S) batteries boast a longer history than commonly utilized lithium–ion batteries counterparts such as LiCoO2 (LCO) and LiFePO4 (LFP) series, yet they have been slow to achieve commercialization. This delay, significantly impacting loading capacity and cycle life, stems from the long‐criticized low conductivity of the cathode and its byproducts, alongside challenges related to the shuttle effect, and volume expansion. Strategies to improve the electrochemical performance of Li–S batteries involve improving the conductivity of the sulfur cathode, employing an adamantane framework as the sulfur host, and incorporating catalysts to promote the transformation of lithium polysulfides (LiPSs). 2D MXene and its derived materials can achieve almost all of the above functions due to their numerous active sites, external groups, and ease of synthesis and modification. This review comprehensively summarizes the functionalization advantages of MXene‐based materials in Li–S batteries, including high‐speed ionic conduction, structural diversity, shuttle effect inhibition, dendrite suppression, and catalytic activity from fundamental principles to practical applications. The classification of usage methods is also discussed. Finally, leveraging the research progress of MXene, the potential and prospects for its novel application in the Li–S field are proposed. [ABSTRACT FROM AUTHOR]

In the face of growing environmental challenges and the need for alternative energy storage, lithium‐sulfur (Li‐S) batteries stand out for their high theoretical energy density and sulfur's eco‐friendliness. However, the practical application of Li‐S batteries faces significant obstacles, particularly at the cathode and anode. This study explores the transformative impact of 2D tellurene, focusing on how its dimensional variations influence Li‐S battery performance. At the cathode, tellurene not only improves the conductivity and sulfur utilization but also accelerates the conversion of lithium polysulfides (LiPSs). Its reduced size, compared to the bulk counterpart, offers numerous active sites for efficient Li‐ion migration and promotes LiPSs decomposition. At the anode, the protective polytellurosulfides are formed, thereby establishing a stable solid‐electrolyte interphase (SEI) and enhancing reversible lithium deposition. Diminishing the dimensions of tellurene improves its catalytic interface, leading to faster polysulfide conversion kinetics at the cathode and robust SEI formation at the anode. Li‐S batteries equipped with ultra‐thin tellurene‐modified separators demonstrate exceptional performance, exhibiting high areal capacity and significantly reduced capacity decay. Computational simulations further validate the advantages of optimizing tellurene dimensions, confirming its essential role in LiPSs decomposition and overall battery efficiency. [ABSTRACT FROM AUTHOR]

Lithium‐sulfur (Li−S) batteries exhibit great potential as the next‐generation energy storage techniques. Application of catalyst is widely adopted to accelerate the redox kinetics of polysulfide conversion reactions and improve battery performance. Although significant attention has been devoted to seeking new catalysts, the problem of catalyst passivation remains underexplored. Herein, we find that metal‐N coordination has a previously overlooked role in preventing the catalyst passivation. In the case of nickel, the Ni catalyst reacts with S8 to produce NiSx compounds on the surface, leading to catalyst passivation and slow the kinetics of LiPSs conversion. In contrast, when Ni is coordinated with N (typically Ni−N4), S8 remains stable on the surface. The Ni−N4 exhibits excellent resistance to passivation and rapid kinetics of LiPSs conversion. Consequently, the sulfur cathode with Ni−N4 exhibits a high rate capability of 604.11 mAh g−1 at 3 C and maintains a low capacity decay rate of 0.046 % per cycle over 1000 cycles at 2 C. Furthermore, preventing S passivation in M−N coordination applies not only to Ni−N4 but also to various coordination numbers and transition metals. This study reveals a new aspect of metal‐N coordination in inhibiting catalyst passivation, improving our understanding of catalysts in Li−S batteries. [ABSTRACT FROM AUTHOR]

Integration of solar cell and secondary battery cannot only promote solar energy application but also improve the electrochemical performance of battery. Lithium–sulfur battery (LSB) is an ideal candidate for photoassisted batteries owing to its high theoretical capacity. Unfortunately, the researches related the combination of solar energy and LSB are relatively lacking. Herein, a freestanding photoelectrode is developed for photoassisted lithium–sulfur battery (PALSB) by constructing a heterogeneous structured Au@N‐TiO2 on carbon cloths (Au@N‐TiO2/CC), which combines multiple advantages. The Au@N‐TiO2/CC photoelectrode can produce the photoelectrons to facilitate sulfur reduction during discharge process, while generating holes to accelerate sulfur evolution during charge process, improving the kinetics of electrochemical reactions. Meanwhile, Au@N–TiO2/CC can work as an electrocatalyst to promote the conversion of intermediate polysulfides during charge/discharge process, mitigating induced side reactions. Benefiting from the synergistic effect of electrocatalysis and photocatalysis, PALSB assembled with an Au@N‐TiO2/CC photoelectrode obtains ultrahigh specific capacity, excellent rate performance, and outstanding cycling performance. What is more, the Au@N‐TiO2/CC assembled PALSB can be directly charged under light illumination. This work not only expands the application of solar energy but also provides a new insight to develop advanced LSBs. [ABSTRACT FROM AUTHOR]

Iron‐nitrogen functionalized graphene has emerged as a promising cathode host for rechargeable lithium‐sulfur batteries (RLSBs) due to its affordability and enhanced battery performance. To optimize its catalytical efficiency, we propose a novel approach involving coordination engineering. Our investigation spans a plethora of catalysts with varied coordination environments, focusing on elements B, C, N and O. We revealed that Fe−C4 and Fe−B2C2−h are particularly effective for promoting Li2S oxidation, whereas Fe‐N4 excels in catalyzing the sulfur reduction reaction (SRR). Importantly, our study identified specific descriptors – namely, the Integrated Crystal Orbital Hamilton Population (ICOHP) and the bond length between Fe and S in Li2S adsorbed state – as the most effective predictive descriptors for Li2S oxidation barriers. Meanwhile, Li2S adsorption energy emerges as a reliable descriptor for assessing the SRR barrier. These identified descriptors are expected to be instrumental in rapidly identifying promising cathode hosts across various metal‐centered systems with diverse coordination environments. Our findings not only offer valuable insights into the role of coordination environment, but also present an effective path for rapidly identifying high performance catalysts for RLSBs, enabling the acceleration of advanced RLSBs development. [ABSTRACT FROM AUTHOR]

Commercial lithium‐ion batteries are gradually approaching their theoretical specific energy, which cannot meet the fast‐growing energy storage demands. Lithium‐sulfur (Li−S) batteries are anticipated to supersede lithium‐ion batteries as the next‐generation energy storage system owing to their high atheoretical specific capacity (1675 mAh g−1) and energy density (2600 Wh kg−1). Nonetheless, Li−S batteries encounter several challenges, including the inadequate conductivity of sulfur and lithium sulfide, sulfur's volume expansion, and the shuttle effect of lithium polysulfides, all of which significantly impact the practical utilization of Li−S batteries. Electrospun carbon‐based nanofibers can simultaneously resolve these issues with their economical preparation, distinctive nanostructure, and exceptional flexibility. This review presents the most recent research findings on electrospun carbon‐based nanofibers materials serving as sulfur hosts and interlayer components in Li−S batteries. We analyzed the impact of the material's structural design on the performance of Li−S batteries and the relative underlying mechanism. Finally, the current challenges and issues faced by carbon‐based nanofibers composites in the application of Li−S batteries are summarized, and the future development trajectory are outlined. [ABSTRACT FROM AUTHOR]

The lithium–sulfur (Li–S) battery system has attracted considerable attention due to its ultrahigh theoretical energy density and promising applications. However, with the increasing demands on S loading and electrolyte content, practical Li–S batteries still face several serious challenges, such as slow reaction kinetics at the cathode interface, unstable anode interface reactions, and undesirable crosstalk effects between the cathode and anode. Traditional electrolyte systems often struggle to address these challenges under practical conditions, thereby rendering it imperative to establish a new electrolyte system for practical Li–S batteries. This review first discusses the necessity of establishing a new electrolyte and propose specific parameter requirements, such as the electrolyte‐to‐sulfur mass ratio (Em/S). Subsequently, some electrolyte modification strategies proposed by researchers are summarized to address the different challenges associated with practical Li–S batteries. Finally, the combination of different strategies is reviewed, aiming to reveal more effective design approaches that simultaneously address multiple challenges, while providing guidance for establishing a new balanced electrolyte for practical Li–S batteries. This article promotes the development of new electrolytes for practical Li–S batteries and can act as a reference for the development of electrolytes for other secondary batteries. [ABSTRACT FROM AUTHOR]

The developing electric vehicles and portable electronics urgently require rechargeable lithium batteries with high energy density and high safety. Lithium‐sulfur (Li‐S) batteries have shown significant advantages in their high energy density. However, the use of traditional polymer binders faces significant challenges, such as soluble polysulfides, large volume changes, and electrode flammability, resulting in performance degradation and safety hazards. Here, a polymeric aluminophosphate (AP) is for the first time proposed as an inorganic polymer binder to simultaneously realize high energy density, long cycling stability, and reliable safety of Li‐S batteries. Benefiting from the synergistic effect of polar P‐O and Al‐O chain segments, the AP binder provides strong mechanical adhesion, anchors polysulfides, and promotes the redox kinetics of sulfur electrodes. The AP binder also ensures high flame retardancy for sulfur electrodes at an extremely low dosage of 2 wt%. Consequently, the retardant sulfur electrode can be operated stably with high specific capacities (1190 mAh g−1), high capacity retention rates (>99.1%) during 500 cycles, and excellent rate capability (3 C). Based on the entire cell, the soft‐packaged Li‐S full battery provides high capacities (3.6 mAh cm−2), high cell energy density (415 Wh kg−1 and 297 Wh L−1), and high capacity retention rates (>99.8%). [ABSTRACT FROM AUTHOR]

Lithium–Sulfur (Li─S) batteries are renowned for their high theoretical specific capacity and cost‐effectiveness. Nevertheless, their performance could be impeded by obstacles including lithium dendrite growth and lithium polysulfide (LiPS) shuttle, particularly under harsh conditions. Herein, an economical strategy is reported for modifying polyolefin separators (PP) with covalent organic polymer networks (TPE) to alter Li solvent structure, enhance lithium‐ion transport, and suppress shuttle effects. Combining in situ/ex situ characterization and theoretical calculations, it is demonstrated that the lithiophilic groups (‐C═N‐) in the TPE@PP separator form strong interaction with lithium, facilitating the dissociation of Li─Solvent/LiPS‐solvent to release freer lithium ion and shape a stable solid electrolyte interface rich in LiF and Li3N. The polymer network serves as a "highway" that accelerates Li transport and promotes uniform nucleation behavior. Therefore, the Li|TPE@PP|CNT/S cell enables 60% capacity retention after 2000 cycles at 1.0 C and exhibits stable cycling performance of 100 cycles from ‐40 to 80 °C. Moreover, the pouch cell maintains a capacity of more than 600 mA h g−1 after 30 cycles at 0 °C. This study provides a promising avenue for the application of high‐performance batteries in harsh environment from the perspective of separator engineering. [ABSTRACT FROM AUTHOR]

Lithium–sulfur (Li–S) batteries are gaining tremendous attention as promising energy storage solutions due to their impressive energy density and the affordability of sulfur. However, the practical use of Li–S batteries encounter major obstacles such as the polysulfide shuttle effect, which leads to capacity loss and decreased cycling stability. Herein, a polyethylene imidazole/polyacrylonitrile (PVIMPAN) nanofibers‐modified Celgard separator is constructed via a facile electrospinning strategy and used as a polysulfides barrier for Li–S batteries. The electron‐deficient imidazole groups introduced on the surface of PVIMPAN separators create a barrier that prevents polysulfide shuttling and extends cycle life. Additionally, the developed PVIMPAN separator exhibits a significantly enhanced Li+ transfer number of 0.60, compared to the commercial Celgard separator (0.20). This enhancement can be attributed to the strong binding energy between imidazole groups and bis(trifluoromethanesulphonyl)imide anion, leading to improved Li plating and stripping performance. Consequently, incorporating the PVIMPAN separator into Li–S batteries enable the achievement of a discharge capacity of 786.0 mAh g−1 with close to 100% Coulombic efficiency after 500 cycles at 1C (25 °C). It is believed that this work can provide valuable insights for designing suitable and robust separators for metal–sulfur batteries. [ABSTRACT FROM AUTHOR]