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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

Multifunctional MoSe2@rGO coating on the cathode versus the separator as an efficient polysulfide barrier for high-performance lithium-sulfur battery

Yu You,Mengli Wei,Likun Yang,Jingwen Wang,Yongxing Zhang,Jun Xu

The practical applications of high-performance lithium-sulfur batteries are severely hindered by the insulating nature of sulfur and intractable shuttling of the polysulfide intermediates. In this work, we report a novel MoSe 2 @rGO cathode coating consisting of two-dimensional MoSe 2 and reduced graphene oxide (rGO) as a multifunctional barrier to suppress polysulfide shuttling. Few-layered MoSe 2 nanosheets are in situ grown on the rGO surface by basal plane contact. Besides, some cotton-like MoSe 2 nanospheres assembled from porous nanosheets are decorated on the surface of rGO nanosheets. Benefitted from the strong chemical adsorption of polar MoSe 2 and excellent electrical conductivity of rGO, the MoSe 2 @rGO coatings exhibit highly efficient polysulfide anchoring and significantly enhanced electrocatalytic chemistry. Moreover, the MoSe 2 @rGO cathode coatings are much superior to its separator coatings in the recycling of the adsorbed active materials because of good interfacial conductivities. The cell with the MoSe 2 @rGO cathode coating delivers a high reversible capacity up to 1216 mAh g −1 at 0.2 C and outstanding cycling stability with a low capacity fading rate of 0.03% at 1 C over 1000 cycles.

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 Energy Chemistry · 2023 · IF 13.1

Integrated host configuration of flexibly fibrous skeleton towards efficient polysulfide conversion and dendrite-free behavior in stable lithium-sulfur pouch cells

Tongtao Wan,Yusen He,Zongke He,Wenjia Han,Yongguang Zhang,Guihua Liu

The commercialization of lithium-sulfur (Li-S) batteries is obstructed by the sluggish sulfur electrochemical reaction, severe polysulfide shuttling effect, and damaging dendritic lithium growth. Herein, a three-dimensional (3D) conductive carbon nanofibers skeleton-based bifunctional electrode host material is fabricated, which consists of a two-dimensional (2D) ultra-thin NiSe 2 -CoSe 2 heterostructured nanosheet built on one-dimensional (1D) carbon nanofibers (NiSe 2 -CoSe 2 @CNF). When serving as cathodic host, the heterostructured NiSe 2 -CoSe 2 @CNF offers a synergistic function of polysulfide confinement and catalysis conversion. The S/NiSe 2 -CoSe 2 @CNF cathode shows outstanding cycling stability of 0.03% capacity decay rate per cycle over 500 cycles at 1 C. As anodic host, the NiSe 2 -CoSe 2 @CNF with high-flux Li + diffusion property and good lithiophilic capability realizes dendrite-free Li plating/stripping behavior. Benefiting from these synergistically merits, the Li-S full cell with S/NiSe 2 -CoSe 2 @CNF|Li/NiSe 2 -CoSe 2 @CNF electrodes exhibits excellent electrochemical performance including a high specific capacity of 1021 mA h g −1 over 100 cycles at 0.2 C and reversible areal capacity of 3.05 mA h cm −2 under a high sulfur loading of 4.33 mg cm −2 at 0.1 C. The pouch cell also delivers ultra-stable Li/S electrochemistry. This study demonstrates a rational and universal electrode construction strategy for developing practical and high-energy Li-S batteries.

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LANGMUIR · 2025 · IF 3.9

Zn–V-MOF-Derived Hierarchical Zn3V2O8 Modified Separator for Synergistic Polysulfide Trapping and Catalytic Conversion in High-Energy Lithium–Sulfur Batteries

Lina Jin,Baozhong Li,Xinye Qian,Hexiang Xu

Lithium–sulfur batteries (LSBs) are recognized as promising candidates for next-generation high-energy-density energy storage technologies due to their exceptionally high theoretical energy density (2600 Wh kg–1), low cost, and environmental sustainability. However, several challenges, including the polysulfide(LiPS) shuttle effect, the low conductivity of the sulfur cathode, and lithium dendrite growth, have significantly impeded their practical application. In this research, we developed a hierarchical porous Zn3V2O8 (ZVO) modified separator through the high-temperature calcination of a Zn–V-MOF precursor to effectively mitigate LiPS shuttle effects via a dual mechanism. The porous architecture of ZVO facilitates efficient adsorption and rapid conversion of polysulfides through both physical confinement and catalytic activity arising from vanadium’s multivalent states. Additionally, the nitrogen-doped carbon network enhances electrode conductivity while strengthening polysulfide anchoring. The performance of the ZVO-modified separator reveals an initial discharge capacity of 882.9 mAh g–1 at 0.5C with a sulfur loading of 2.8 mg cm–2, demonstrating retention at 541.2 mAh g–1 after 500 cycles-yielding a capacity retention rate of 61.3%. Notably, under commercially viable conditions (5 mg cm–2 sulfur loading and 0.1C), the battery exhibits stable cycling performance, underscoring the potential applicability of ZVO-based separators in practical high-energy-density LSB systems.

研究领域: 储能技术 · 材料科学 · 电化学 · 纳米技术 · 电池技术
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Hierarchical biomass-derived carbon framework with asymmetric ZnCo dual-atom pairs for synergistic polysulfide adsorption and catalysis in Lithium-sulfur batteries

Zichun Luo,Jiayi Wang,Enqi Chen,Lin Yang,Xin Wang,Zhongwei Chen

Lithium‑sulfur (Li S) batteries have recently attracted ever-increasing attention owing to their ultrahigh specific energy and substantial cost benefits of sulfur. However, the sluggish redox kinetics from the critical conversion of soluble long-chain lithium polysulfide to solid-state Li 2 S remains a fundamental challenge. Herein, hierarchical porous nitrogen-doped carbon frameworks with asymmetric Zn Co dual-atom pairs (Zn-Co/NC) were successfully constructed using biomass-derived porous carbon as structural matrix through in situ growth and assisted pyrolysis strategy. The resulting hierarchical porous structure offers abundant electrochemically active interface and facilitates ultrafast electron/ion transport. In addition, the well-constructed Zn Co dual-atom pairs demonstrates strong adsorption and catalysis effect for sulfur species. Consequently, Li S cells incorporating Zn-Co/NC@PP deliver a 0.2C initial discharge capacity of 1263.5 mAh g −1 , coupled with exceptional 500-cycle durability at 1C. Furthermore, when the battery is under the conditions of high sulfur loading (6.6 mg cm −2 ) and low electrolyte (E/S = 5.0 μL mg −1 ), a satisfying surface capacity of 4.9 mAh cm −2 can still be achieved. Such a precise design of versatile dual-atom pairs catalysts involving synergistic adsorption and catalysis provides valuable insights for multistage sulfur conversion reactions.

研究领域: 储能 · 材料科学 · 电化学 · 纳米技术 · 催化
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2D Materials · 2022 ·Vol. 9 ·期 2 ·025028 · IF 6.861

2D Cu2− x Se@graphene multifunctional interlayer boosting polysulfide rapid conversion and uniform Li2S nucleation for high performance Li–S batteries

Meng Yuan,Haodong Shi,Cong Dong,Shuanghao Zheng,Kai Wang,Shaoxu Wang,Zhong-Shuai Wu

Some vital challenges are main obstacles for further development of lithium–sulfur (Li–S) batteries such as low capacity and poor cycle stability resulted from polysulfide shuttling behavior, the physical/chemical entrapment is regarded as an effective method to inhibit and catalyze polysulfides. Herein we design a cross-linked framework of reduced graphene oxide anchored with Cu2−xSe nanoparticles (Cu2−xSe@rGO) by building an electrolyte/Cu2−xSe/graphene triple-phase interface to be a high-efficiency electrocatalyst for Li–S batteries. Importantly, this three-dimensional conductive network possesses a large specific surface area with high ion transport capability, meanwhile providing strong physical constraint for efficient adsorption of soluble polysulfides. Further, this triple-phase catalytic interface provides strong chemical adsorption and abundant Cu2−xSe nanoparticle sulfiphilic active sites, effectively inhibiting the dissolution of polysulfides and guaranteeing the efficient polysulfide adsorption catalysis as well as rapidly uniform Li2S nucleation. Consequently, with the Cu2−xSe@rGO separator, a lower capacity decay rate about 0.059% per cycle after 500 cycles at 2 C is obtained. What's more, with a higher areal sulfur loading of 3.0 mg cm−2, the capacity is still maintained at 805 mAh g−1 over 100 cycles. Therefore, this work will open new avenue to construct 2D transition metal selenide for superior performance Li–S batteries.

研究领域: 材料科学 · 能源存储与转换
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Journal of Materials Chemistry A · 2019 ·Vol. 7 ·期 13 ·7897-7906 · IF 10.733

Fast electrochemical kinetics and strong polysulfide adsorption by a highly oriented MoS2 nanosheet@N-doped carbon interlayer for lithium–sulfur batteries

Jingyi Wu,Xiongwei Li,Hongxia Zeng,Yang Xue,Fangyan Chen,Zhigang Xue,Yunsheng Ye,Xiaolin Xie

The polysulfide shuttle effect and sluggish reaction kinetics can severely reduce the sulfur utilization and cycle stability of Li–S batteries, undermining their use in practical applications. Herein, we design a core–shell nanocomposite by encapsulating radially oriented MoS2 nanosheets by porous nitrogen-doped carbon (MoS2@NC) via an eco-friendly method. The highly oriented MoS2 nanosheets in MoS2@NC avoid aggregation of the active sites for polysulfide adsorption, and the desirable integration of the catalytic MoS2 nanosheet core and a highly conductive carbon shell provides a constant flow of electrons to the captured polysulfides for improved polysulfide conversion kinetics. The combined benefits of high polysulfide inhibition and smooth electron and Li+ transfer by a thin layer of MoS2@NC (3.3 μm thick) enable a simple sulfur–carbon black cathode with high reversible capacities, good rate performances (876 mA h g−1 at 3C), an excellent cycle stability over 1500 cycles with a negligible 0.034% decay per cycle, and satisfactory areal capacities with increased sulfur loading (2.0–3.7 mA h cm−2 at various rates). This work provides a proof-of-concept study on the rational design of interlayer materials in energy storage systems.

研究领域: 材料科学 · 电化学
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Materials Today Sustainability · 2023 · IF 7.8

Rutile titanium dioxide and graphene-like OCN tailoring free-standing carbon fiber aerogel as polysulfide anchoring materials for lithium–sulfur batteries

D. Yang,T. Wu,H. Gao,M. Jia,L. Ji,J. Wang,Q. Zhuang,B. Yu,L. Lu,Y. Zhang,J. Liu

The rational design of a host material with strong adsorption and excellent electrical conductivity function for sulfur cathode to suppress the shuttle effects of soluble lithium polysulfide (LiPS) is crucial to advance the lithium–sulfur (Li–S) battery for future commercial applications. In this work, we designed a three-dimensional (3D) carbon fiber aerogel with graphene-like oxygenated carbon nitrogen (OCN) and TiO 2 (OCNF–TiO 2 ) as a sulfur anchoring material for Li–S battery and explored the regulating effects of TiO 2 on the electrochemical performances. The OCNF–TiO 2 /S cathode presents an initial discharge-specific capacity of 1039 mAh/g (0.1C), a rate capacity of 690 mAh/g at 1C, a cycling performance with a capacitance retention of 72.1%, and the decay of 0.13% per cycle after 200 cycles at 0.5C.

CAS / MDL: 12125-02-9 7704-34-9
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

N-doped porous carbon coated g-C3N4/ g-C3N4 heterojunction for polysulfide restriction and catalytic conversion towards enhanced lithium-sulfur batteries

Youlan Zou,Haiyan Zou,Zhuoran Ao,Yiyang Lv,Nantao Chen,Yuxing Huang

Notorious shuttle effects and poor electrical conductivity of S have long hindered the commercialization of lithium-sulfur (Li-S) batteries. Herein, N-doped porous carbon coated graphitic carbon nitride heterojunction (g-C 3 N 4 / g-C 3 N 4 @C) composites was prepared by growing g-C 3 N 4 / g-C 3 N 4 heterojunction on the pores of the porous carbon. The effective interface adhesion of g-C 3 N 4 / g-C 3 N 4 heterojunction and high conductive porous carbon served as S host insure the initial specific capacity of 752 mAh/g at 1 C, reversible capacity of 496 mAh/g at 1 C after 400 cycles, and higher rate capacity of 468 mAh/g at 2 C after 500 cycles for Li-S batteries. The mechanism of this ternary synergetic system for enhancement of electrochemical performance is based on effective interface adhesion and conductive property caused by different band energies of g-C 3 N 4 and the N-doped porous carbon.

CAS / MDL: 57-13-6 62-56-6
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Nano Energy · 2019 · IF 15.548

Reviving catalytic activity of nitrides by the doping of the inert surface layer to promote polysulfide conversion in lithium-sulfur batteries

Boyu Hao,Huan Li,Wei Lv,Yunbo Zhang,Shuzhang Niu,Qi Qi,Shujie Xiao,Jia Li,Feiyu Kang,Quan-Hong Yang

Lithium-sulfur batteries show great promise among future battery technologies, but their cycle life is mainly restricted by the shuttling effect of soluble lithium polysulfides (LiPSs). The catalytic conversion of LiPSs appears to be a fundamental way of suppressing this. The highly conductive metal nitrides show great potentials as high-performance catalysts, but the presence of a thin surface oxidation layer, which is normal for nanomaterials, restrains the surface electron transfer and catalytic activity. In this study, we demonstrate that the doping of the oxidation layer is an ideal solution to reviving and enhancing the catalytic activity of nitrides. As a proof of concept, sulfur-doping of a titanium nitride (TiN) oxidation layer is presented here, and the Ti S bonds formed are responsible for transmitting electrons from the conductive TiN matrix thus guaranteeing a high catalytic activity. Interfacing of Ti S with Ti O bonds at the atomic level helps realize strong trapping and fast conversion of LiPSs simultaneously. As a result, the specific capacity, rate performance, and cyclic stability are all greatly improved by the interlayer composed of sulfur-doped TiN and graphenes, which indicates a practical avenue for building high performance lithium-sulfur batteries.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

A calcium fluoride composite reduction graphene oxide functional separator for lithium-sulfur batteries to inhibit polysulfide shuttling and mitigate lithium dendrites

Weitao Jing,Kunyang Zou,Xin Dai,Ming Shi,Junjie Sun,Dongdong Zhu,Shengwu Guo,Yuanzhen Chen,Yongning Liu

Lithium-sulfur (Li-S) batteries have attracted tremendous attention as promising next-generation energy-storage systems due to their high specific capacity and high specific energy. However, the shuttle of polysulfides and the growth of Li dendrites severely obstruct the practical applications of these batteries. In this work, a functional separator is designed and fabricated in which nano-calcium fluoride (CaF 2 ) particles are embedded in reduced graphene oxide (rGO) and bladed on a PP separator. The density functional theory (DFT) calculations of the adsorption energy and bond length reveal that CaF 2 has a satisfying adsorption and catalytic effect on polysulfides (Li 2 S n ). The factional separator could accelerate homogenous Li + flow and retard the growth of Li dendrites. In addition, an initial specific capacity of 1504 mAh g −1 at 0.05C is achieved, and it still retains a discharge capacity of 1050 mAh g −1 over 100 cycles at 0.2C. Moreover, the capacity decay rate is only 0.06% per cycle over 420 cycles at a high current density of 0.5 C. The excellent performance could be attributed to the CaF 2 @rGO modified separator not only accelerating the transmission of electrons but also effectively inhibiting the shuttling of polysulfides. This work provides a better method for attaining practical applications of high-performance lithium-sulfur batteries.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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CHEMISTRY-A EUROPEAN JOURNAL · 2024 ·Vol. 30 ·期 37 ·e202400945 · IF 3.9

Modulating the Coordination Chemistry of Cobalt Catalytic Sites by Ruthenium Species to Accelerate the Polysulfide Conversion Kinetics in Lithium-Sulfur Batteries

Zhiqian Lin,Haoxian Zhu,Liyuan Qian,Xiaohui Tang,Jiangnan Wen,Yun Wang,Xiaofei Wang,Songbai Han,Jinlong Zhu,Haibin Lin,Yusheng Zhao

Graphical The well-dispersed Ru in the Co−NC carbon matrix altered the total charge distribution over the Co−N−C catalytic sites and led to the formation of electron-rich Co−N, which is highly active for the polysulfide conversion reactions. Additionally, introducing Ru in the Co−NC matrix provided additional catalytic sites over the Ru−N x species to manifest optimal adsorption behavior of polysulfides. The performance of lithium-sulfur batteries is compromised by the loss of sulfur as dissolved polysulfides in the electrolyte and consequently the polysulfide redox shutting effect. Accelerating the conversion kinetics of polysulfide intermediates into sulfur or lithium sulfide through electrocatalysis has emerged as a root-cause solution. Co−N−C composite electrocatalyst is commonly used for this purpose. It is illustrated here that how the effectiveness can be improved by modulating the coordination chemistry of Co−N−C catalytic sites through introducing Ru species (RuCo−NC). The well-dispersed Ru in the Co−NC carbon matrix altered the total charge distribution over the Co−N−C catalytic sites and led to the formation of electron-rich Co−N, which is highly active for the polysulfide conversion reactions. Using Ru to modulate the electronic structure in the Co−N−C configuration and the additional catalytic sites over the Ru−N x species can manifest optimal adsorption behavior of polysulfides. Consequently, the sulfur cathode with RuCo−NC can reduce the capacity fade rate from 0.11 % per cycle without catalyst (initial capacity of 701 mAh g −1 ) to 0.054 % per cycle (initial capacity of 1074 mAh g −1 ) over 400 cycles at 0.2 C rate. The results of this study provide the evidence for a feasible catalyst modification strategy for the polysulfide electrocatalysis.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Nanoscale · 2021 ·Vol. 14 ·期 3 ·700-714 · IF 7.79

A flame-retardant polyimide interlayer with polysulfide lithium traps and fast redox conversion towards safety and high sulfur utilization Li–S batteries

Zhiyu Zhou,Zexiang Chen,Yang Zhao,Huifang Lv,Hualiang Wei,Bingbing Chen,Zengjie Gu,Yan Wang

In recent years and following the progress made in lithium-ion battery technology, substantial efforts have been devoted to developing practical lithium–sulfur (Li–S) batteries for next-generation commercial energy storage devices. The practical application of Li–S batteries is still limited by dramatically reduced capacities, cycling instabilities, and safety issues arising from flammable components. In this study, we designed and fabricated a flame-retardant, multifunctional interlayer which integrated electroconductive networks, lithium polysulfide (LiPS) traps and catalysts to significantly elevate the electrochemical performance and safety of pristine Li–S batteries. The LiPS adsorptive polymer polyimide (PI) constrains polysulfides to the cathode region and effectively suppresses the shuttle effect. Coralloid PI/multiwalled carbon nanotube (MCNT) compounds provide plentiful reaction sites for active materials. The catalytic Ni on the metal skeleton surface notably promotes Li+ diffusion, lowers the redox overpotential and accelerates LiPS conversion, which improves the redox kinetics associated with sulfur-related species and significantly elevates sulfur utilization. At different current densities of 0.2 C and 0.5 C, impressive initial discharge capacities of 1275.3 mA h g−1 and 1190.9 mA h g−1 are attainable respectively, with high capacity retentions of 80.3% and 78.6% over 600 cycles. Besides, the multifunctional interlayer can also act as a flame-retardant layer to promote the safety of Li–S batteries by inhibiting the spread of fire. This study provides a feasible and prospective strategy that adopts a multifunctional interlayer to develop Li–S batteries with higher capacities, longer cycling lives and safer working conditions.

研究领域: 材料科学 · 电化学 · 能源存储技术
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