IONICS
·
2021
·Vol. 27
·期 9
·3895-3902
·
IF 2.817
Long Canghai,Li Libo,Shan Yuhang,Zhai Mo,Chen Xiaochuan,Zhao Yangmingyue,Cui Wenjun,Zhou Da,Du Jintian
Lithium-sulfur (Li–S) battery has a very remarkably specific capacity of 1675 mAh g −1 . To avoid the shuttle effect and build the safety and stability of the Li–S battery system, we demonstrated a new conductive carbon as the host material with 0.35-nm micropores and mesopores prepared by a one-step process for a quasi-solid electrolyte. PVDF acted as a precursor and PMMA acted as an additive in this one-step preparation process. In addition, the mesopores enhanced the contact area and the content of sulfur, while the 0.35-nm micropores provided a trap site for the polysulfide by an effective physical absorption when the sulfur embedded in the host material. Finally, the PVDF-based quasi-solid polymer electrolyte avoided the inflammable and explosive risk and achieved an initial specific capacity of 1038 mAh g −1 at 0.1 C, and maintained at 441 mAh g −1 even after 500 cycles (a decay of 0.12% per cycle).
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Materials Reports: Energy
·
2024
·
IF 0
Han Wang,Sidra Jamil,Muhammad Fasehullah,Shujuan Bao,Yi Li,Maowen Xu
Lithium-sulfur (Li-S) batteries are one of the most promising energy storage and conversion devices due to the high theoretical capacity and cost-effectiveness of sulfur. However, they still suffer from sluggish redox kinetics and the shuttle effect caused by complex polysulfides. In this work, graphitic carbon nitride (g-C 3 N 4 ) is utilized as a template and further hydrothermally treated with an Mn source and glucose. The pyrolysis of g-C 3 N 4 gives rise to N-doped carbon nanotubes, producing abundant sites for physical confinement and chemical adsorption of polysulfides, while glucose carbonization brings forth amorphous carbon and Mn source produces metal spheres. Afterward, polydopamine (PDA) induces N-doped carbon coating and promotes interface connection as well as electron immigration. This synergistic design possesses a high surface area of micropores and mesopores to aggregate sulfur and accelerate redox kinetics. As a result, the N-doped carbon nanotube with Mn spheres and PDA coating@sulfur (CN/Mn-PDA@S) exhibits a high reversible capacity of 813.5 mAh g −1 at 1 C with a decay rate of 0.064% per cycle and remarkable capacity retention at 2 C with rate performance up to 4 C. Therefore, the novel design of N-doped carbon nanotubes with Mn spheres and PDA coating serves as an efficient polysulfide immobilizer for Li-S batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Henan Jia,Wenjun Zhang,Jiayi Luo,Tianyu Huo,Zhen Liang,Hui Li,Fuling Tang,Haoyan Liang
Work-function differences between SnO 2 and SnSe 2 induces interfacial band bending and constructing a built-in electric field • The BIEF enriches electrons on Sn sites for strong adsorption, while populating Li- S antibonding orbitals to weaken the bonds • Complementary barriers of SnO 2 /SnSe 2 with HCNF anchoring/buffering enable Li-S battery high capacity and long cycling The shuttle effect and sluggish conversion kinetics of polysulfides severely hinder the practical application of lithium‑sulfur (Li S) batteries. In this work, a novel SnO 2 /SnSe 2 heterostructure anchored on helical carbon nanofibers (HCNFs) is designed and fabricated as a sulfur cathode host (SnO 2 /SnSe 2 @HCNFs//S). The differences in electronegativity and ionic radius between oxygen and selenium drive interfacial electron transfer and generate a built-in electric field (BIEF), endowing the heterojunction with an electronic configuration that combines strong overall adsorption and weak Li S bonds, thereby breaking the conventional balances between adsorption strength and catalytic activity. SnO 2 exhibits a lower energy barrier for the S 8 to Li 2 S n conversion, while SnSe 2 shows a lower barrier for the Li 2 S n to Li 2 S conversion, demonstrating complementary functions, and the BIEF further reduces the overall energy barrier of the multistep reduction to the lowest level. The defect sites of the helical carbon fibers ensure highly dispersed loading of the heterojunction, and the spring-like helical morphology buffers volume expansion and maintains long-term cycling stability. The SnO 2 /SnSe 2 @HCNFs//S cathode delivers an outstanding discharge specific capacity of 1008.2 mAh g −1 at 0.2C, retains over 99.7% of coulombic efficiency after 200 cycles at 0.2C, and a rate performance of 932.4 mAh g −1 even at 2.0C, with rate and cycling performance significantly superior to those of single-phase materials and control samples. This work provides an effective strategy for the rational design of high-performance sulfur hosts for Li S batteries. Helical carbon nanofibers (HCNFs) with abundant defect sites serve as a substrate for anchoring SnO 2 /SnSe 2 heterojunction nanoparticles, ensuring highly dispersed exposure. Work function mismatch drives electron transfer from SnSe 2 to SnO 2 , enhancing Sn S adsorption while injecting electrons into Li S antibonding orbitals to weaken bonds. SnO 2 lowers reaction barrier from S 8 to Li 2 S n , and SnSe 2 lowers barrier from Li 2 S n to Li 2 S, and the built-in electric field further reduces the multistep energy barrier of sulfur conversions, thereby achieving efficient polysulfide adsorption and catalytic conversion. Download: Download high-res image (295KB) Download: Download full-size image
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Jinze Song,Lixia Zhu,Ying Song,Zhaobo Wang,Kaixiang Shi,Xiaolei Song,Quanbing Liu,Guangfeng Wu
HE-MOF@MXene heterostructure was constructed via in situ growth. • The heterostructure combines physical blocking with chemical LiPSs anchoring. • Multi-metal synergy accelerates catalytic conversion of LiPSs. • HE-MOF@MXene//PP delivers 1445 mAh g −1 at 0.2C and 690 mAh g −1 at 5C. • HE-MOF@MXene//PP shows only 0.059% decay per cycle over 900 cycles at 1C. Lithium‑sulfur batteries (LSBs) offer high energy density, yet their performance is restricted by uncontrolled lithium polysulfides (LiPSs) migration and the intrinsically slow multistep conversion of sulfur species. To alleviate these issues, a Fe/Co/Ni/Cu/Mn high-entropy metal-organic framework (HE-MOF) was directly grown on MXene nanosheets to form an HE-MOF@MXene heterostructure, which was subsequently employed as a separator modifier in LSBs. The reciprocal structural regulation between HE-MOF and MXene effectively suppresses component aggregation and layer re-stacking, thereby increasing the accessible surface area of the heterostructure and promoting greater active-site exposure. Meanwhile, the two components are functionally integrated. The well-exposed high-entropy multimetal sites in HE-MOF can effectively exert their adsorption and catalytic advantages toward sulfur species with the assistance of the efficient electron/ion transport network constructed by MXene. Density functional theory calculations suggest distinct electronic structures and d-d interactions among the metal sites in HE-MOF. The resulting multimetal synergy may help accommodate the differentiated adsorption requirements of sulfur species and facilitate their subsequent conversion. Consequently, with the separator functionalized by HE-MOF@MXene, the cell achieves 1445 mAh g −1 at 0.2C. At a high rate of 5C, the cell still delivers 690 mAh g −1 . Moreover, continuous operation over 1000 cycles at 3C results in an average capacity loss of merely 0.060% per cycle. HE-MOF@MXene heterostructure-modified separators integrate efficient physical blocking, strong polysulfide anchoring and rapid sulfur redox reaction kinetics, effectively suppressing shuttle effects and enabling high-performance lithium-sulfur batteries. Download: Download high-res image (239KB) Download: Download full-size image
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DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·Vol. 14
·期 31
·14031-14044
·
IF 7.6
Zhang Chengyang,Xia Guoqiang,Du Xiaohan,Zhen Mengmeng
Lithium−sulfur batteries (LSBs) hold great promise for next-generation energy storage, yet their practical application is hindered by the polysulfide shuttle effect and sluggish redox kinetics, especially under lean-electrolyte conditions. While high-entropy MXenes (HE-MX) exhibit promising electrocatalytic potential for addressing these issues, their performance is compromised by nanosheet restacking and an unfavorable electronic structure. Herein, we propose a synergistic dual-defect engineering strategy to address these limitations. A three-dimensional (3D) network consisting of P-doped, anion-vacancy-rich TiVCrMoC 3 T x HE-MX integrated with carbon nanotubes (P-HE-MX@C) is constructed as a multifunctional separator coating for LSBs. Comprehensive experimental analyses and density functional theory calculations reveal that the co-introduction of P-dopants and anionic vacancies upshifts the d -band center of HE-MX, optimizing polysulfide adsorption, substantially reducing the energy barriers for Li 2 S nucleation/decomposition, and accelerating Li + diffusion. This multifunctional electrocatalytic enhancement markedly expedites overall sulfur redox kinetics. Consequently, the cell employing the P-HE-MX@C modified separator achieves a low-capacity decay rate of 0.048% per cycle over 900 cycles at 1.0 C. Even under a high sulfur loading (5.69 mg cm −2 ) and a lean electrolyte (4.53 μL mg −1 ), the cell still delivers a high areal capacity of 5.67 mAh cm −2 at 0.1 C after 100 cycles. Additionally, the pouch cell with high sulfur loading maintains an ultrahigh capacity of 1.92 Ah over 20 cycles. This work establishes a fundamental design principle for the synergistic electronic engineering of high-entropy electrocatalysts, facilitating the development of high-energy, long-lifespan energy storage systems.
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Ke-Meng Song,Shi-Ye Chang,Yuan Yuan,Fang-Lei Zeng,Ning Li,Han-Bing Chen,Ping Lu,Ning-Yi Yuan,Jian-Ning Ding
Lithium (Li) metal’s extremely high specific energy and low potential make it critical for high-performance batteries. However, uncontrolled dendrite growth and an unstable solid-electrolyte interphase (SEI) during repeated cycling still seriously hinder its practical application in Li metal batteries. Herein, we demonstrate a facile and effective approach to fabricate a flexible and robust hybrid SEI layer using two kinds of organo-polysulfides with different sulfur chain lengths [bis(3-(triethoxysilyl)propyl)disulfide (Si–O–2S) and bis(3-(triethoxysilyl)propyl)tetrasulfide (Si–O–4S)] as the additives in the electrolyte. Compared to Si–O–2S, the siloxane and the long sulfur chain in Si–O–4S are conducive to the production of LixSiSy inorganic components on lithium metal surfaces and the formation of an organic–inorganic hybrid stable SEI layer in conjunction with LixSiOy, thereby improving the stability of the SEI layer and inhibiting the growth of lithium dendrites. Specifically, with 10 wt % Si–O–4S as the additive, an excellent cycling lifespan (1400 h) was achieved with a low hysteresis voltage of ∼17 mV at 1.0 mA cm–2 in a Li–Li symmetrical cell. Moreover, the lithium–sulfur battery also exhibits long cycling stability (850 mA h g–1 at 0.5 C after 200 cycles) and good Coulombic efficiency (99.5%). This study provides an electrolyte additive strategy for the Li anode fabricating a stable SEI layer and long cycling batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
eScience
·
2025
·
IF 36.6
Lijing Wang,Chang Wu,Yu Gao,Hongfang Du,Shailendra K. Sharma,Aaron T. Marshall,Yang Liu,Yi Zhao,Shixue Dou,Liang Huang,Shaowei Zhang,Chao Wu,Liangxu Lin
The catalytic conversion of polysulfides remains a critical bottleneck in the development of high-performance lithium–sulfur batteries (LSBs). Despite extensive efforts to engineer carbon-based materials for LSBs, such as nitrogen (N)-doped graphene, the intrinsic limitations of conventional N-doped configurations have hindered catalytic effectiveness. Here, we reveal how the curvature-rich structure of N-doped graphene (N-CR-G) regulates catalytic properties to promote the sulfur reduction reaction (SRR). This architecture induces a diversity of active N configurations and optimizes the local electronic structure, directly accelerating the polysulfide redox kinetics. Unlike conventional carbon-based materials, the main N-doped configuration of N-CR-G catalyzes an uncommon asymmetric reaction pathway involving the rapid generation of soluble radicals, effectively suppressing the accumulation of insoluble Li 2 S 2 intermediates and enhancing sulfur utilization. While the curvature structure also facilitates carbon vacancy formation and enables room-temperature N doping, its primary contribution lies in tailoring the catalytic landscape of graphene. This work underscores the significance of curvature engineering for activating and regulating electrocatalytic behavior, offering a powerful strategy to design advanced cathode materials for highly promising LSBs.
研究领域:
材料科学
·
电化学
·
储能技术
·
纳米技术
·
催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Zihan Huang,Zhixuan Zhang,Yifeng Han,Liya Rong,Hongling Yao,Changwen Li,Xianbao Wang,Tao Mei
The practical application of high-performance lithium‑sulfur batteries (LSB) was primarily hindered by polysulfides shuttling and sluggish sulfur redox kinetics. To overcome these limitations, this study introduces a multifunctional three-phase heterostructured TiO 2 /ZnS@MXene catalyst engineered to synergistically combine high adsorption capacity and strong catalytic activity. The TiO 2 component, known for its' strong chemical affinity and ZnS, serving as an efficient electrocatalyst, were homogeneously anchored onto the highly conductive MXene substrate via in situ growth. Additionally, the MXene hollow microsphere structure effectively inhibited the self-stacking of lamellar host to ensure the maximum exposure of the active sites, providing a favorable buffer space for the volume expansion throughout the reaction process. The elaborately integrated TiO 2 /ZnS@MXene heterostructure provides a synergistic effect to realize the function of sequential capture-diffusion-transformation of sulfur species throughout the reaction process. As a result, the LSB containing TiO 2 /ZnS@MXene heterostructures could retain 821.7 mAh g −1 after 1000 cycles at 1C with only 0.010 % capacity decay per cycle. Even with a sulfur content of 5.8 mg cm −2 and lean electrolyte conditions (5.1 μL mg −1 ), it still delivers an area capacity of 4.1 mAh cm −2 at 0.2C.
研究领域:
材料科学
·
电化学
·
能源存储
·
纳米材料
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Changfeng Zhao,Xiaoxia Yang,Guang Xia,Jinglei Liu,Wenqian Zhang,Jie Xue,Shifeng Hou,Cheng Hu
Li-S batteries have been regarded as one of the most prospective energy-storage systems because of its high-energy-density. To suppress the shuttling effect of dissolved lithium polysulfides, different mass ratios petal-like nickel hydroxide nanosheets (NHN) decorated reduced graphene oxide (rGO) materials are synthesized in this study using a one-step hydrothermal method and applied modified separators in Li-S batteries. With up to 73.5 wt% of sulfur content in the cathode, the optimized sample (the mass ratio of graphene oxide to nickel nitrate is 1:9) enables discharge capacities up to 1579 mAh g −1 at 0.2 C (the areal sulfur loading is 5 mg cm −2 ). The cell also exhibits a retention of 840 mAh g −1 in specific capacity after 200 cycles, exhibiting higher utilizations and better cycling stabilities for Li-S batteries. Electrochemical measurements and density functional theory (DFT) calculations prove that NHN plays a critical role in promoting the redox reaction kinetics of Li-S batteries, and the high conductivity of rGO enhances the electrochemical function of NHN. This study provides a low cost approach for the developments of modified separators in future practical Li-S batteries.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
高影响因子
Small
·
2023
·Vol. 19
·期 37
·2301085
·
IF 13.3
Guo Liu,Qi Zeng,Xinyi Sui,Shuhao Tian,Xiao Sun,Qingfeng Wu,Xijuan Li,Yuhao Zhang,Kun Tao,Erqing Xie,Zhenxing Zhang
Polysulfide shuttle effect and sluggish sulfur reaction kinetics severely impede the cycling stability and sulfur utilization of lithium-sulfur (Li-S) batteries. Modulating d-band electronic structures of molybdenum disulfide electrocatalysts via p/n doping is promising to boost polysulfide conversion and suppress polysulfide migration in lithium-sulfur batteries. Herein, p-type V-doped MoS 2 (V-MoS 2 ) and n-type Mn-doped MoS 2 (Mn-MoS 2 ) catalysts are well-designed. Experimental results and theoretical analyses reveal that both of them significantly increase the binding energy of polysulfides on the catalysts’ surface and accelerate the sluggish conversion kinetics of sulfur species. Particularly, the p-type V-MoS 2 catalyst exhibits a more obvious bidirectional catalytic effect. Electronic structure analysis further demonstrates that the superior anchoring and electrocatalytic activities are originated from the upward shift of the d-band center and the optimized electronic structure induced by duplex metal coupling. As a result, the Li-S batteries with V-MoS 2 modified separator exhibit a high initial capacity of 1607.2 mAh g −1 at 0.2 C and excellent rate and cycling performance. Moreover, even at a high sulfur loading of 6.84 mg cm −2 , a favorable initial areal capacity of 8.98 mAh cm −2 is achieved at 0.1 C. This work may bring widespread attention to atomic engineering in catalyst design for high-performance Li-S batteries.
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DOI
PubMed
高影响因子
Polymer Chemistry
·
2019
·Vol. 10
·期 21
·2697-2705
·
IF 4.76
Haixia Li,Wentao Tang,Yifu Huang,Wenhong Ruan,Mingqiu Zhang
Lithium–sulfur (Li–S) batteries have attracted tremendous attention as the next generation of lithium batteries. In the battery construction, a nanopore separator can improve the performance of the Li–S battery by working as a nanofiltration film, inhibiting the migration of soluble polysulfide ions between the electrodes. Herein, a new strategy to synthesize a nanopore separator of poly(propylene glycol)-co-pentaerythritol triacrylate (PPG-co-PETA) particles to suppress polysulfide shuttling has been proposed. The PPG-co-PETA cross-linked particles were easily obtained by a facile approach of UV-induced monomer polymerization while implementing molecular cross-linking for nanopore control. The characteristic nanopore size of the PPG-co-PETA separator ranged from ∼1.24 nm to ∼1.86 nm upon changing the type of photo-initiator and content of cross-linking agent. The results showed that the optimized separator for a Li–S battery could possess an electrolyte uptake of 350% with excellent thermal, mechanical and electrochemical properties. Notably, the Li–S battery using such a new type of nanopore separator exhibits superior retention discharge capacity (>200 cycles). It is believed that the nanopore separator of cross-linked PPG-co-PETA is a potential alternative to the commercial Celgard separator for effectively blocking polysulfide shuttling in Li–S batteries.
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DOI
高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Ling Zhang,Jiaying Bi,Tao Liu,Xiaorong Chu,Haijian Lv,Daobin Mu,Borong Wu,Feng Wu
The rapid decay of the charge/discharge capacity of lithium-sulfur batteries due to the sluggish reaction kinetics and the shuttling behaviour of soluble polysulfides significantly restricts their practical application in energy storage systems. Herein, two-dimensional TiN/TiC heterostructures embedded with single tungsten atoms (SWA) are developed and introduced as a modified interlayer (SWA-TiN/TiC) in Li-S battery devices. The SWA-TiN/TiC material has a large specific surface area, which provides a physical barrier while supplying numerous active sites for polysulfides reactions. TiN and TiC both demonstrate excellent electronic conductivity and catalytic activity, which facilitate the conversion of polysulfides. Meanwhile, the uniformly-dispersed SWAs significantly enhance the chemical affinity with polysulfides and accelerate their redox reactions. As a result, the sulfur cathodes coated with the SWA-TiN/TiC interlayer achieve excellent rate performance and long-term cycling stability. An ultrahigh specific capacity of up to 1577.7 mAh g −1 at 0.1 C is achieved, and even at high sulfur loading (6.25 mg cm −2 ), a high areal capacity of 4.63 mAh cm −2 is obtained. This work highlights the potential of single metallic atoms on non-carbonaceous matrix for the development of high-performance catalysts that can achieve strong polysulfides immobilization for practical applications in lithium-sulfur batteries.
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高影响因子
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