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To cope with the shuttling of soluble lithium polysulfides in lithium–sulfur batteries, confinement tactics, such as trapping of sulfur within porous carbon structures, have been extensively studied. Although performance has improved a bit, the slow polysulfide conversion inducing fast capacity decay remains a big challenge. Herein, a NiS2/carbon (NiS2/C) composite with NiS2 nanoparticles embedded in a thin layer of carbon over the surface of micro-sized hollow structures has been prepared from Ni-metal–organic frameworks. These unique structures can physically entrap sulfur species and also influence their redox conversion kinetics. By improving the reaction kinetics of polysulfides, the NiS2/carbon@sulfur (NiS2/C@S) composite cathode with a suppressed shuttle effect shows a high columbic efficiency and decent rate performance. An initial capacity of 900 mAh g−1 at the rate of 1 C (1 C = 1675 mA g−1) and a low-capacity decline rate of 0.132% per cycle after 500 cycles are obtained, suggesting that this work provides a rational design of a sulfur cathode. [ABSTRACT FROM AUTHOR]

[Display omitted] The sluggish redox reaction kinetics and "shuttle effect" of lithium polysulfides (LPSs) impede the advancement of high-performance lithium-sulfur batteries (LSBs). Transition metal phosphides exhibit distinctive polarity, metallic properties, and tunable electron configuration, thereby demonstrating enhanced adsorption and electrocatalytic capabilities towards LPSs. Consequently, they are regarded as exceptional sulfur hosts for LSBs. Moreover, the introduction of a heterogeneous structure can enhance reaction kinetics and expedite the transport of electrons/ions. In this study, a composite of hollow CoP-FeP cubes with heterostructure modified carbon nanotube (CoFeP-CNTs) was fabricated and utilized as sulfur host in advanced LSBs. The presence of carbon nanotubes (CNTs) facilitates enhanced electron and Li+ transport. Meanwhile, the active sites within the heterogeneous interface of CoP-FeP suppress the "shuttle effect" and enhance the conversion kinetics of LPSs. Therefore, the CoFeP-CNTs/S electrode exhibited exceptional cycling stability and demonstrated a capacity attenuation of merely 0.051 % per cycle over 600 cycles at 1C. This study presents a highly effective tactic for synthesizing dual-acting transition metal phosphides with heterostructure, which will play a pivotal role in advancing the development of efficient LSBs. [ABSTRACT FROM AUTHOR]

This study reveals the role of thermal instability in hydrogen-substituted graphdiyne (HsGDY) and its impact on lithium–sulfur (Li–S) battery performance. HsGDY undergoes significant chemical and physical transformations when subjected to thermal heating, both in the presence and absence of sulfur. Our findings suggest that the structural transformation of HsGDY into a graphene-like structure is primarily responsible for enhancing sulfur trapping and reducing the polysulfide shuttle effect, rather than the previously hypothesized alkyne–sulfur chemical interactions. [ABSTRACT FROM AUTHOR]

The New Journal of Chemistry, published by The Royal Society of Chemistry and the Centre National de la Recherche Scientifique, features a variety of research articles on topics such as nanocrystals synthesis, luminescence efficiency improvement, and visible light photocatalysis. The journal covers a wide range of subjects, including biochemistry, pharmacology, and environmental catalysis, providing valuable insights into cutting-edge research in the field of chemistry. With a focus on innovative directions in chemistry, the journal aims to connect the global chemistry community and reinvest profits back into the field. [Extracted from the article]

[Display omitted] • Mo 2 C-Co heterostructure embedded in carbon nanosheets is designed to modify both interlayer and cathode for Li-S battery. • Mo 2 C-Co has abundant adsorption sites to adsorb polysulfides and accelerate Li+ migration. • Mo 2 C-Co enables rapid uniform deposition and complete oxidation of Li 2 S. • Superior Li-S battery performance is achieved under high rate, high sulfur loading or low temperature. The practical applications of lithium sulfur batteries (LSBs) are hindered by notorious shuttle effect and sluggish conversion kinetics of intermediate polysulfides. Herein, Mo 2 C-Co heterogeneous particles decorated two-dimensional (2D) carbon nanosheets grown on hollow carbon microtubes (CCC@MCC) are synthesized. Three-dimensional (3D) carbon framework with Mo 2 C-Co heterogeneous particles combines the conductivity, adsorption and catalysis, effectively trapping and accelerating the conversion of polysulfides. As evidenced experimentally, the hetero-structured Mo 2 C-Co with high Li+ diffusion coefficient enables uniform precipitation and complete oxidation of Li 2 S. Meanwhile, CCC@MCC is found to have multiple application possibilities for lithium-sulfur batteries. As an interlayer, the cells deliver an excellent capacity of 881.1 mAh/g at 2C and still retain 438.2 mAh/g after 500 cycles under the low temperature of 0 ℃. As a sulfur carrier, the cell with a sulfur loading of 7.0 mg cm−2 exhibits a high area capacity of 5.3 mAh cm−2. This work provides an effective strategy to prepare heterostructured material and imaginatively exploit the application potential of it. [ABSTRACT FROM AUTHOR]

A covalent organic frameworks (COFs) material with regular pores and stable structure can be used as the host of lithium-sulfur batteries to improve battery kinetics and polysulfides conversion. Herein, we designed and synthesized two kinds of rod-liked bulk COFs by adjusting different pore sizes (COF-BTD and COF-TFB), unfortunately, the active sites masking and sluggish kinetics have not met our expectations. Generally, the available layered COFs prepared from mechanochemical can expose abundant active sites and favorable kinetics than bulk COFs. Thus, simple mechanical ball milling is applied to activate the above COFs (M-COFs group). It is worth noting that layered R--COF--BTD is directly synthesized from rod-liked precursors by simple morphological reconstruction. A series of characterization methods are used to systematically explore the advantages of the group of M-COFs@S electrodes in the cycling process, including the effects of specific morphology on the kinetics and transformation of polysulfides. Our research provides a feasible plan for the development and selection of the host material of lithium-sulfur batteries. [ABSTRACT FROM AUTHOR]

This study introduces a novel approach to inverse vulcanization by utilizing a commercially available triaziridine crosslinker as an alternative to conventional olefin‐based crosslinkers. The model reactions reveal a self‐catalyzed ring‐opening of “unactivated” aziridine with elemental sulfur, forming oligosulfide‐functionalized diamines. The triaziridine‐derived polysulfides exhibit impressive mechanical properties, achieving a maximum stress of ~8.3 MPa and an elongation at break of ~107 %. The incorporation of silicon dioxide (20 wt %) enhances the composite's rigidity, yielding a Young's modulus of ~0.94 GPa. Furthermore, these polysulfides display excellent adhesion strength on various substrates, such as aluminum (~7.0 MPa), walnut (~9.6 MPa), and steel (~11.0 MPa), with substantial retention of adhesion strength (~3.3 MPa on steel) at −196 °C. The straightforward synthetic process, combined with the accessibility of the triaziridine crosslinker, emphasizes the potential for further innovations in sulfur polymer chemistry. [ABSTRACT FROM AUTHOR]

The realization of a low negative/positive capacity (N/P) ratio is essential for attaining high energy density in lithium‐sulfur batteries (LSBs). However, it has been challenging to maintain the stability of the Li metal anode at low N/P ratios. Herein, it is revealed that the corrosion of the Cu current collector by dissolved intermediates of polysulfides ‐a largely overlooked perspective‐ significantly contributes to the instability of Li metal anode at low N/P ratios. The reduced Li/Li+ redox rates on the corroded Cu surface result in uneven and porous Li deposits that severely deteriorate cycling stability. To address this issue, an anti‐corrosion alloy coating is developed to passivate the Cu surface against polysulfides. LSBs with passivated current collectors at a low N/P ratio (1.5) and lean electrolyte (5 µL mgs −1) show a ten fold extension in cycle and calendar life. This study not only provides the initial evidence of the impact of Cu corrosion on the failure mechanism of low N/P ratio LSBs but also proposes a practical yet effective strategy to stabilize high‐energy‐density LSBs. [ABSTRACT FROM AUTHOR]

Developing a deep understanding of the fascinating properties of MFM-300 (MFM = Manchester framework material) opens up a world of new and thrilling applications. The unique dynamic metal–ligand bonding for MFM-300(Sc) and MFM-300(In) is chronologically presented here, highlighting the exacting applications that were associated with such special behaviour (i.e., description of complex NH3 adsorption mechanisms, conversion of toxic H2S to polysulfides for promising fabrication of lithium–sulphur batteries and heterogeneous catalysis). This highlight aims to showcase the current advances in semi-open metal sites inherent to MFM-300(Sc) and MFM-300(In) to inspire new investigations to be carried out to develop new applications of this promising family of MOF materials. [ABSTRACT FROM AUTHOR]

Lithium‐sulfur (Li−S) batteries, recognized as one of the most promising next‐generation energy storage systems, are still limited by the "shuttle effect" of soluble polysulfides (LiPSs) on the cathode and the uncontrolled growth of lithium dendrites on the anode. These issues are critical obstacles to their practical application. Currently, many researchers have addressed these challenges from a unilateral perspective. Herein, we propose bifunctional hosts based on high‐entropy selenides (HE−Se) to simultaneously tackle the persistent problems on both the positive and negative electrodes of Li−S batteries. On the one hand, HE−Se interacts with polysulfides to promote their conversion, effectively mitigating the shuttle effect. On the other hand, HE−Se provides multiple lithophilic sites during the initial nucleation of Li+, which reduces overpotential and exhibits excellent lithophilicity and cyclic stability. As a result, Li−S batteries incorporating the HE−Se hosts demonstrate outstanding performance in terms of rate capability and cycling stability. Additionally, the porous lithophilic HE−Se structure offers sufficient nucleation sites, inhibits the growth of dendritic lithium, and accommodates volume changes during charging and discharging cycles. This study highlights the potential of sulphophilic/lithophilic high‐entropy materials in designing advanced Li−S batteries and encourages further exploration in this area. [ABSTRACT FROM AUTHOR]

Lithium–sulfur batteries (LSBs) exhibit high theoretical specific capacities, abundant resource reserves, and low costs, making them promising candidates for next-generation lithium-ion batteries (LIBs). However, significant challenges, such as the shuttle effect and volume expansion, hinder their practical applications. To address these issues, this study introduces a unique intermediate layer comprising N-doped carbon nanofiber/TiO2/diatomite (NCNF/TiO2/DE) from the perspective of membrane modification. The intermediate layer comprises nitrogen-doped titanium dioxide/carbon nanofiber (NCNF/TiO2) materials, with diatomite filling the fiber gaps. This forms a three-dimensional (3D) conductive network that provides ample space for sulfur volume expansion and numerous adsorption active sites, thereby accelerating electrolyte penetration and lithium-ion diffusion. These features collectively contribute to the outstanding electrochemical performance of the battery. At 0.1 C, the NCNF/TiO2/DE-800-coated separator battery achieved a first-cycle discharge specific capacity of 1311.1 mAh g−1, significantly higher than the uncoated lithium–sulfur battery (919.6 mAh g−1). Under varying current densities, the NCNF/TiO2/DE-800 material demonstrates good electrochemical reversibility and exhibits high lithium-ion diffusion rates and low charge-transfer resistance. Therefore, this study provides an advanced intermediate layer material that enhances the electrochemical performance of lithium–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]

Carbazole-based COFs were synthesized and applied as the sulfur-host in cathode materials for lithium–sulfur batteries (LSBs), which effectively mitigate the shuttle effect of lithium polysulfides. A high initial capacity of 1232 mAh g−1 at 0.1C is achieved, while also showing excellent capacity retention and stability in cyclic experiments. This work highlights the potential application of carbazole-based COFs for LSBs. [ABSTRACT FROM AUTHOR]

The practical development of Li | |S batteries is hindered by the slow kinetics of polysulfides conversion reactions during cycling. To circumvent this limitation, researchers suggested the use of transition metal-based electrocatalytic materials in the sulfur-based positive electrode. However, the atomic-level interactions among multiple electrocatalytic sites are not fully understood. Here, to improve the understanding of electrocatalytic sites, we propose a multi-view machine-learned framework to evaluate electrocatalyst features using limited datasets and intrinsic factors, such as corrected d orbital properties. Via physicochemical characterizations and theoretical calculations, we demonstrate that orbital coupling among sites induces shifts in band centers and alterations in the spin state, thus influencing interactions with polysulfides and resulting in diverse Li-S bond breaking and lithium migration barriers. Using a carbon-coated Fe/Co electrocatalyst (synthesized using recycled Li-ion battery electrodes as raw materials) at the positive electrode of a Li | |S pouch cell with high sulfur loading and lean electrolyte conditions, we report an initial specific energy of 436 Wh kg−1 (whole mass of the cell) at 67 mA and 25 °C. The atomic-level interactions among electrocatalytic sites in Li | |S batteries remain unclear. Here, authors propose a multiview machine-learned framework to evaluate electrocatalyst features using limited datasets and intrinsic factors, thus enhancing the understanding of electrocatalytic sites. [ABSTRACT FROM AUTHOR]

To address the inherent limitations of conventional carbon nanotubes (CNTs), such as their tendency to agglomerate and scarcity of catalytic sites, the development of branched carbon nanotubes (BCNTs) with a unique hierarchical structure has emerged as a promising solution. Herein, gram scale quantities of densely branched and structurally consistent Ni−Fe decorated branched CNTs (Ni−Fe@BCNT) have been prepared. This uniform and densely branched architecture ensures excellent dispersibility and superior electrical conductivity. Additionally, each branched tip is equipped with Ni−Fe particles, thereby providing numerous catalytic sites which endow them with exceptional catalytic activity for the conversion of polysulfides. The polypropylene (PP) separator modified with Ni−Fe@BCNT interlayer is fabricated as a multifunctional barrier for Li–S batteries. The experimental results demonstrate that Ni−Fe@BCNT interlayer can effectively suppress the shuttle effect of polysulfides and enhance their redox kinetics. The outstanding catalytic ability of Ni−Fe@BCNT interlayer enables batteries with high specific capacities, outstanding rate performance, and remarkable cycling stability. This approach proposed in this work paves a new path for synthesizing BCNTs and shows great potential for scaling up the production of BCNTs to address more demanding applications. [ABSTRACT FROM AUTHOR]

Lithium sulfide (Li2S) is a promising electrode material with high specific capacity and can be paired with commercial anode materials such as graphite. However, bulk Li2S requires a high activation energy during the initial charge due to its inert electrochemical activity, resulting in high charge overpotential. Here, lithium phenyl selenide (PhSeLi) is proposed as a mediator that can effectively activate Li2S by altering the oxidation pathway in the initial charge process. It enables Li2S to release normal capacity over the general voltage range (1.5–3 V). The composite cathode with the Li2S:PhSeLi molar ratio of 4:1 exhibits a high reversible capacity of 615.9 mAh g−1 at 0.2 A g−1 after 400 cycles in all‐solid‐state batteries with Li7P3S11 sulfide electrolyte and In–Li anode (the corresponding capacity based on Li2S is 1016.6 mAh g−1). In a full cell with a partially pre‐lithiated silicon anode, it can still provide an average discharge capacity of 524 mAh g−1 at 0.1 A g−1 (the capacity based on Li2S is 844.2 mAh g−1). This work will contribute to the further development of Li2S‐based all‐solid‐state Li–S batteries. [ABSTRACT FROM AUTHOR]

Lithium‐sulfur (Li‐S) batteries, with their high theoretical energy density and cost‐effectiveness, have become one of the most promising next‐generation energy storage devices. However, they still face challenges such as the “shuttle effect” caused by the dissolution of polysulfide intermediates and the slow sulfur conversion kinetics. In this study, based on the Co7Fe3 alloy catalyst, additional Co metal is introduced to form a Co7Fe3Co catalyst with a heterostructure through a simple heat treatment process. This catalyst is incorporated into Ketjenblack (KB) to form a sulfur‐infused cathode material (designated as S/KB/Co7Fe3Co). Li‐S batteries using S/KB/Co7Fe3Co as the cathode demonstrate outstanding electrochemical performance, maintaining a reversible specific capacity of over 500 mAh g−1 after 1000 cycles at a current density of 1 C, with a capacity decay rate of 0.046% per cycle. DFT theoretical calculations and experimental results both reveal that the introduction of additional Co effectively regulates the d‐band center of the material, enhancing the adsorption of polysulfide intermediates by Co7Fe3Co and promoting bidirectional catalytic sulfur conversion. This work highlights the importance of the simple construction of heterostructured catalytic materials and their role in improving the performance of Li‐S batteries. [ABSTRACT FROM AUTHOR]

Electrolyte and interfacial engineering of photoanodes has become a crucial approach to enhance photoelectrochemical water-splitting performance. By optimizing both the electrolyte and the interfacial properties of the photoanode, the synergistic effects of the heterojunction and electrolyte can be leveraged to improve efficiency. In this work, we explore the crucial role of electrolyte and interfacial engineering in optimizing photoanode performance. By engineering an In 2 O 3 film in a polysulfide electrolyte to form an in-situ In₂S₃/In₂O₃ heterojunction interface, we demonstrate a significant increase in anodic photocurrent compared to traditional aqueous Na 2 SO 4 or NaOH electrolytes. This enhancement is attributed to both the thermodynamically favorable oxidation of sulfide and sulfite, and the unique electronic structure developed at the In₂S₃/In₂O₃ junction, which significantly improves charge separation and overall performance. Based on this finding, an efficient In₂S₃/In₂O 3 heterojunction interface through optimal anion exchange with sulfur was developed, leading to a maximum photocurrent density of 5.57 mA cm−2 in the polysulfide electrolyte. In addition, detailed structural, optical, and photoelectrochemical properties of the In₂S₃/In₂O₃ interface providing insights into the mechanisms underlying the enhanced water-splitting performance have also been discussed. [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]

This study addresses the persistent challenge of polysulfide dissolution in lithium–sulfur (Li–S) batteries by introducing magnesium oxide (MgO) nanoparticles as a novel additive. MgO was integrated with sulfur using a scalable process involving solid-state melt diffusion treatment followed by planetary ball milling. XRD measurements confirmed that sulfur (S8) retains its orthorhombic crystalline structure (space group F d d d ) following the MgO incorporation, with minimal peak shifts indicating slight lattice distortion, while the increased peak intensity suggests enhanced crystallinity due to MgO acting as a nucleation site. Additionally, Raman spectroscopy demonstrated sulfur's characteristic vibrational modes consistent with group theory (point group D 2 h ) and highlighted multiwalled carbon nanotube (MWCNT′s) D, G, and 2D bands, with a low ID/IG ratio (0.47), which indicated low defects and high crystallinity in the prepared cathode. The S–MgO composite cathode exhibited superior electrochemical behavior, with an initial discharge capacity (950 mA h g−1 at 0.1 C), significantly improved compared to pristine sulfur's. The presence of MgO effectively mitigated the polysulfide shuttle effect by trapping polysulfides, leading to enhanced stability over 400 cycles and the consistent coulombic efficiency of over 99.5%. After 400 cycles, EDS and SEM analyses confirmed the structural integrity of the electrode, with only minor fractures and slight sulfur content loss. Electrochemical impedance spectroscopy further confirmed the enhanced performance. [ABSTRACT FROM AUTHOR]

Li–S batteries are promising large-scale energy storage systems but currently suffer from performance issues; a major reason is the dissolution of polysulfides in electrolytes. To this end, we report a high-energy-density Lithium–Sulfur (Li–S) battery that combines a catholyte and a sulfur-free carbon nanofiber (CNF) cathode. The cathode was synthesized by carbonizing binder-free polyacrylonitrile (PAN) nanofibers, affording a high surface area. In the catholyte, added polysulfides acted as both conductive Li salts and active materials. Investigating the electrochemical performance of this concept in both Swagelok- and pouch-type cells afforded energy densities exceeding 3 mAh cm−2 at a discharge rate of 0.1 C. This combination could also be utilized in high-capacity pouch cells with capacities of up to 250 mAh g−1. Both cell types exhibited good cycle performance. Adding LiNO3 to the electrolyte suppressed the redox shuttle reactions. Moreover, the cathode being binder-free increased the energy density and simplified cathode fabrication. Characterizing the cathode before and after cycling revealed that deposition was reversible, and that cell reactions at least partially formed sulfur as the end product, resulting in high sulfur amounts in the cell. We expect our concept to greatly aid in the development of practically applicable Li–S cells. [ABSTRACT FROM AUTHOR]

Despite concerns regarding safety, economics, and the environment, lithium-ion batteries (LIBs) are considerably utilized on account of their low energy density and capacity. Li–sulfur (Li–S) batteries have become a promising substitute for LIBs. Here, we first compared both systems in their cons and pros and analyzed the leading countries and companies in Li–S research are assessed through the utilization of an academic database. The scope of our research includes performance-enhancing design elements, cathode components, and binder materials. Synthetic and natural binders are trialed in an effort to enhance Li–S performance. Understanding the fundamental mechanisms enables the development of durable cathodes and binders. To overcome obstacles such as polysulfide adsorption, shuttle effect, and ion transport limitations, conducting polymers, metal/metal oxides, carbon-based compounds, MOFs, and Mxenes are investigated as potential cathode materials. In addition to pore characteristics and active polar sites, the efficacy of a battery is influenced by the anode surface geometry and heteroatom doping. Our review indicates that binders and sulfur/host composites must be meticulously chosen for Li–S battery cathode materials. This research advances energy storage technology by establishing the foundation for economically viable lithium–sulfur batteries with superior performance. [ABSTRACT FROM AUTHOR]

Lithium‐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. [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 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]

The photo‐assisted strategy is regarded as a crucial approach to enhance the conversion kinetics of polysulfides in lithium–sulfur (Li–S) batteries. However, the development of photo‐assisted Li–S batteries still faces important challenges, such as the rapid recombination of photogenerated electron−holes on cathode and more severe shuttle effect. Herein, a breakthrough in overcoming the challenges has been made by constructing a promising photo‐assisted Li−S battery based on semiconducted metal−organic frameworks. During the discharging progress, the photoexcited electrons generated by H2BPDC ligand based on ligand‐to‐metal charge transfer (LMCT) effect, are injected into the Ti‐oxo clusters in Ti‐MOF, thereby facilitating the sulfur reduction to Li2S. And photoexcited holes are capable of promoting the decomposition kinetics of Li2S during charging. More importantly, the stronger chemical interaction between Ti‐BPDC‐d and polysulfides under light inhibits the polysulfides dissolution and shuttling, which fundamentally addresses the issue of light‐accelerated shuttling. As a result, the photo‐assisted Li–S batteries deliver a reversible capability of 1090.21 mAh g−1 at 0.2 C with a capacity retention of 82.91% over 150 cycles, and a superior rate capability of 673.58 mAh g−1 at 5 C. The findings are promising in advancing the design principles for photo‐rechargeable Li−S batteries. [ABSTRACT FROM AUTHOR]

Lithium‐sulfur batteries (LiSBs) with high energy density still face challenges on sluggish conversion kinetics, severe shuttle effects of lithium polysulfides (LiPSs), and low blocking feature of ordinary separators to LiPSs. To tackle these, a novel double‐layer strategy to functionalize separators is proposed, which consists of Co with atomically dispersed CoN4 decorated on Ketjen black (Co/CoN4@KB) layer and an ultrathin 2D Ti3C2Tx MXene layer. The theoretical calculations and experimental results jointly demonstrate metallic Co sites provide efficient adsorption and catalytic capability for long‐chain LiPSs, while CoN4 active sites facilitate the absorption of short‐chain LiPSs and promote the conversion to Li2S. The stacking MXene layer serves as a microscopic barrier to further physically block and chemically anchor the leaked LiPSs from the pores and gaps of the Co/CoN4@KB layer, thus preserving LiPSs within efficient anchoring‐conversion reaction interfaces to balance the accumulation of "dead S" and Li2S. Consequently, with an ultralight loading of Co/CoN4@KB‐MXene, the LiSBs exhibit amazing electrochemical performance even under high sulfur loading and lean electrolyte, and the outperforming performance for lithium‐selenium batteries (LiSeBs) can also be achieved. This work exploits a universal and effective strategy of a double‐layer functionalized separator to regulate the equilibrium adsorption‐catalytic interface, enabling high‐energy and long‐cycle LiSBs/LiSeBs. [ABSTRACT FROM AUTHOR]

The catalytic process of Li2S formation is considered a key pathway to enhance the kinetics of lithium‐sulfur batteries. Due to the system's complexity, the catalytic behavior is uncertain, posing significant challenges for predicting activity. Herein, we report a novel cascaded dual‐cavity nanoreactor (NiCo−B) by controlling reaction kinetics, providing an opportunity for achieving hierarchical catalytic behavior. Through experimental and theoretical analysis, the multilevel structure can effectively suppress polysulfides dissolution and accelerate sulfur conversion. Furthermore, we differentiate the adsorption (B−S) and catalytic effect (Co−S) in NiCo−B, avoiding catalyst deactivation caused by excessive adsorption. As a result, the as‐prepared battery displays high reversible capacity, even with sulfur loading of 13.2 mg cm−2 (E/S=4 μl mg−1), the areal capacity can reach 18.7 mAh cm−2. [ABSTRACT FROM AUTHOR]

Herein, MoS2 quantum dots (QDs) are constructed to serve as electrolyte additives for lithium–sulfur batteries, which can 'solidify' soluble polysulfides by chemisorption and promote sulfur conversion chemistry by electrocatalysis. The Li–S cell with MoS2 QDs shows high retained capacity and high-rate capability, much better than the counterpart without MoS2 QDs. [ABSTRACT FROM AUTHOR]

High‐performance rechargeable aluminum‐sulfur batteries (RASB) have great potential for various applications owing to their high theoretical capacity, abundant sulfur resources, and good safety. Nevertheless, the practical application of RASB still faces several challenges, including the polysulfide shuttle phenomenon and low sulfur utilization efficiency. Here, we first developed a synergistic copper heterogeneous metal oxide MoO2 derived from polymolybdate‐based metal‐organic framework as an efficient catalyst for mitigating polysulfide diffusion. This composite enhances sulfur utilization and electrical conductivity of the cathode. DFT calculations and experimental results reveal the catalyst Cu/MoO2@C not only effectively anchors aluminum polysulfides (AlPSs) to mitigate the shuttle effect, but also significantly promotes the catalytic conversion of AlPSs on the sulfur cathode side during charging and discharging. The unique nanostructure contains abundant electrocatalytic active sites of oxide nanoparticles and Cu clusters, resulting in excellent electrochemical performance. Consequently, the established RASB exhibits an initial capacity of 875 mAh g−1 at 500 mA g−1 and maintains a capacity of 967 mAh g−1 even at a high temperature of 50 °C. [ABSTRACT FROM AUTHOR]

Background: Hydrogen sulfide (H2S) is an endogenous transmitter with the potential to regulate aqueous humor dynamics and protect retinal neurons from degeneration. The aim of the present study was two-fold: (a) to evaluate the release of H2S from two polysulfides, diallyl disulfide (DADS), and diallyl trisulfide (DATS); and (b) to investigate their ocular hypotensive actions in normotensive male and female rabbits in the presence and absence of GSH. Materials and Methods: H2S was quantified hourly for up to 6 h using a H2S-Biosensor (World Precision Instruments, Sarasota, Fl). Intraocular pressure (IOP) was assessed in normotensive New Zealand Albino rabbits using a pneumotonometer (model 30 classic; Reichert Ophthalmic Instruments, Depew, NY, USA). Results: In the presence of GSH, there was an increase in the in vitro release of H2S produced by DADS and DATS. Both DADS and DATS also caused a dose-dependent reduction in IOP in male and female rabbits, in both treated and untreated eyes. For instance, in male animals, the presence of GSH (3% and 5%) significantly (p < 0.05, n = 5) enhanced the ocular hypotensive action of DADS (2%) and DATS (2%) from 14.02 ± 2.89% to 18.67 ± 5.6% and from 16.22 ± 3.48 to 23.62 ± 5.79%, respectively. Conclusions: GSH enhanced both H2S release and ocular hypotensive action of the polysulfides in a manner that was dependent on the number of sulfur atoms present in each polysulfide. Furthermore, female animals were less sensitive to the IOP-lowering action of the polysulfides, when compared to their male counterparts. [ABSTRACT FROM AUTHOR]

Inverse vulcanization utilizes alkenyl monomers and elemental sulfur, an excessive by-product of oil and gas refineries, to synthesize dynamically crosslinked sulfur-rich polymers, therefore providing a new way to construct sustainable and versatile materials. The inverse vulcanization of the biological extracts and natural polymers gives rise to a variety of bio-based polysulfides aligning with the concept of green chemistry. In this paper, the development of synthesis strategies, corresponding mechanisms, scope of renewable cross-linking agents, and the properties as well as the potential applications of polysulfides are reviewed. In particular, the progress in the preparation of various polysulfides from fossil resources to bio-based counterparts is deliberated with multiple modification methods elucidated. The bio-derived polysulfides are proved to be outstanding materials and prominent alternatives for traditional petroleum-based products especially for the use as effective ion absorbents, Li-S battery cathode materials, adhesives and controlled release fertilizers, etc. Finally, a few prospects and challenges about the future of these intriguing sulfur-based polymers are raised and discussed. [ABSTRACT FROM AUTHOR]

A novel method for the speciation and quantification of polysulfide anions and molecular sulfur in lithium polysulfide solutions in organic solvents is reported. The technique is based on hyphenation of highperformance liquid chromatography (HPLC) and inductively coupled plasma mass spectrometry (ICPMS). A sector-field mass-spectrometer was utilized which made it possible to quantify various sulfur compounds without the need for single component standards and conduct the direct detection of the main isotope of sulfur regardless of interferents such as highly abundant 16O2. Key aspects of separation and sample preparation were considered which allowed complete separation of derivatized polysulfide anions. Gradual adjustment of essential parameters and hardware is described. Variation of plasma settings allowed for obtaining chromatograms with desired analyte peak shapes. The optimized method was applied for the quantification of various lithium polysulfide mixtures in organic solvents showing the accessibility of the corresponding polysulfide distributions with this technique. [ABSTRACT FROM AUTHOR]

Cationic lithium polysulfides (LiPSs) within ether‐based electrolytes are essential intermediates pivotal in instigating the shuttle effect. Suppressing the generation of cationic LiPSs is crucial for enhancing the performance of high‐energy‐density Li‐S batteries in practical applications. Herein, for the first time, it is demonstrated that cobalt phthalocyanine (CoPc) can significantly enhance the dissociation of LiPSs, leading to a decrease in cationic LiPSs species within the electrolyte. Employing NMR and in‐situ Raman spectroscopy, it is observed that CoPc interacts with sulfur anions within LiPSs, modifying the dissociation equilibrium of LiPSs in 1,2‐dimethoxyethane (DME)/1,3‐dioxolane (DOL) electrolyte. This CoPc‐mediated shift toward dissociation equilibrium reduces the concentration of cationic LiPSs, effectively suppressing the electromigration of LiPSs intermediates toward the Li anode during the charging process of Li‐S battery. As a result, the Li‐S battery enabled a high reversible areal capacity of 4.2 mAh cm−2 at a high sulfur loading of 5.0 mg cm−2 and a low electrolyte/sulfur (E/S) ratio of 3 µL mgs−1. This work affords a promising strategy for tackling the fundamental challenges regarding Li‐S batteries. [ABSTRACT FROM AUTHOR]

The dissolution/shuttling of sodium polysulfides, coupled with sodium dendrites growth, severely compromises the lifespan and stability of room temperature sodium–sulfur (RT Na–S) batteries. Herein, it proposes employing a functionalized porous ZIF‐based membrane (PZM) to address these two challenges. First, the metal ions embedded within the zeolitic imidazolate framework chemically bind with polysulfide anions, curtailing their detrimental shuttling. Second, the tailored porous structure of the membrane ensures a selective and uniform pathway for sodium ions, significantly reducing non‐uniform deposition and curbing dendritic sodium growth. Third, the intrinsically non‐combustible nature of the ZIF‐based membrane acts as a fortification against thermal outbursts and electrolyte decomposition. Implementing this polysulfide‐resistant, dendrite‐inhibiting and flame‐retardant PZM with a standard S/C cathode leads to the creation of a robust separator with lean electrolyte RT Na–S battery. This configuration may impart a novel perspective for the advancement and enhancement of RT Na–S battery systems. [ABSTRACT FROM AUTHOR]

Sulfur-containing dynamic polymers had attracted significant attention due to their unique chemical structures with high reversibility. Utilizating sulfur, an inexpensive industrial waste product, to synthesize dynamic polysulfide polymers through reverse vulcanization has been a notable approach. However, this method required high temperatures and resulted in the release of unpleasant oders. In this study, we presented a robust method for the preparation of sulfur-rich polymers with dynamic polysulfide bonds from elemental sulfur and inexpensive epoxide monomers via a one-pot strategy at the mild room temperature. Different types of polysulfide molecules and polymers were synthesized by reacting various epoxide compounds with sulfur, along with the investigation of their structures and dynamic behaviors. It was noteworthy that the obatined polymers prepared from m-(2,3-epoxypropoxy)-N,N-bis(2,3-epoxypropyl)aniline and elemental sulfur exhibit multiple dynamic behaviors, including polysulfide metathesis and polysulfide-thiol exchange, enabling their rapid stress relaxation, self-healing, reprocessing and degradable properties of the cross-linked polymer. More importantly, the hydroxyl groups at the side chains from epoxide ring opening exhibited potential transesterification. This work provided a facile strategy for designing dynamic sulfur-rich polymers via a mild synthesis route. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Room‐temperature sodium‐sulfur (RT‐Na/S) batteries display attractive potential in large‐scale energy‐storage, but their practical application was still restricted by the serious dissolution of polysulfides. Herein, supported by the constructing of interface engineering, the metal sulfide‐carbon nanocomposite can be prepared with considerable electrochemical properties. Utilizing the double‐helix structure of carrageenan‐metal hydrogels as precursors, in‐situ metal sulfide (MxSy) nanostructure/3D carbon aerogels (3D CAs) can be successfully constructed. Importantly, with the assistance of the vulcanization process, 3D carbon architecture was maintained in the composites and acted as a skeleton to optimize their structural stability. As the cathode of RT‐Na/S batteries, ZnS/S@C and NiS2/S@C delivered an excellent cycling stability and rate performance (179.8 mAh·g−1 at 20 A·g−1 after 10000 cycling for ZnS/S@C, 220.3 mAh·g−1 at 10 A·g−1 after 3000 cycling for NiS2/S@C). The detailed investigation of mechanism revealed that the powerful adsorption for Na2S4 originated from 3D metal sulfide‐carbon structure. The well‐designed architecture of sulfide‐carbon composites servers as an electrocatalyst to alleviate the shuttle effect of polysulfides, resulting in the long‐term electrochemical stability. Given this, the work is expected to provide promising insights for designing advanced cathode materials for RT‐Na/S batteries. [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]

Although Li-S batteries have a high theoretical capacity, their application are significantly hindered by the complex shuttle effect of polysulfides. To address the issues, in this paper, Ni² V2 O7 prepared by a simple method is proposed as an efficient catalyst for S cathodes. Ni² V2 O7 composed of Ni-O octahedra and V-O tetrahedra has a specific electronic structure. The Ni and V atoms interacted, enabling a fast kinetics of polysulfide redox. Moreover, Ni² V2 O7 contains metal sites (Ni and V) and oxygen vacancies, providing a high adsorption capacity and abundant active sites for polysulfide redox. Therefore, Li-S batteries consisting of Ni² V2 O7 -based cathodes exhibit an excellent cycling stability with a capacity of 1061 mAh g-1 and capacity retention of 87.6% after 150 cycles at 0.2 C. Moreover, at 1 C rate, the batteries exhibit a capacity of 706 mAh g-1 after 300 cycles with a minimal capacity decay of only 0.08% per cycle. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Room‐temperature sodium‐sulfur (RT‐Na/S) batteries display attractive potential in large‐scale energy‐storage, but their practical application was still restricted by the serious dissolution of polysulfides. Herein, supported by the constructing of interface engineering, the metal sulfide‐carbon nanocomposite can be prepared with considerable electrochemical properties. Utilizing the double‐helix structure of carrageenan‐metal hydrogels as precursors, in‐situ metal sulfide (MxSy) nanostructure/3D carbon aerogels (3D CAs) can be successfully constructed. Importantly, with the assistance of the vulcanization process, 3D carbon architecture was maintained in the composites and acted as a skeleton to optimize their structural stability. As the cathode of RT‐Na/S batteries, ZnS/S@C and NiS2/S@C delivered an excellent cycling stability and rate performance (179.8 mAh·g−1 at 20 A·g−1 after 10000 cycling for ZnS/S@C, 220.3 mAh·g−1 at 10 A·g−1 after 3000 cycling for NiS2/S@C). The detailed investigation of mechanism revealed that the powerful adsorption for Na2S4 originated from 3D metal sulfide‐carbon structure. The well‐designed architecture of sulfide‐carbon composites servers as an electrocatalyst to alleviate the shuttle effect of polysulfides, resulting in the long‐term electrochemical stability. Given this, the work is expected to provide promising insights for designing advanced cathode materials for RT‐Na/S batteries. [ABSTRACT FROM AUTHOR]

[Display omitted] • Bimetallic POM was used to synthesize metal cation doped 1T-2H MoS 2 heterostructure. • Vanadium induces the phase transition and stabilizes the metallic 1T phase MoS 2. • Vanadium enhances the active electronic states, improves the sulfur redox kinetics. • A discharge capacity of 4.98 mAh cm−2 is obtained with S loading of 5.41 mg cm−2. The active electronic states in 1T-MoS 2 are highly desirable for catalyzing polysulfides conversion. However, stable 1T-MoS 2 is difficult to produce using common approaches. Herein, V uniformly doped in-plane 1T-2H heterostructured MoS 2 nanosheets (V-MoS 2) are prepared by a facile hydrothermal method with a polyoxometalate precursor containing periodic Mo and V atomic arrangement. The doping of V induces the phase transition from semiconducting 2H-MoS 2 to metallic 1T-MoS 2 and stabilizes the resulted 1T phase. Importantly, the incorporation of V not only modifies the surface electronic property of MoS 2 , enhancing the active site density, but also improves the adsorption of polysulfides and the catalytic efficiency for sulfur redox reactions. With these advantages, the Li-S batteries using V-MoS 2 electrocatalyst achieve accelerated reaction kinetics and superior electrochemical performance. When the S loading of the cathode is 5.41 mg cm−2, a favorable discharge capacity of 4.98 mAh cm−2 is obtained with satisfying cycle stability. This work provides an efficient atomic engineering approach for the design of high performance electrocatalyst for Li-S batteries. [ABSTRACT FROM AUTHOR]

[Display omitted] • A novel high-entropy Co 0.29 Ni 0.15 Fe 0.33 Cu 0.16 Ca 3.9 (PO 4) 3 (OH) was synthesized modified separator in Li-S battery. • Multiple metals in HE-CHP synergistically enhance the enrichment of active sites and catalytic activity, contributing to the capture and conversion of LiPSs. • The HE-CHP modified separator exhibits superb electrochemical performance in Li-S batteries. • The HE-CHP based Li-S pouch cell realizes 432 Wh/kg. The shuttle effect of lithium polysulfides (LiPSs) significantly hinders the practical application of lithium-sulfur batteries (LSBs). Herein, a high-entropy hydroxyphosphate (Co 0.29 Ni 0.15 Fe 0.33 Cu 0.16 Ca 3.9 (PO 4) 3 (OH), denoted as HE-CHP), was synthesized by metal cation exchange with calcium hydroxyphosphate (CHP) and then coated on polypropylene (PP) separators to suppress the shuttling of LiPSs. Density functional theory calculations indicated that the various introduced metal cations could effectively modulate the binding strength of soluble polysulfides and enhance the reaction kinetics of LiPSs conversion. As a result, LSBs using the HE-CHP@PP separator exhibited an excellent discharge capacity (1297 mAh g−1 under 0.2 C) and a slow capacity decay during long-term cycling (0.046 % per cycle at 2 C). At a sulfur loading of up to 6.5 mg cm−2, the LSB with HE-CHP@PP separator displayed a discharge capacity of 5.8 mAh cm−2. Notably, the CNT@S||Li Li-S pouch cell with HE-CHP modified separator delivered an initial energy density of 432 Wh kg−1. [ABSTRACT FROM AUTHOR]

[Display omitted] Lithium-sulfur batteries (LSBs) have been increasingly recognized as a promising candidate for the next-generation energy-storage systems. This is primarily because LSBs demonstrate an unparalleled theoretical capacity and energy density far exceeding conventional lithium-ion batteries. However, the sluggish redox kinetics and formidable dissolution of polysulfides lead to poor sulfur utilization, serious polarization issues, and cyclic instability. Herein, sulfiphilic few-layer MoSSe nanoflake decorated on graphene (MoSSe@graphene), a two-dimensional and catalytically active hetero-structure composite, was prepared through a facile microwave method, which was used as a conceptually new sulfur host and served as an interfacial kinetic accelerator for LSBs. Specifically, this sulfiphilic MoSSe nanoflake not only strongly interacts with soluble polysulfides but also dynamically promotes polysulfide redox reactions. In addition, the 2D graphene nanosheets can provide an extra physical barrier to mitigate the diffusion of lithium polysulfides and enable much more uniform sulfur distribution, thus dramatically inhibiting polysulfides shuttling meanwhile accelerating sulfur conversion reactions. As a result, the cells with MoSSe@graphene nanohybrid achieved a superior rate performance (1091 mAh/g at 1C) and an ultralow decaying rate of 0.040 % per cycle after 1000 cycles at 1C. [ABSTRACT FROM AUTHOR]

Abstract Room‐temperature sodium‐sulfur (RT Na‐S) batteries are a promising next‐generation energy storage device due to their low cost, high energy density (1274 Wh kg−1), and environmental friendliness. However, RT Na‐S batteries face a series of vital challenges from sulfur cathode and sodium anode: (i) sluggish reaction kinetics of S and Na2S/Na2S2; (ii) severe shuttle effect from the dissolved intermediate sodium polysulfides (NaPSs); (iii) huge volume expansion induced by the change from S to Na2S; (iv) continuous growth of sodium metal dendrites, leading to short‐circuiting of the battery; (v) huge volume expansion/contraction of sodium anode upon sodium plating/stripping, causing uncontrollable solid‐state electrolyte interphase growth and “dead sodium” formation. Various strategies have been proposed to address these issues, including physical/chemical adsorption of NaPSs, catalysts to facilitate the rapid conversion of NaPSs, high‐conductive materials to promote ion/electron transfer, good sodiophilic Na anode hetero‐interface homogenized Na ions flux and three‐dimensional porous anode host to buffer the volume expansion of sodium. Heterostructure materials can combine these merits into one material to realize multifunctionality. Herein, the recent development of heterostructure as the host for sulfur cathode and Na anode has been reviewed. First of all, the electrochemical mechanisms of sulfur cathode/sodium anode and principles of heterostructures reinforced Na‐S batteries are described. Then, the application of heterostructures in Na‐S batteries is comprehensively examined. Finally, the current primary avenues of employing heterostructures in Na‐S batteries are summarized. Opinions and prospects are put forward regarding the existing problems in current research, aiming to inspire the design of advanced and improved next‐generation Na‐S batteries.

The high theoretical capacities and excellent redox activities motivate transitional metal sulfides (TMSs) to serve as promising anode materials for sodium‐ion batteries. However, TMSs would experience low electronic conductivity as well as notorious polysulfides dissolution and shuttle effect during charge/discharge processes, which leads to unsatisfactory rate capability and cycling stability. Herein, TMSs‐based anode materials with NiS2 nanoparticles tightly anchoring on nitrogen‐doped graphene (NiS2/NG) via the Ni–N covalent bond have been developed through an electrostatic self‐assembly approach between exfoliated positively charged layered double hydroxide and negatively charged graphene oxide nanosheets, followed by a sulfidation process. The strong coupling between conductive and active components enables NiS2/NG to possess good structural integrity, high ion/electron conductivity, and strong polysulfides adsorption capability, ensuring fast reaction kinetics and energetically stable performance. In consequence, the NiS2/NG delivers a high capacity of 664 mAh g−1 at 0.1 A g−1, good rate performance of 545 mAh g−1 at 2 A g−1, and excellent cycling stability with a retained capacity of 589.9 mAh g−1 after 1200 cycles at 0.5 A g−1, among the best results of reported TMSs‐based anodes. The study provides an effective strategy to design heterostructured materials with strong coupling interaction for high‐efficient‐stable sodium 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]

Practical application of lithium–sulfur (Li–S) batteries is severely impeded by the random shuttling of soluble lithium polysulfides (LiPSs), sluggish sulfur redox kinetics, and uncontrollable growth of lithium dendrites, particularly under high sulfur loading and lean electrolyte conditions. Here, nitrogen‐doped bronze‐phase TiO2(B) nanosheets with oxygen vacancies (OVs) grown in situ on MXenes layers (N‐TiO2−x(B)‐MXenes) as multifunctional interlayers are designed. The N‐TiO2−x(B)‐MXenes show reduced bandgap of 1.10 eV and high LiPSs adsorption‐conversion‐nucleation‐decomposition efficiency, leading to remarkably enhanced sulfur redox kinetics. Moreover, they also have lithiophilic nature that can effectively suppress dendrites growth. The cell based on the N‐TiO2−x(B)‐MXenes interlayer under sulfur loading of 2.5 mg cm−2 delivers superior cycling performance with a high specific capacity of 690.7 mAh g−1 over 600 cycles at 1.0 C. It still has a notable areal capacity of 6.15 mAh cm−2 after 50 cycles even under a high sulfur loading of 7.2 mg cm−2 and a low electrolyte‐to‐sulfur (E/S) ratio of 6.4 µL mg−1. The Li‐symmetrical battery with the N‐TiO2−x(B)‐MXenes interlayer showcases a low over‐potential fluctuation with 21.0 mV throughout continuous lithium plating/stripping for 1000 h. This work offers valuable insights into the manipulation of defects and heterostructures to achieve high‐energy Li–S batteries. [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]