ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yanqing Wang,Jianjiang He,Zengqi Zhang,Zhihong Liu,Changshui Huang,Yongcheng Jin
Graphdiyne (GDY), a new type of carbon material with an electron-rich conjugated structure, has been investigated as a separator coating layer to enhance the electrochemical performance of lithium–sulfur (Li–S) battery. Acetylenic bond (−C≡C–C≡C−) and benzene ring in the GDY coating layer are experimentally verified to reversibly attract the soluble lithium polysulfides by chemical adsorption during cycling. Meanwhile, the shuttle effect of soluble polysulfides is further physically restricted by the GDY coating layer due to the evenly distributed pores (5.42 Å) and a consistent interlayer spacing (3.65 Å) of GDY. Moreover, GDY is a conducting carbon skeleton with high Li+ mobility that can improve the rate performance. Hence, Li–S battery with an as-prepared GDY coating layer shows excellent electrochemical performances including superior specific capacity, excellent rate performance, and low capacity attenuation rate. The high initial discharge capacity of 1648.5 mA h g–1 at 0.1C and 819.5 mA h g–1 even at a high rate of 2C is achieved by this novel separator. The initial capacity of 1112.9 mA h g–1 at 0.5C is retained to 816.7 mA h g–1 after 200 cycles with a low attenuation rate of 0.13% per cycle. Compared with other coated separators, these results show that the GDY coating layer endows the separator with superior electrochemical performances for Li–S battery.
研究领域:
材料科学
·
电化学
·
能源存储
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DOI
PubMed
高影响因子
Gels
·
2025
·Vol. 11
·期 12
·
IF 5.3
Zhenzhen Shan,Xiaoxiong Li,Yalei Li,Yong Wang,Yusen He,Guangyu Sun,Yamin Geng,Guoqing Chang
Lithium–sulfur (Li-S) batteries are renowned for their high theoretical energy density and low cost, yet their practical implementation is hampered by the polysulfide shuttle effect and sluggish redox kinetics. Herein, a sol–gel strategy is proposed to engineer a multifunctional MXene/Fe3O4composite as an efficient mediator for the cathode interlayer. The synthesized composite features Fe3O4nanospheres uniformly anchored on the highly conductive Ti3C2TxMXene lamellae, forming a unique 0D/2D conductive network. This structure not only provides abundant polar sites for strong chemical adsorption of polysulfides but also significantly enhances charge transfer, thereby accelerating the conversion kinetics. As a result, the Li-S battery based on the MXene/Fe3O4interlayer delivers a high initial discharge capacity of 1367.1 mAh g−1at 0.2 C and maintains a stable capacity of 1103.4 mAh g−1after 100 cycles, demonstrating an exceptionally low capacity decay rate of only 0.19% per cycle. Even at a high rate of 1 C, a remarkable capacity of 1066.1 mAh g−1is retained. Electrochemical analyses confirm the dual role of the composite in effectively suppressing the shuttle effect and catalyzing the polysulfide conversion. This sol–gel engineering approach offers valuable insight into the design of high-performance mediators for advanced Li-S batteries.
研究领域:
材料科学
·
储能
·
电化学
·
纳米材料
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产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·Vol. 14
·期 31
·14182-14193
·
IF 7.6
Dong Lei,Zhang Pengfei,Wang Xiuzhen,Zhu Ying,Cao Yilin,Cao Zhangcheng,Song Meijia,Xu Jingjing
The commercial deployment of lithium–sulfur batteries remains largely obstructed by the notorious shuttling behavior of lithium polysulfides (LiPSs) alongside their slow redox kinetics. Herein, a synergistic heterostructure composed of SnS and CoS nanoparticles (SnS-CoS@rGO) is developed as a multifunctional interlayer for separator modification. The SnS-CoS@rGO heterojunction integrates the strong chemisorption capability of SnS and the superior catalytic efficiency of CoS, while the interfacial electric field significantly accelerates interfacial charge transfer. Consequently, the SnS-CoS@rGO-modified separator effectively traps LiPSs and promotes their rapid catalytic conversion. With the SnS-CoS@rGO separator, the Li–S battery exhibits a remarkable first-cycle discharge capacity of 1528.2 mAh g –1 at 0.1 C and maintains exceptional long-cycle durability after more than 1000 cycles at 1 C, with a mere capacity degradation rate of 0.0375% cyclically. Furthermore, the modified separator exhibits favorable lithiophilicity and flame retardancy, thereby effectively impeding the growth of lithium dendrites and enhancing the battery safety performance. This study demonstrates the potential of SnS-CoS@rGO heterostructured electrocatalysts, providing an innovative avenue for designing advanced Li–S batteries.
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2026
·
IF 2.6
Guang Li,Yuehao Bai,Xiaoli Duan,Li Sun,Jiasui Jiang,ChangAn Yang,Yong Tao
Lithium-sulfur (Li–S) batteries are regarded as a promising candidate for next-generation energy storage technologies due to their high theoretical capacity and energy density. However, their practical application remains constrained by critical issues such as the polysulfide shuttle effect and cathode volume expansion. To address this, a multi-functional zwitterionic polyethyleneimine-based binder (PEI-LiCF) was synthesized via nucleophilic substitution between branched polyethyleneimine (PEI) and the highly polar lithium 3-chloropropyltrifluoromethylsulfonyl imide (LiCPSI). Structural analysis confirmed the successful incorporation of oppositely charged groups—quaternary ammonium (positive) and sulfonyl imide (negative)—which form a zwitterionic network. The electrostatic interactions within this network enhance Li+ migration and improve its diffusion kinetics. Furthermore, the abundant polar groups in the network exhibit strong polysulfide-anchoring capabilities. With an optimized PEI:LiCPSI mass ratio of 2 : 1 (denoted PEI-LiCF2), Li–S batteries employing this binder exhibit excellent electrochemical performance, even under a high current density of 1 C. They achieved an initial discharge capacity of 815.7 mAh g−1, maintaining a reversible capacity of 511.9 mAh g−1 after 500 cycles, which corresponds to an ultralow decay rate of merely 0.074% per cycle. This multifunctional water-soluble binder therefore represents a promising candidate material for high-performance Li–S batteries.
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DOI
高影响因子
Small Science
·
2026
·Vol. 6
·期 8
·e70382
·
IF 7
Min Chen,Yaping Lu,Xinmin Zhang,Yixin Song,Fengtao Shao,Xuetao Gao,Zhichao Liu,Chunmei Xu,Yiting Peng,Yaping Feng,Kai Xi,Yatao Liu
Lithium–sulfur (Li–S) batteries represent promising energy storage devices by virtue of their ultrahigh theoretical energy density, yet their practical deployment is severely impeded by the polysulfide shuttle, sluggish sulfur redox kinetics, and progressive degradation of lithium anodes. Herein, we design a thiol-functionalized UiO-66 (UiO-66-SH)-coated polypropylene separator that addresses these challenges simultaneously. The UiO-66-SH combines abundant coordinatively unsaturated Zr sites and SH groups, enabling both strong chemical anchoring of lithium polysulfides and catalytic acceleration of their conversion to Li 2 S. The modified separator exhibits superior electrolyte wettability, a high Li + transference number (0.76), and enhanced ionic conductivity. Furthermore, it regulates lithium deposition to achieve a dendrite-free anode and mitigates polysulfide-induced corrosion. Consequently, Li–S cells incorporating UiO-66-SH/PP separator deliver an initial discharge capacity of 821.3 mAh g −1 at 1 C, retain 521 mAh g −1 after 500 cycles, and achieve a high-rate capacity of 590.9 mAh g −1 at 5 C. Even under a high sulfur loading of 5.05 mg cm −2 , a reversible capacity of 620.1 mAh g −1 is maintained after 200 cycles. This work offers a rational design of a multifunctional MOF-based separator that integrates polysulfide entrapment, catalytic conversion, and anode protection, paving the way toward high-performance, long-life Li–S batteries.
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产品关联
DOI
高影响因子
Energy Materials
·
2026
·Vol. 6
·期 8
·N
·
IF 11.9
Jingjing Qie\u003Csup\u003E1,\u003C\u002Fsup\u003E,Huiyue Sun\u003Csup\u003E1,\u003C\u002Fsup\u003E,Shuang Geng\u003Csup\u003E1,\u003C\u002Fsup\u003E,Yongqi Shang\u003Csup\u003E1\u003C\u002Fsup\u003E,Qunzhi Huang\u003Csup\u003E1\u003C\u002Fsup\u003E,Jishi Wei\u003Csup\u003E1,2,\u003C\u002Fsup\u003E,Ke Chen\u003Csup\u003E1\u003C\u002Fsup\u003E,Taifeng Liu\u003Csup\u003E3\u003C\u002Fsup\u003E,Shuxi Dai\u003Csup\u003E1,\u003C\u002Fsup\u003E,Wuxing Hua\u003Csup\u003E1,4,\u003C\u002Fsup\u003E,Zhen Zhou\u003Csup\u003E4\u003C\u002Fsup\u003E
Developing an effective electrocatalyst to regulate the kinetics of the sulfur redox reaction is essential for inhibiting polysulfide shuttling in Li-S batteries. Here, the electronic structure of CoTe, modulated by cation doping, is systematically investigated to elucidate how orbital hybridization optimizes sulfur redox electrocatalysis. Among the cation-doped CoTe compounds, the introduction of Ni dopants results in the most significant shift of the p-band center of CoTe (Ni-CoTe) towards the Fermi energy level, which facilitates the formation of numerous Te vacancies on the CoTe surface. This structural configuration endows CoTe with a multitude of active sites that bind polysulfide intermediates, lowering the activation energy (Ea) of the sulfur reduction reaction, specifically reducing the Ea for the conversion of lithium polysulfides to Li2S from 0.73 eV to 0.65 eV. As a result, the Li-S battery with Ni-CoTe catalyst delivers exceptional cyclability, with a low-capacity decay of 0.049% per cycle over 1,000 cycles at 2.0 C. Moreover, an initial areal capacity of 13.5 mAh cm-2 at 0.02 C is achieved with a high sulfur loading (10.0 mg cm-2) and a low electrolyte-to-sulfur ratio (5.0 µL mg-1). These findings will provide fundamental insights into orbital-level catalyst design principles for advanced sulfur electrochemistry.
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产品关联
DOI
高影响因子
Sustainable Energy & Fuels
·
2025
·Vol. 9
·期 4
·1002-1010
·
IF 4.1
Yan Yuan,Yaxin Kong,Xiuping Peng,Lei Zhang,Zeyu Li,Hai Lu
To overcome the application bottlenecks of poly(ethylene oxide) (PEO)-based solid polymer electrolytes (SPEs) related to low ionic conductivity and unstable interface chemistry at both electrodes, Li+-conductive solvate ionic liquid (SIL) and soluble long-chain polysulfide (Li2S6) were introduced into the SPE as a liquid plasticizer and functional additive, respectively. Additionally, an integrated structure with a cathode-supported SPE was adopted to enhance interface contact. The modified PEO-based SPE exhibited excellent comprehensive properties, including high ionic conductivity, Li-ion transfer number, oxidation potential and Li metal compatibility. In particular, the moderate addition of Li2S6 was found to not only decrease the PEO crystallinity through strong interaction and uniform dispersion but also effectively stabilized the Li surface and suppressed dendrite growth via chemical reduction. The synergistic effect of the two functional agents and the integrated design endowed the Li metal battery with high reversible capacity and superior cycle stability when operated at room temperature.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ChemElectroChem
·
2020
·Vol. 7
·期 23
·4737-4744
·
IF 4.154
Binren Fang,Xiaolu Tian,Te Wang,Tao Wang,Long Qu,Mingtao Li
Graphical Polysulfide anchor : A high-entropy metal nitride (HEMN) was prepared as an innovative anchor to restrain lithium polysulfides via the chemical bonding interaction. The composite of HEMN and sulfur was encased by graphene to reduce the interface resistance. The absorptivity of HEMN and the high conductivity of graphene improves the capacity and cycle stability concurrently because of their synergistic effect. Lithium−sulfur (Li−S) batteries with ultrahigh theoretical specific capacity (1675 mAh g −1 ) have become a research hotpot, which focuses on the solution of shuttle effect of soluble lithium polysulfides (LIPS). Chemical immobilization of LIPS and encapsulation structure of the sulfur cathode are effective strategies to suppress the shuttle effect. Herein, high entropy metal nitride (HEMN) was prepared by mechanochemical-assisted synthesis as an innovative anchor to restrain LIPS via the chemical bonding interaction between HEMN and LIPS. Furthermore, the composite of HEMN and S was encased by graphene (GR) through electrostatic attraction caused by opposite zeta potential, thus as the effective cathode (HEMN/S@GR) of Li−S batteries. HEMN has plentiful active metal sites which can chemically adsorb LIPS, enhancing the cycle life of Li−S batteries. Graphene can accelerate surface charge transfer of sulfur cathode to reduce the interface resistance because of its high conductivity. The initial specific capacity of HEMN/S@GR cathode is 1193 mAh g −1 and still maintains 695 mAh g −1 after 100 cycles at 0.1 C. When increased to 1.0 C, the initial specific capacity is 556 mAh g −1 and exhibits remarkable stability in long cycles. This study presents the synergetic effect of HEMN and graphene on LIPS in Li−S batteries, which introduces a new application way of high entropy materials in the field of energy storage devices.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Yanlei Shen,Boyu Li,Ziyao Zhang,Jiajing Liu,Huanhuan Ren,Yuman Zhou,Weitao Zhou,Jianxin He
Spinel-structured catalysts demonstrate significant potential for sulfur reduction reaction (SRR) catalysis in lithium-sulfur batteries (LSBs) owing to their geometrically tunable active sites, yet precise structural optimization for simultaneous enhancement of lithium polysulfides (LiPSs) adsorption and catalytic conversion remains challenging. This study addresses this gap through strategic cation occupancy regulation in Co x Mn 3-x O 4 spinels, establishing a dual-active-site system comprising tetrahedral Co 3+ (Td) and octahedral Mn 3+ (Oh) centers that drive selective LiPSs electrocatalysis via geometric synergy. Theoretical and experimental analyses confirm Co 1.2 Mn 1.8 O 4 as the optimal configuration, where optimized Td/Oh Site Distribution Enables: (i) stable covalent Co-S bonding for strong LiPSs adsorption at Td sites, and (ii) dynamic Mn³⁺ (Oh)-S d -p orbital coupling via delocalized d² electrons that critically reduce LiPSs desorption energy barriers (ΔG ≤ 0.82 eV). Leveraging this complementary functionality, a Co 1.2 Mn 1.8 O 4 -embedded carbon nanofiber interlayer delivers exceptional cycling stability—achieving 400 cycles at 1 C with 74.6 % capacity retention. This work extends the application of spinel-type SRR catalysts to high-performance lithium-sulfur batteries.
研究领域:
材料科学
·
电化学
·
纳米技术
·
能量存储
·
催化
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2019
·Vol. 32
·期 4
·1904876
·
IF 25.809
Yuan Tian,Gaoran Li,Yongguang Zhang,Dan Luo,Xin Wang,Yan Zhao,Hui Liu,Puguang Ji,Xiaohang Du,Jingde Li,Zhongwei Chen
The shuttling behavior and sluggish conversion kinetics of the intermediate lithium polysulfides (LiPSs) represent the main obstructions to the practical application of lithium–sulfur (Li–S) batteries. Herein, an anion-deficient design of antimony selenide (Sb 2 Se 3− x ) is developed to establish a multifunctional LiPS barrier toward the inhibition of polysulfide shuttling and enhancement of battery performance. The defect chemistry in the as-developed Sb 2 Se 3− x promotes the intrinsic conductivity, strengthens the chemical affinity to LiPSs, and catalyzes the sulfur electrochemical conversion, which are verified by a series of computational and experimental results. Attributed to these unique superiorities, the obtained LiPS barrier efficiently promotes and stabilizes the sulfur electrochemistry, thus enabling excellent Li–S battery performance, e.g., outstanding cyclability over 500 cycles at 1.0 C with a minimum capacity fading rate of 0.027% per cycle, a superb rate capability up to 8.0 C, and a high areal capacity of 7.46 mAh cm −2 under raised sulfur loading. This work offers a defect engineering strategy toward fast and durable sulfur electrochemistry, holding great promise in developing practically viable Li–S batteries as well as enlightening the material design of related energy storage and conversion systems.
研究领域:
电化学储能
·
材料科学
·
纳米能源材料
·
固态离子学
·
电池技术
✓ 已验证
DOI
高影响因子
Advanced Science
·
2021
·Vol. 9
·期 3
·2104205
·
IF 16.806
Suya Zhou,Shuo Yang,Dong Cai,Ce Liang,Shuang Yu,Yue Hu,Huagui Nie,Zhi Yang
Lithium–sulfur batteries possess high theoretical energy density but suffer from rapid capacity fade due to the shuttling and sluggish conversion of polysulfides. Aiming at these problems, a biomimetic design of cofactor-assisted artificial enzyme catalyst, melamine (MM) crosslinked hemin on carboxylated carbon nanotubes (CNTs) (i.e., [CNTs–MM–hemin]), is presented to efficiently convert polysulfides. The MM cofactors bind with the hemin artificial enzymes and CNT conductive substrates through FeN 5 coordination and/or covalent amide bonds to provide high and durable catalytic activity for polysulfide conversions, while π – π conjugations between hemin and CNTs and multiple Li-bond networks offered by MM endow the cathode with good electronic/Li + transmission ability. This synergistic mechanism enables rapid sulfur reaction kinetics, alleviated polysulfide shuttling, and an ultralow (<1.3%) loss of hemin active sites in electrolyte, which is ≈60 times lower than those of noncovalent crosslinked samples. As a result, the Li–S battery using [CNTs–MM–hemin] cathode retains a capacity of 571 mAh g −1 after 900 cycles at 1C with an ultralow capacity decay rate of 0.046% per cycle. Even under raising sulfur loadings up to 7.5 mg cm −2 , the cathode still can steadily run 110 cycles with a capacity retention of 83%.
研究领域:
材料科学
·
电化学
·
催化科学
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DOI
高影响因子
ACS Nano
·
2022
·
IF 18.027
Lanxiang Feng,Peng Yu,Xuewei Fu,Zheng-Min Zhang,Kenneth Davey,Yu Wang,Zaiping Guo,Wei Yang
Polar host materials with strong adsorption capacity of polysulfides are designed to limit the shuttle effect in sulfur cathodes. However, a critical problem is to control diffusion and deposition of lithium polysulfides during cycling, which significantly impacts cycling stability and sulfur utilization. Here, we report using a sequential adsorption-guided self-assembly to design two types of core–shell sulfur particles with opposite polysulfide adsorption gradients to explore quantitatively the regulation of polysulfide diffusion and deposition. We show that a positive core–shell design of sulfur particles (PCSD@SP), i.e., polysulfide adsorption capability decreasing from the interior to the exterior of the host, is more effective in restricting polysulfide diffusion and regulating polysulfide deposition than the negative core–shell counterpart (NCSD@SP). As a result, the PCSD@SP electrode with a sulfur loading of 7 mg cm–2 exhibits a stable areal capacity of 6 mAh cm–2 over 130 cycles at 0.2C. At intermittent discharge/charge, the PCSD@SP electrode retains excellent stability compared with the NCSD@SP. We conclude that rational design of positive core–shell active materials can be used to regulate polysulfide diffusion and deposition to boost electrochemical reaction dynamics and performance. The reported findings will be of immediate benefit to a range of researchers in the design of high-performance lithium–sulfur batteries.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）