JOURNAL OF POWER SOURCES
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2022
·
IF 9.794
Chen Chang,Chengyin Yang,Qiyue Wu,Xuyang Wang,Hui Nie,Xingping Zhou,Xiaolin Xie,Bingjoe Hwang,Yunsheng Ye
Designing an optimum separator configuration that can address severe lithium polysulfide (LiPS) shuttling and uncontrollable Li dendrite growth at the evaluated temperature is imperative for developing a high-performance, reliable, and safe Li–S battery (LSB). Herein, a promising LSB separator design is proposed, which consists of LiPS catalytic layer (LCL) and thermal conductive layer (TCL) fabricated by dual side filtrating the flower-like vanadium pentoxide (V 2 O 5 ) microspheres and aluminum oxide (Al 2 O 3 ) nanosheets , respectively. The LCL between the separator and S-cathode as combined LiPS trapper and catalyst significantly improves the redox reaction and sulfur utilization. At the anode/separator interface, the TCL uniforms Li-ion flux and thermal distribution to prevent undesirable Li dendrite growth under the temperature gradient ( TG ) effect. The Janus-type LCL-TCL separator with two parallel functions can achieve synchronous improvements in cathodic and anodic performance in LSB. Consequently, the LSB with Janus-type LCL-TCL separator exhibits excellent cycling stability with an ultralow capacity decay rate of 0.036% per cycle over 2000 cycles at 1C and superior rate capability up to 4C. The novel strategy can pave a new way to simultaneously tackle the limitations faced by anode and cathode in LSB.
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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
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Tong Wu,Jinting Ye,Tunan Li,Yuong Liu,Liu Jia,Liqun Sun,Jinghai Liu,Haiming Xie
Numerous efforts can improve reversible capacity and long cycling stability for lithium-sulfur (Li–S) batteries, however, challenges remain in achieving high sulfur utilization and suppressing the shuttle effect , especially for cells with a low electrolyte/sulfur (E/S) ratio. In this research, we utilize tetrathiafulvalene (TTF) as multifunctional catalyst for high-performance Li–S batteries through optimizing electrolyte chemistry for the first time. With TTF additive in electrolyte, it acts as π-electron donor molecule to improve the electron transport of Li 2 S x due to the van der Waals interaction , and promote LiNO 3 to Li 3 N to form highly conductive passivation layer on lithium anode (Li-anode). Furthermore, TTF functions as a catalyst to improve the redox kinetics of Li 2 S x thus slowing down the “shuttle effect”, improve the utilization of sulfur, and protect the Li-anode. As a result, the cell with TTF exhibits excellent performances with high discharge capacity (1359 mAh g −1 at 0.1C), long-term cycling stability (509 mAh g −1 after 500 cycles at 0.5C), and excellent cycling performance even at low E/S ratio (5.5 μL mg −1 ) (initial discharge capacity of 1129 mAh g −1 with a capacity decay rate of 0.20% per cycle at 0.1C for 200 cycles).
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高影响因子
Nanoscale
·
2020
·Vol. 12
·期 47
·24196-24205
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IF 6.895
Heng Zhang,Peigen Zhang,Long Pan,Wei He,Qi Qi,Zhuoheng Bao,Li Yang,Wei Zhang,Michel W. Barsoum,ZhengMing Sun
Lithium–sulfur (Li–S) batteries are regarded as potential next-generation energy storage systems due to their high theoretical energy densities. However, the dissolution of lithium polysulfides (LiPSs) upon cycling can result in severe capacity degradation. Achieving high rate capabilities with good cycling stability remains a huge obstacle for the practical implementation of Li–S batteries. Here we developed a novel, multifunctional, hierarchical structure by self-assembling core–shell MnO2 nanorods @ hollow porous carbon with 2D Ti3C2Tx nanosheets, labelled as MCT, as an efficient polysulfide mediator for Li–S cathodes. The integration of the polar MnO2 core and hollow porous carbon shell captures LiPSs two ways: physical confinement and chemisorption. The conductive Ti3C2Tx nanosheets construct a continuous and conductive network, which not only promotes charge transfer and ion diffusion but also boosts LiPS adsorption and conversion. Based on these merits, the MCT/S cathode delivers good rate capability (688 mA h g−1 at 2.0C) and outstanding long-term cyclability (0.044% capacity decay per cycle over 600 cycles at 2.0C).
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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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高影响因子
ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Zhifei Liu,Chunxiang Lu,Shuxia Yuan,Wei Cui,Shijie Wu,Xiaodan Ren,You Chen
As a prospective substitution for conventional lithium-ion batteries, lithium–sulfur batteries have been propelled into the spotlight on account of their merits, such as high energy density and ecofriendliness, among other things. Their commercialization, however, has run up against thorny impediments, with them primarily embodying sluggish evolution kinetics of sulfur species, the adverse shuttle effect of soluble polysulfide ions, and insufficient electronic conductivity of S8/Li2S2/Li2S. Herein, a multifunctional separator modifier based on porous carbonaceous microspheres inlaid with Fe3Se4 nanoparticles (Fe3Se4/PCM) is proposed to surmount these hurdles. The porous carbon skeleton offers a wealth of adsorption sites for the physical immobilization of polysulfides in tandem with excellent electrical conductivity. Beyond chemically fixing polysulfide intermediates, the embedded Fe3Se4 can facilitate the conversion reaction from Li2S2 to Li2S. Attributed to the superiority of Fe3Se4/PCM, the final batteries deliver a high utilization rate of sulfur (1179.2 mAh·g–1 at 0.1 C), a superb rate capability of 486.4 mAh·g–1 at 3 C, and prolonged cycling stability (a low degradation rate of 0.04% per cycle over 500 cycles at 1 C). This work may provide a novel formula for designing a string of transition-metal selenides/porous carbon composites as separator modifiers to achieve robust lithium–sulfur batteries.
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高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Xiaoli Peng,Pengfei Wan,Long Yuan,Shilan Li,Shengdong Jing,Fuyu Xiao,Lingxing Zeng,Yaozhu Tian,Zhu Luo,Haosen Fan
The slow redox kinetics and shuttle effect of polysulfides are primary challenges that hinder the further application of lithium-sulfur batteries (LSBs) due to the poor conductivity of sulfur and low sulfur utilization. Separator modification through synergistic capture-catalysis-conversion of polysulfides proves to be an effective approach to address these challenges. In this paper, we successfully design and prepare double shell core-shell Co@Co 9 S 8 @NSC nanocrystals encapsulated in sulfur- and nitrogen-co-doped carbon nanotubes (Co@Co 9 S 8 @NSC) as a separator modifier for LSBs. The modified layer (Co@Co 9 S 8 @NSC//PP) exhibits excellent adsorption-catalytic properties, effectively immobilizing soluble lithium polysulfides (LiPSs) and promoting their electrochemical conversion, thereby enhancing lithium ion (Li + ) transport and facilitating a homogeneous lithium deposition process. When we utilize the Co@Co 9 S 8 core-shell structure to coat the polypropylene (PP) separator, the results demonstrate that the modified separator achieves a high reversible capacity of 591 mAh g −1 after 500 cycles at 1 C and reaches a reversible capacity of 442 mAh g −1 after 1000 cycles at 2 C, accompanied by a low capacity decay rate of only 0.05 % per cycle. The Li/Li symmetric batteries, which have Co@Co 9 S 8 @NSC-coated separators, exhibit long lifetimes exceeding 800 h at current densities of 2 mA cm −2 and 2 mAh cm −2 , along with a low voltage hysteresis of approximately 55 mV. This provides enhanced lithium stripping/plating stability compared to Li/Li symmetric batteries with pure PP separators. This study presents a novel approach to interlayer construction to achieve high sulfur utilization in long-life LSBs by accelerating the redox kinetics of LiPS and mitigating the shuttle effect.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Guanyu Mu,Min Hu,Xin Tian,Xin Ma,Junwu Xiao,Fei Xiao,Shuai Wang
Adsorption and catalytic conversion of polysulfides plays a pivotal role in improving the reaction dynamics and mitigating the shuttle effect within lithium-sulfur (Li-S) batteries. Nevertheless, overly strong adsorption will commonly hinder the conversion of polysulfides leading to low cycling stability. Herein, x Fe-CoP catalysts were designed and synthesized by introducing the sulfur-affinity metal Fe to establish a synergistic balancing network of “moderate capturing” “accelerated catalysis” and “rapid conversion” of polysulfide to improve the Li-S reaction kinetics. In combination with theoretical analysis, we evaluate the affinity effect between catalysts with different Fe content and polysulfide, and emphasize the role of moderate adsorption. Consequently, the sulfur-loaded x Fe-CoP ( 0.33 Fe-CoP/S) delivered a high initial discharge capacity of 1441 mAh g −1 at 0.1C and manifested impressive cyclic performances with 84.2 % capacity retention over 500 cycles at 1.0C. Even with a sulfur loading of 6.5 mg cm −2 and low electrolyte/sulfur ratio (E/S) of 3.7 µL mg −1 , the cell demonstrates an attainable areal capacity of 7.0 mAh cm −2 . This research is poised to establish a theoretical framework for developing high-capacity, long-life Li-S batteries with high sulfur load and lean electrolyte requirements.
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PubMed
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Yingjie Zhang,Yuzheng Li,Chengxiao Xu,Daming Li,Jun Cao,Peipei Huo
Lithium‑sulfur batteries (LSBs) are recognized as promising candidates for the next generation of secondary batteries due to their high energy density, high theoretical capacity, and low environmental impact. However, the poor electrical conductivity of sulfur and Li 2 S, the “shuttle effect” of polysulfides, and the slow kinetics of redox reactions have significantly hindered the practical application of LSBs. In this work, CoSe 2 -loaded carbon nanofibers (CoSe 2 @CNF) derived from metal-organic frameworks were successfully prepared by electrospinning and used as a functional coating on the polypropylene separator. The three-dimensional network structure of CNFs not only improves the electrical conductivity of the material but also provides channels to facilitate ion and electron transport, while the CoSe 2 particles distributed on the surface effectively act as adsorption and catalytic active sites for lithium polysulfides. Under the synergistic effect, the CoSe 2 @CNF-modified separator suppressed the shuttle effect and significantly enhanced the kinetics of redox reactions. The LSBs assembled with CoSe 2 @CNF-modified separator exhibited excellent electrochemical performance, achieving an initial capacity of 1445.6 mAh g −1 at 0.5C and maintaining a discharge specific capacity of 849.5 mAh g −1 after 275 cycles.
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高影响因子
2D Materials
·
2022
·Vol. 9
·期 2
·025028
·
IF 6.861
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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高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 13
·7897-7906
·
IF 10.733
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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高影响因子
Energy Storage Materials
·
2017
·
IF 0
Chunlong Dai,Linyu Hu,Min-Qiang Wang,Yuming Chen,Jin Han,Jian Jiang,Yan Zhang,Bolei Shen,Yubin Niu,Shu-Juan Bao,Maowen Xu
Lithium-sulfur (Li-S) batteries are of great importance as promising electrochemical-energy storage systems in view of their overwhelming advantage of energy density . However, their commercial applications are still far away mainly due to fast capacity decay in a high sulfur content caused by low utilization of active material and severe polysulfide dissolution during electrochemical cycling. Here we have designed and prepared uniform α-Ni(OH) 2 hollow spheres constructed from ultrathin nanosheets with the thickness of ~3.5 nm as a hollow sulfur nanosphere host for Li-S batteries. Specifically, the synthesized hierarchical hollow spheres not only manifest the advantages of hollow structure and robust protective shell to encapsulate a very high content of sulfur up to 81 wt%, but also offer sufficient functionalized surfaces to directly bond and entrap polysulfides in hollow sphere. When used as cathode materials for Li-S batteries, the S@Ni(OH) 2 double-shell hollow hybrids exhibit a highly stable cycle life over 1000 cycles at 1 C with a very small capacity decay rate of only ~0.04% per cycle.
研究领域:
材料科学
·
能源存储
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