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ACS Applied Materials & Interfaces · 2016 · IF 7.145

The Effective Design of a Polysulfide-Trapped Separator at the Molecular Level for High Energy Density Li–S Batteries

Chao-Ying Fan,Hai-Yan Yuan,Huan-Huan Li,Hai-Feng Wang,Wen-Liang Li,Hai-Zhu Sun,Xing-Long Wu,Jing-Ping Zhang

In this work, the lightweight and scalable organic macromolecule graphitic carbon nitride (g-C3N4) with enriched polysulfide adsorption sites of pyridinic-N was introduced to achieve the effective functionalization of separator at the molecular level. This simple method overcomes the difficulty of low doping content as well as the existence of an uncontrolled form of nitrogen heteroatom in the final product. Besides the conventional pyridinic–N-Li bond formed in the vacancies of g-C3N4, the C–S bond was interestingly observed between g-C3N4 and Li2S, which endowed g-C3N4 with an inherent adsorption capacity for polysulfides. In addition, the microsized g-C3N4 provided the coating layer with good mechanical strength to guarantee its restriction function for polysulfides during long cycling. As a result, an excellent reversible capacity of 840 mA h g–1 was retained at 0.5 C after 400 cycles for a pure sulfur electrode, much better than that of the cell with an innocent carbon-coated separator. Even at a current density of 1 C, the cell still delivered a stable capacity of 732.7 mA h g–1 after 500 cycles. Moreover, when further increasing the sulfur loading to 5 mg cm–2, an excellent specific capacity of 1134.7 mA h g–1 was acquired with the stable cycle stability, ensuring a high areal capacity of 5.11 mA h cm–2. Besides the intrinsic adsorption ability for polysulfides, g-C3N4 is nontoxic and mass produced. Therefore, a scalable separator decorated with g-C3N4 and a commercial sulfur cathode promises high energy density for the practical application of Li–S batteries.

研究领域: 材料科学 · 储能 · 电化学 · 纳米材料
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ACS Nano · 2019 · IF 13.903

Enhanced Chemical Immobilization and Catalytic Conversion of Polysulfide Intermediates Using Metallic Mo Nanoclusters for High-Performance Li–S Batteries

Yuanjian Li,Chong Wang,Wenyu Wang,Alex Yong Sheng Eng,Mintao Wan,Lin Fu,Eryang Mao,Guocheng Li,Jiang Tang,Zhi Wei Seh,Yongming Sun

Rechargeable lithium–sulfur batteries have attracted tremendous scientific attention owing to their high energy density. However, their practical application is greatly hindered by the notorious shuttling of soluble lithium polysulfide (LPS) intermediates with sluggish redox reactions and uncontrolled precipitation behavior. Herein, we report a semiliquid cathode composed of an active LPS solution/carbon nanofiber (CNF) composite layer, capped with a carbon nanotube (CNT) thin film decorated with metallic Mo nanoclusters that regulate the electrochemical redox reactions of LPS. The trace amount (0.05 mg cm–2) of metallic Mo on the CNT film provides sufficient capturing centers for the chemical immobilization of LPS. Together with physical blocking of LPS by the compact CNT film, free diffusion of LPS is significantly restrained and the self-discharge behavior of the Li–S cell is thus effectively suppressed. Importantly, the metallic Mo nanoclusters enable fast catalytic conversion of LPS and regular deposition of lithium sulfide. As a result, the engineered cathode exhibits a high active sulfur utilization (1401 mAh g–1 at 0.1 C), stable cycling (500 cycles at 1 C with 0.06% decay per cycle), high rate performance (694 mAh g–1 at 5 C), and low self-discharge rate (3% after 72 h of rest). Moreover, a high reversible areal capacity of 4.75 mAh cm–2 is maintained after 100 cycles at 0.2 C for a cathode with a high sulfur loading of 7.64 mg cm–2. This work provides significant insight into the structural and materials design of an advanced sulfur-based cathode that effectively regulates the electrochemical reactions of sulfur species in high-energy Li–S batteries.

研究领域: 储能 · 材料科学 · 电化学 · 纳米材料 · 电池技术
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2026 · IF 9.7

Multifunctional SiO2-anchored catechol-derived coated separators with enhanced thermal safety and polysulfide confinement for advanced lithium-sulfur batteries

Weilong Shao,Delai Jiao,Shanzhe Li,Biao Lu,Bo Liu,Chunling Zhang,Feifei Zhang

Lithium‑sulfur batteries (LSBs) have attracted significant attention as promising energy storage and power sources due to their exceptionally high energy density (2600 Wh kg −1 ) and the low cost of active sulfur materials. However, their practical deployment is hindered by the severe polysulfide shuttle effect and the poor thermal stability of commercial polypropylene (PP) separators, which tend to shrink at elevated temperatures and cause internal short circuits. In this study, a flame-retardant and lithium polysulfides (LiPSs)-anchoring material (SiO 2 @PD) is synthesized and coated onto PP separators (SiO 2 @PD/PP) via a simple slurry-coating method. The synergistic LiPSs adsorption arises from strong interactions between the phosphorus‑oxygen double bonds (P=O) and hydroxyl groups (-OH) of PD and the Si–O–Si bonds of SiO 2 , effectively suppressing the LiPSs shuttle effect and facilitating Li + transport. Moreover, the release of phosphorus species from PD at elevated temperatures, together with the thermal barrier provided by SiO 2 , significantly enhances flame retardancy and ensures structural integrity under high-temperature operation. Benefiting from these combined effects, LSBs employing SiO 2 @PD/PP separators deliver exceptionally low capacity decay rate of 0.027% per cycle over 1000 cycles at 2.5C, and exhibit excellent thermal resilience, retaining 730.32 mA h g −1 after 100 cycles at 60 °C. This work provides a practical and scalable strategy for designing multifunctional separators toward high-performance and intrinsically safe LSBs.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Polymers · 2026 ·Vol. 18 ·期 2 ·184 · IF 4.9

Enhanced Mechanical and Thermal Properties of Epoxy Resins Through Hard–Soft Biphasic Synergistic Toughening with Modified POSS/Polysulfide Rubber

Xi Yuan,Zhineng Tan,Shengwen Liu,Hang Luo,Zhuo Chen,Dou Zhang

Toughening modification of epoxy resin (EP) matrices is important for advancing high-performance fiber-reinforced composites. A promising strategy involves the use of multi-component additive systems. However, synergistic effects in such additive systems are difficult to achieve for multidimensional performance optimization due to insufficient interfacial interactions and competing toughening mechanisms. Herein, a “hard–soft” biphasic synergistic toughening system was engineered for epoxy resin, composed of furan-ring-grafted polyhedral oligomeric silsesquioxane (FPOSS) and liquid polysulfide rubber. The hybrid toughening agent significantly enhanced the integrated performance of the epoxy system: Young’s modulus, tensile strength, and elongation at break increased by 13%, 56%, and 101%, respectively. These improvements are attributed to the formation of enriched molecular chain entanglement sites and optimized dispersion, facilitated by nucleophilic addition reactions between flexible rubber segments and rigid FPOSS units with the epoxy matrix. The marked enhancement in toughness primarily stems from the synergistic toughening mechanism involving “crazing pinning” and “crazing-shear band”. Concurrently, FPOSS incorporation effectively modulated the curing reaction kinetics, rendering the process more gradual while substantially elevating the glass transition temperature (Tg) of the cured system by 16.82 °C and endowing it with superior thermal degradation stability. This work provides a simple and unique strategy to leverage multi-scale mechanisms for the construction of epoxy-based composites with good toughness and strength, and enhanced heat resistance.

CAS / MDL: 2530-83-8 617-89-0
✓ 已验证 产品关联 DOI PubMed 高影响因子
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Inorganic Chemistry Frontiers · 2026 · IF 6.2

Constructing dynamic Na+ transport channels in RT Na–S battery separators to suppress polysulfide shuttling and accelerate reaction kinetics

Xiaoxue Mao,Zhiyong Xiong,Yuhao Xiang,Shihang Guo,Xin Chen,Hongyang Zeng,Jian Jiang,Sirui Wan,Yi Li,Maowen Xu

Room-temperature sodium–sulfur batteries (RT Na–S) hold great potential for energy storage due to the abundance of sodium and sulfur, low costs, and high theoretical energy density. However, their development is limited by the shuttle effect of polysulfides, slow reaction kinetics, and the growth of sodium dendrites. These issues lead to rapid capacity decay and poor cycling stability, which are difficult to mitigate using traditional separators. Inspired by ion channels in biological membranes, we developed a carboxylate-modified MIL-121/Na separator. Its sub-nanometer channels enable highly selective Na+ transport with an ionic conductivity of 2.27 × 10−4 S cm−1, a migration number of 0.74, and a wide electrochemical window of up to 5.1 V. When applied in RT Na–S batteries, it effectively inhibits the polysulfide shuttle and promotes the reaction kinetics, achieving a first-cycle discharge capacity of 1182 mAh g−1 at a 0.5C rate and stable cycling for over 400 cycles, demonstrating excellent rate performance and long cycle life. Even in pouch cells, the performance can be stabilized at a 1C rate for 100 cycles and the cycle-to-cycle stability can be maintained. This study provides a new strategy for separator design to advance high-performance sodium–sulfur batteries.

✓ 已验证 产品关联 DOI 高影响因子
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ACS Applied Materials & Interfaces · 2026 · IF 7.8

Enabling Durable Quasi-Solid-State Li–S Batteries with an Organic Nitrate Additive for Anode Protection and Polysulfide Confinement

Xinlong Fan,Guojian Lin,Zhouyu Huang,Tianqi Yang,Wenkui Zhang,Dan Li,Haiyuan Zhang,Hui Huang,Wenlong Song,Yang Xia,Jun Zhang

Poly(1,3-dioxolane) (PDOL)-based electrolytes are promising candidates for lithium–sulfur (Li–S) batteries due to their high ionic conductivity and low cost. However, their poor interfacial compatibility with lithium metal impedes the formation of a stable solid electrolyte interphase (SEI). This challenge is further exacerbated by the fact that conventional nitrate additives (e.g., LiNO3) inhibit 1,3-dioxolane (DOL) polymerization. Herein, we propose isosorbide dinitrate (ISDN), a covalent organic nitrate, as a multifunctional additive that not only promotes DOL polymerization but also enables the formation of an inorganic-rich hybrid SEI (Li3N and LiNxOy), as verified through X-ray photoelectron spectroscopy (XPS) analysis and theoretical calculations. The reinforced SEI enhances interfacial ion transport and mechanical robustness, thereby achieving uniform and dendrite-free lithium deposition. Density functional theory (DFT) calculations further reveal strong chemical interactions between ISDN and PDOL, which effectively enhance the adsorption of polysulfide onto PDOL to suppress the shuttle effect. Benefiting from these synergistic functions, Li|PDOL@ISDN|Li symmetric cells achieve stable cycling exceeding 1000 h without short-circuit failure. Quasi-solid-state Li–S batteries also demonstrate excellent cycling stability, with a capacity retention of 84.7% after 100 cycles at 0.2C. This work offers a promising strategy for designing high-performance solid-state Li–S batteries based on PDOL electrolytes.

✓ 已验证 DOI PubMed 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Bifunctional NiCoP nanofiber arrayed on carbon cloth for fast polysulfide conversion and uniform lithium deposition in lithium sulfur batteries

Zhenzhen Yang,Wenqiang Lu,Chao Sun,Mingguang Yao,Nan Chen,Heng Jiang,Chunzhong Wang,Dong Zhang,Fei Du

The severe polysulfides shuttling and irregular lithium dendrites impede the widespread adoption of lithium-sulfur (Li-S) batteries. Here, a sulfiphilic/lithiophilic NiCoP nanofiber arrayed on carbon cloth (NiCoP@CC) as the sulfur/lithium host is reported, providing a dual solution for both cathode and anode issues. Both theoretical calculations and experiments confirm that NiCoP@CC enhances the cycling stability of sulfur cathode and lithium anode by facilitating polysulfides conversion and homogenizing lithium deposition. Additionally, the unique structure of NiCoP nanofiber-decorated carbon cloth provides ample space to accommodate active materials and ensures even distribution of sulfur and lithium. Consequently, Li-S half cells containing NiCoP@CC exhibit an outstanding cycling life of 900 cycles at 1 C. Moreover, the Li@NiCoP@CC electrode achieves a stable, long cycling performance for 3000 h at 1 mA cm −2 . Notably, Li-S full cells show enhanced cycling performance, maintaining stability over 750 cycles with a decay rate of 0.04 % per cycle at 1 C and a low N/P (negative/positive capacity) ratio of 2.4. A high areal capacity of 7.75mAh cm −2 is obtained at a high sulfur loading of 8.6 mg cm −2 . This study presents a new strategy for designing bimetallic phosphides as bifunctional materials to overcome difficulties in practical Li-S batteries.

研究领域: 能源材料 · 电化学 · 纳米材料 · 电池技术
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2019 · IF 3.218

A hydrogel-coated porous sulfur particle as volume-accommodable, conductivity-improved, and polysulfide-adsorptive cathode for lithium‑sulfur batteries

Jinyun Liu,Yu Chen,Wen Zhang,Xirong Lin,Haikuo Zhang,Ping Zhou,Yong Wu,Cuiping Gu

Simultaneously achieving a high conductivity and a good volume-change accommodation for sulfur cathode in lithium‑sulfur batteries is highly required. Herein, we present a unique porous sulfur composite consisting of a porous sulfur particle coating with conductive hydrogel polypyrrole , which is prepared through a templated method. The pores inside the sulfur particles offer a good buffering space for the volume expansion of sulfur upon lithiation; while the external polypyrrole coating improves the conductivity and suppress the transfer of polysulfides . The porous sulfur@polypyrrole composite exhibits a capacity of about 900 mAh g −1 after cycling for 100 times at 0.12   C, along with a good Coulombic efficiency around 99.9%, which is much better than the polypyrrole-coated non-porous sulfur particles and pure sulfur particles. When cycled for 500 times, the capacity fading rate is as low as 0.09% per cycle. After three rounds of rate-performance measurements, the capacity retention of the sulfur@polypyrrole at different rates remain above 97%. The density functional theory calculations and electrochemical impedance spectra demonstrate a polysulfide-adsorptive and a stable electric transportation surface of the sulfur@polypyrrole composite, respectively.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 电池技术
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Journal of Materials Chemistry A · 2018 ·Vol. 6 ·期 40 ·19358-19370 · IF 9.931

Interwoven V2O5 nanowire/graphene nanoscroll hybrid assembled as efficient polysulfide-trapping-conversion interlayer for long-life lithium–sulfur batteries

Yi Guo,Yin Zhang,Yun Zhang,Mingwu Xiang,Hao Wu,Huakun Liu,Shixue Dou

An alternative strategy for blocking the shuttling of soluble polysulfides in lithium–sulfur (Li–S) batteries involved introducing an interlayer between the cathode and separator. However, tailoring the interlayer components, structure, and chemistry to realize efficient conversion of polysulfides into insoluble lithium sulfides remains challenging. Herein, a flexible self-standing hybrid interlayer is engineered by intertwining one-dimensional (1D) V2O5 nanowires (NWs) with graphene nanoscrolls (GNS) into a robust interconnected 3D network to be used as both an upper current collector and physical/chemical polysulfide-trapper. The highly conductive and open GNS framework provides bicontinuous transfer channels for rapid electron and ion transport across the cathode/separator interface. Meanwhile, the V2O5 NWs act as ideal redox mediators to dynamically block polysulfide dissolution and facilitate their conversion into sulfides via formation of active intermediate polythionate complexes. Therefore, these cells with 70 wt% sulfur content in the whole cathode have significantly improved performance with a long cycling life (1000 cycles), low capacity decay (0.041% per cycle), and considerable areal capacity (>4 mA h cm−2), even at a high sulfur loading of 5.5 mg cm−2. This novel interlayer design strategy has great potential for promoting the practical use of Li–S batteries.

研究领域: 电化学 · 能源材料 · 纳米材料科学 · 储能技术 · 界面化学
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Nanomaterials · 2022 ·Vol. 12 ·期 20 ·3551 · IF 5.719

Oxygen Vacancies in Bismuth Tantalum Oxide to Anchor Polysulfide and Accelerate the Sulfur Evolution Reaction in Lithium–Sulfur Batteries

Chong Wang,Jian-Hao Lu,An-Bang Wang,Hao Zhang,Wei-Kun Wang,Zhao-Qing Jin,Li-Zhen Fan

The shuttling effect of soluble lithium polysulfides (LiPSs) and the sluggish conversion kinetics of polysulfides into insoluble Li2S2/Li2S severely hinders the practical application of Li-S batteries. Advanced catalysts can capture and accelerate the liquid–solid conversion of polysulfides. Herein, we try to make use of bismuth tantalum oxide with oxygen vacancies as an electrocatalyst to catalyze the conversion of LiPSs by reducing the sulfur reduction reaction (SRR) nucleation energy barrier. Oxygen vacancies in Bi4TaO7nanoparticles alter the electron band structure to improve instinct electronic conductivity and catalytic activity. In addition, the defective surface could provide unsaturated bonds around the vacancies to enhance the chemisorption capability with LiPSs. Hence, a multidimensional carbon (super P/CNT/Graphene) standing sulfur cathode is prepared by coating oxygen vacancies Bi4TaO7−xnanoparticles, in which the multidimensional carbon (MC) with micropores structure can host sulfur and provide a fast electron/ion pathway, while the outer-coated oxygen vacancies with Bi4TaO7−xwith improved electronic conductivity and strong affinities for polysulfides can work as an adsorptive and conductive protective layer to achieve the physical restriction and chemical immobilization of lithium polysulfides as well as speed up their catalytic conversion. Benefiting from the synergistic effects of different components, the S/C@Bi3TaO7−xcoin cell cathode shows superior cycling and rate performance. Even under a high level of sulfur loading of 9.6 mg cm−2, a relatively high initial areal capacity of 10.20 mAh cm−2and a specific energy density of 300 Wh kg−1are achieved with a low electrolyte/sulfur ratio of 3.3 µL mg−1. Combined with experimental results and theoretical calculations, the mechanism by which the Bi4TaO7with oxygen vacancies promotes the kinetics of polysulfide conversion reactions has been revealed. The design of the multiple confined cathode structure provides physical and chemical adsorption, fast charge transfer, and catalytic conversion for polysulfides.

研究领域: 材料科学 · 电化学 · 储能技术 · 纳米材料 · 催化
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Journal of Energy Storage · 2023 · IF 9.4

Free-standing graphene/polyetherimide/ZrO2 porous interlayer to enhance lithium-ion transport and polysulfide interception for lithium-sulfur batteries

Jiuqing Liu,Fanli Zeng,Zikun Hong,Junying He,Qihou Li,Feifei Song,Lishun Bai,Chen Cheng,Zehao Chen,Liandong Tang,Chen Duan,Zhirong Chen

Attributing to high theoretical specific capacity and energy density , lithium-sulfur batteries (LSBs) are receiving great attention. However, the commercialization of such technology is seriously hindered by the shuttle effect of polysulfides during the round-trip charge and discharge process. Herein, with three types of carbon materials and ZrO 2 nanoparticles filled in polyetherimide (PEI) support framework with good stability, porous composite films were obtained by a simple non-solvent phase separation (NIPS) as free-standing interlayers for LSBs. The obtained interlayers can not only provide hierarchical channels for improving lithium-ion transfer number, but also own excellent physicochemical stability and strong adsorption capability towards lithium polysulfide (LiPS). Compared with the pristine one, the representative LSB with graphene/polyetherimide/ZrO 2 interlayer (GPZ) shows good initial cycle discharge specific capacity (1280 mAh g −1 ), better capacity retention (749 mAh g −1 after 200 cycles) and good rate performance (580 mAh g −1 at 2C). This work provides a facile and promising way to achieve functional interlayer with high stability for high performance LSBs.

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ACS Nano · 2022 · IF 18.027

A Molybdenum Polysulfide In-Situ Generated from Ammonium Tetrathiomolybdate for High-Capacity and High-Power Rechargeable Magnesium Battery Cathodes

Dong Chen,Donggang Tao,Xin Ren,Fanjue Wen,Ting Li,Zhongxue Chen,Yuliang Cao,Fei Xu

Rechargeable magnesium batteries (RMBs) are a promising large-scale energy-storage technology with low cost and high reliability. However, developing high-performance cathode materials remains the most prominent obstacle because of the insufficient magnesium-storage active sites and unfavorable magnesium cation transport paths, as well as the strong interaction between the cathode material and the bivalent magnesium cation. Herein, ammonium tetrathiomolybdate is demonstrated to be a high-performance RMB cathode material. Ammonium tetrathiomolybdate exhibits a high capacity of 333 mAh g–1 at 50 mA g–1 and a good rate performance of 129 mAh g–1 at 5.0 A g–1 (∼15 C). An amorphous structure with plenty of efficient magnesium-storage active sites and open magnesium transport paths is in situ formed during the first cycle via ammonium extraction. The covalent-like bond between the molybdenum and sulfur delocalizes the negative charge, weakening the interaction with the bivalent magnesium cation and accelerating the kinetics. The covalent-like molybdenum–sulfur bond also promotes the simultaneous redox of molybdenum and sulfur, leading to a high specific capacity. The present work introduces a high-capacity and high-power RMB cathode material, elucidates the origin of the high performance, and provides insights for the design and optimization of RMB cathode materials.

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