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1
Chung, Sheng-Heng, and Cun-Sheng Cheng. "(Digital Presentation) A Design of Nickel/Sulfur Energy-Storage Materials for Electrochemical Lithium-Sulfur Cells." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 542. http://dx.doi.org/10.1149/ma2022-024542mtgabs.
Повний текст джерелаАнотація:
Introduction As one of the next-generation rechargeable battery technologies beyond the lithium-ion chemistry, the lithium-sulfur chemistry enables the low-cost sulfur cathode to generate a high theoretical capacity of 1,675 mAh g-1 (10 times higher capacity than those of lithium-ion battery cathode). It further exhibits a high theoretical energy density of 2,600 Wh kg-1 in lithium-sulfur batteries (2–3 times higher energy density than lithium-ion batteries). However, as reported in recent publications, the development is far from adequate with respect to the high-loading sulfur cathode with high active-material content in building advanced lithium-sulfur batteries with a high energy density. The material challenges result from the use of an insulating sulfur as the active material, which would generate lithium polysulfides that can easily diffuse out from the cathode. The high cathode resistance and fast loss of the active material lead to the poor electrochemical utilization and efficiency of lithium-sulfur battery cathodes. These negative impacts subsequent derive the additional electrochemical challenges. A high amount of conductive and porous substrates is added in the cathode to replace the active material, which results in the limited amount of sulfur in the cathode and further blocks the improvement of designing high-energy-density sulfur cathodes. To address the above-mentioned issues, the research progresses of high-performance sulfur cathodes aim to design functional host for sulfur cathodes with the use of carbon for high conductivity, polymers for high ionic transfer, porous materials for physical polysulfide retention, polar materials for chemical polysulfide adsorption, catalysts for high reaction kinetics, etc. However, metallic materials that naturally have high conductivity, strong polysulfide adsorption capability, and catalytic conversion ability, are rarely reported. This is because metals have the highest density as compared to the aforementioned host materials, which commonly causes an insufficient amount of active material in the cathode and therefore inhibits the design of metal-sulfur nanocomposite in sulfur cathodes. To explore the metal/sulfur nanocomposite as a new research trend in sulfur cathodes, we propose a design for a nickel/sulfur nanocomposite as a novel energy-storage material by the electroless nickel plating method, and discuss its applications in lithium–sulfur battery cathodes. The nickel/sulfur energy-storage material possesses metallic nickel on the surface of the insulating sulfur particles as a result of the reduction of nickel ions during autocatalytic plating. By controlling the synthesis and fabrications conditions, the nickel/sulfur energy-storage material attains adjustable high sulfur contents of 60–95 wt% and adjustable high sulfur loadings of 2–10 mg cm−2 in the resulting cathode. The high-loading cathode with the nickel/sulfur energy-storage material demonstrates high electrochemical utilization and stability, which attains a high areal capacity of 8.2 mA∙h cm−2, an energy density of 17.3 mW∙h cm−2, and a stable cyclability for 100 cycles. Results and Discussion Here, in our presentation, we discuss our novel method for the fabrication of nickel/sulfur energy-storage material as an advanced composite cathode material for exploring battery electrochemistry and battery engineering. We adopt a modified electroless-plating method to synthesize nickel/sulfur energy-storage materials characterized by adjustable high sulfur contents and promising cathode performance. The plated nickel coating provides the nickel/sulfur energy-storage materials with metallic conductivity and polysulfide adsorption ability, which addresses the two major issues of sulfur cathodes.[1,2] Therefore, the nickel/sulfur energy-storage material attains high sulfur contents in the cathode and exhibits a high charge-storage capacity of 1,362 mA∙h g−1 and an excellent cyclability for 100 cycles. Moreover, the nickel/sulfur energy-storage material enables high-loading sulfur cathodes with a sulfur loading of 10 mg cm−2, a high areal capacity of 8.2 mA∙h cm−2, and an energy density of 17.3 mW∙h cm−2. Conclusion In summary, the summary of our nickel/sulfur energy-storage materials presented in this presentation would demonstrate a light-weight metallic nickel coating technique for fast charge transfer and strong polysulfide retention in the sulfur nanocomposites composite sulfur cathode. Moreover, our systematic analysis of the nickel/sulfur energy-storage materials exhibits their achievements in attaining both high electrochemical designs of high sulfur content and loading as well as possessing high energy density and electrochemical stability. References C.-S. Cheng, S.-H. Chung, Chem. Eng. J. 2022, 429, 132257. C.-S. Cheng, S.-H. Chung, Batter. Supercaps 2022, 5, e202100323.
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Yu, Chien-Hsun, Yin-Ju Yen, and Sheng-Heng Chung. "Nanoporosity of Carbon–Sulfur Nanocomposites toward the Lithium–Sulfur Battery Electrochemistry." Nanomaterials 11, no. 6 (June 8, 2021): 1518. http://dx.doi.org/10.3390/nano11061518.
Повний текст джерелаАнотація:
An ideal high-loading carbon–sulfur nanocomposite would enable high-energy-density lithium–sulfur batteries to show high electrochemical utilization, stability, and rate capability. Therefore, in this paper, we investigate the effects of the nanoporosity of various porous conductive carbon substrates (e.g., nonporous, microporous, micro/mesoporous, and macroporous carbons) on the electrochemical characteristics and cell performances of the resulting high-loading carbon–sulfur composite cathodes. The comparison analysis of this work demonstrates the importance of having high microporosity in the sulfur cathode substrate. The high-loading microporous carbon–sulfur cathode attains a high sulfur loading of 4 mg cm−2 and sulfur content of 80 wt% at a low electrolyte-to-sulfur ratio of 10 µL mg−1. The lithium–sulfur cell with the microporous carbon–sulfur cathode demonstrates excellent electrochemical performances, attaining a high discharge capacity approaching 1100 mA∙h g−1, a high-capacity retention of 75% after 100 cycles, and superior high-rate capability of C/20–C/3 with excellent reversibility.
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Weret, Misganaw Adigo, Wei-Nien Su, and Bing-Joe Hwang. "Organosulfur Cathodes with High Compatibility in Carbonate Ester Electrolytes for Long Cycle Lithium–Sulfur Batteries." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 536. http://dx.doi.org/10.1149/ma2022-024536mtgabs.
Повний текст джерелаАнотація:
Lithium-sulfur batteries (LSBs) are potential candidates for high energy storage technologies due to their theoretical gravimetric energy density of ∼2600 Wh kg-1 and lightweight electrodes. In LSBs, ether electrolytes are frequently utilized because sulfur cathodes and the polysulfide redox intermediate species are chemically stable. However, LSBs in ether electrolytes suffer from the dissolution of higher-order polysulfides, and migration of the soluble polysulfides into electrolytes causes the polysulfide shuttle effect. The shuttle polysulfides react with the lithium anode and give rise to the irreversible deposition of lithium sulfides, deteriorate the morphology of the anode, and cause rapid capacity fading. Moreover, ether electrolytes are highly flammable and trigger safety issues. As an alternative, carbonate ester electrolytes are promising choices to substitute ether electrolytes in LSBs. Organic carbonate electrolytes used in LSBs result in irreversible reactions with long-chain polysulfide anions that cause the cell to shut down. Therefore, carbonate ester electrolytes compatible sulfur cathodes design needs special attention. Sulfurized polyacrylonitrile (SPAN) and short-chain sulfur cathodes are compatible with organic carbonate electrolytes. However, the sulfur contents in these cathodes are mostly below 50 wt% which hamper the practical application of the LSBs. Here, we designed an organosulfur cathode with a high chemical bonded sulfur content of ~58 wt% in the cathode composite. The prepared organosulfur cathode showed excellent compatibility with carbonate ester electrolytes. The organosulfur cathode exhibits a high initial discharge capacity of 1301 mAh g-1 and long cycle stability for 400 cycles with nearly 99.99% coulombic efficiency.
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Kang, Jukyoung, Jong Won Park, Seok Kim, and Yongju Jung. "Three-Layer Sulfur Cathode with a Conductive Material-Free Middle Layer." Journal of Nanoscience and Nanotechnology 20, no. 8 (August 1, 2020): 4943–48. http://dx.doi.org/10.1166/jnn.2020.17846.
Повний текст джерелаАнотація:
An ingenious design for a three-layer sulfur cathode is demonstrated, in which the pure sulfur layer is sandwiched between carbon nanotube (CNT) films. The unique feature of this particular model is that the sulfur layer does not contain any conductive materials, and therefore, the top CNT film of the prepared three-layer CNT/S/CNT electrode is electrically isolated from the bottom CNT film. Scanning electron microscopy studies revealed that the three-layer cathode was transformed into a single CNT cathode, with proximate contact between the two CNT films in the upper plateau of the first discharge. The lithium–sulfur cells employing a CNT/S/CNT cathode exhibited remarkably enhanced performance in terms of the specific capacity, rate property, and cycling stability compared to the cells with a sulfur-coated CNT cathode. This can mainly be attributed to the top CNT film, which serves not only as an interlayer to trap the migrating polysulfides, but also as an electrode to facilitate the redox reaction of active materials. Such an innovative approach is promising as it may promote the rational design of high-performance sulfur cathodes.
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Song, Jiangxuan, Zhaoxin Yu, Terrence Xu, Shuru Chen, Hiesang Sohn, Michael Regula, and Donghai Wang. "Flexible freestanding sandwich-structured sulfur cathode with superior performance for lithium–sulfur batteries." J. Mater. Chem. A 2, no. 23 (2014): 8623–27. http://dx.doi.org/10.1039/c4ta00742e.
Повний текст джерелаАнотація:
Flexible freestanding sandwich-structured sulfur cathodes are developed for lithium–sulfur batteries, which exhibit excellent cycling stability and rate capability. A high areal capacity of ∼4 mA h cm−2 is also demonstrated based on this new cathode configuration.
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Li, Zhengzheng. "MnO 2 –graphene nanosheets wrapped mesoporous carbon/sulfur composite for lithium–sulfur batteries." Royal Society Open Science 5, no. 2 (February 2018): 171824. http://dx.doi.org/10.1098/rsos.171824.
Повний текст джерелаАнотація:
MnO 2 –graphene nanosheets wrapped mesoporous carbon/sulfur (MGN@MC/S) composite is successfully synthesized derived from metal–organic frameworks and investigated as cathode for lithium-ion batteries. Used as cathode, MGN@MC/S composite possesses electronic conductivity network for redox electron transfer and strong chemical bonding to lithium polysulfides, which enables low capacity loss to be achieved. MGN@MC/S cathodes exhibit high reversible capacity of 1475 mA h g −1 at 0.1 C and an ultra-low capacity fading of 0.042% per cycle at 1 C over 450 cycles.
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Shi, Zeyuan, Bo Gao, Rui Cai, Lei Wang, Wentao Liu, and Zhuo Chen. "Double Heteroatom Reconfigured Polar Catalytic Surface Powers High-Performance Lithium–Sulfur Batteries." Materials 15, no. 16 (August 18, 2022): 5674. http://dx.doi.org/10.3390/ma15165674.
Повний текст джерелаАнотація:
The modification of apolar carbon materials by heteroatom doping is an effective method that can effectively improve the surface polarity of carbon materials. In the main body of the lithium–sulfur battery cathode, the structural properties of the carbon material itself with porous structure and large specific surface area provide sufficient space for sulfur accommodation and mitigate the bulk effect of the sulfur cathode (79%). The polarized surface of the reconstructed carbon material possesses strong adsorption effect on LiPs, which mitigates the notorious “shuttle effect.” In this paper, the surface structure of the Ketjen black cathode body was reconstructed by B and N double heteroatoms to polarize it. The modified polarized Ketjen black improves the adsorption and anchoring ability of LiPs during the reaction and accelerates their kinetic conversion, while its own uniformly distributed small mesopores and oversized BET structural properties are beneficial to mitigate the bulk effect of sulfur cathodes. Lithium–sulfur batteries using B and N modified cathodes have an initial discharge capacity of 1344.49 mAh/g at 0.1 C and excellent cycling stability at 0.5 C (381.4 mAh/g after 100 cycles).
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El Mofid, Wassima, and Timo Soergel. "(Digital Presentation) Impact of the Sulfur Loading Method on the Morphological and Electrochemical Properties of Additive-Free Cathodes for Li-S Batteries Prepared By Composite Electroforming." ECS Meeting Abstracts MA2022-02, no. 1 (October 9, 2022): 86. http://dx.doi.org/10.1149/ma2022-02186mtgabs.
Повний текст джерелаАнотація:
In order to produce conductive agent and binder free electrodes for batteries with a synergistic optimization of the mechanical and electrical bonding of the active material, „composite electroforming“ synthesis method has been developed in Aalen University as a novel approach for additives-free battery electrodes production [1-6]. The aim throughout this method is to achieve high-performance accumulators with a focus on a high gravimetric and volumetric power and energy density. The aspects of energy efficiency, cycleability and safety are also considered, especially that the composite electroforming process allows environmentally friendly and resource-saving production of electrodes. The novel electrodes for Li-S batteries proposed in the present work are composed of Ni matrix which also acts as current collector, and sulfur loaded on etched Al alloy carrier particles AlSi10Mg. The sulfur loading which is a key step of our cathodes manufacturing was conducted using two different ways; by spin coating in melted sulfur at 160°C or by electrochemical loading using potasium sulfide based aqueous electrolyte (K2S)aq and applying a current density of 0,5 A/dm² at room temperature. SEM and elemental mapping measurements of the sulfur spin coated cathode and that with electrochemically loaded sulfur showed a big difference in terms of the sulfur distribution and the surface morphology between the two cathodes. Electrochemical characterization of the sulfur cathodes was then conducted, mainly galvanostatic cycling (GC), by imposing a fixed current to the cell between the two potential limits 1.7 and 2.8 V vs. Li+/Li. The rate, namely the current density applied to the electrode during cycling, was calculated based on the loaded sulfur mass in the tested electrode and the theoretical capacity of sulfur (1673 mAh g-1). By calculating the ratio of the active to the total loaded sulfur, the sulfur accessibilty for the electrochemically loaded cathode was five times higher than the spin coated cathode regardless of holding almost the same sulfur loading (3.9 mg/cm² and 3.96 mg/cm² respectivelly). GC at C/10 rate proved that the two cathodes delivered different values of specific capacity, capacity retention with cycling and coulombic efficiency that are significantly improved for the electrochemically loaded cathode than the spin coated one. Finally, In order to characterize the response of the sulfur electrochemically loaded cathode to different C rates, rate capability test was carried out and illustrated that the tested cathode was able to regain almost its entire initial capacity when back to the initial C rate after applying high C rates. [1]. C. Erhardt, Ş. Sörgel, S. Meinhard, T. Sörgel, J. Power Sources, 296 (2015) 70–77; [2]. T. Sörgel, S. Meinhard, Ş. Sörgel, Film Composite Material, EP 3114721, 2019; [3]. C. Erhardt, S. Meinhard, Ş. Sörgel, T. Sörgel, Galvanotechnik (2015) 7; [4]. V.C. Erhardt, S. Sörgel, S. Meinhard, T. Sörgel, H. Aalen, Jahrb. Oberflächentechnik, 71 (2015) 12; [5]. Ş. Sörgel, O. Kesten, A. Wengel, T. Sörgel, Energy Storage Mater., 10 (2018) 223–232; [6]. T. Sörgel, J. Meyer, WOMag, 9 (2013) 24–33.
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Ramezanitaghartapeh, Mohammad, Mustafa Musameh, Anthony F. Hollenkamp, and Peter J. Mahon. "Conjugated Microporous Polycarbazole-Sulfur Cathode Used in a Lithium-Sulfur Battery." Journal of The Electrochemical Society 168, no. 11 (November 1, 2021): 110542. http://dx.doi.org/10.1149/1945-7111/ac384f.
Повний текст джерелаАнотація:
The electropolymerization of Conjugated Microporous Poly-1,3,5-tris (N-carbazolyl) benzene (CMPTCBz) was investigated using a range of techniques. After the potential window was optimized for the electropolymerization process, a fixed potential was found to generate a CMPTCBz with minimal overoxidation and a high BET surface area. The CMPTCBz was mixed with sulfur and used in the optimized preparation of CMPTCBz-S cathodes. Coin cells were assembled with lithium metal used as the anode and electrochemically evaluated. Results showed that the CMPTCBz-S cathodes with different sulfur loadings have excellent charge/discharge cycling performance with initial discharge capacities ranging from 800 to 1400 mAh·g−1S and a capacity retention greater than 80% after 100 cycles. This is due to both the enhanced electrical conductivity of the cathode and physical confinement of the generated lithium-polysulfides inside the pores of the CMPTCBz. In a further experiment, a high sulfur loaded CMPTCBz-S cathode produced an initial discharge capacity of 548 mAh·g−1S and a capacity retention of 95% after 100 cycles using an organic electrolyte. Analysis using XPS showed that the sulfur to polysulfide conversion coupled with the dual functionality of the CMPTCBz in retaining the generated polysulfide are the key parameters for this superior performance.
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Suzanowicz, Artur M., Youngjin Lee, Hao Lin, Otavio J. J. Marques, Carlo U. Segre, and Braja K. Mandal. "A New Graphitic Nitride and Reduced Graphene Oxide-Based Sulfur Cathode for High-Capacity Lithium-Sulfur Cells." Energies 15, no. 3 (January 19, 2022): 702. http://dx.doi.org/10.3390/en15030702.
Повний текст джерелаАнотація:
Lithium-sulfur (Li-S) batteries can provide at least three times higher energy density than lithium-ion (Li-Ion) batteries. However, Li-S batteries suffer from a phenomenon called the polysulfide shuttle (PSS) that prevents the commercialization of these batteries. The PSS has several undesirable effects, such as depletion of active materials from the cathode, deleterious reactions between the lithium anode and electrolyte soluble lithium polysulfides, resulting in unfavorable coulombic efficiency, and poor cycle life of the battery. In this study, a new sulfur cathode composed of graphitic nitride as the polysulfide absorbing material and reduced graphene oxide as the conductive carbon host has been synthesized to rectify the problems associated with the PSS effect. This composite cathode design effectively retains lithium polysulfide intermediates within the cathode structure. The S@RGO/GN cathode displayed excellent capacity retention compared to similar RGO-based sulfur cathodes published by other groups by delivering an initial specific capacity of 1415 mA h g−1 at 0.2 C. In addition, the long-term cycling stability was outstanding (capacity decay at the rate of only 0.2% per cycle after 150 cycles).
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Perez Beltran, Saul, and Perla B. Balbuena. "First-principles explorations of the electrochemical lithiation dynamics of a multilayer graphene nanosheet-based sulfur–carbon composite." Journal of Materials Chemistry A 6, no. 37 (2018): 18084–94. http://dx.doi.org/10.1039/c8ta04375b.
Повний текст джерелаАнотація:
Graphitized-polymer-based sulfur cathodes have emerged as alternative cathode materials that are able to overcome many of the technical challenges that currently hinder lithium–sulfur (Li–S) batteries from their use in long-term high-energy applications.
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Pan, Hui. "Cationic MOF-Based Cu/Mo Bimetal Doped Multifunctional Carbon Nanofibers As Efficient Catalyst for High Sulfur Loading Lithium-Sulfur Batteries." ECS Meeting Abstracts MA2022-02, no. 64 (October 9, 2022): 2297. http://dx.doi.org/10.1149/ma2022-02642297mtgabs.
Повний текст джерелаАнотація:
High sulfur loading is the key to achieve high energy density promised by lithium-sulfur (Li-S) batteries. However, serious problems such as low sulfur utilization, poor rate performance and cycle stability have been exposed during the scaling up of the sulfur loading for freestanding cathodes. To address these issues, the adsorption/catalytic ability of high sulfur loading cathode toward polysulfides must be improved. Herein, based on excellent properties of cationic MOFs, we proposed that Cu-Mo bimetallic nanoparticles embedded in multifunctional freestanding nitrogen-doped porous carbon nanofiber (Cu-Mo@NPCN) with efficient catalytic sites and high sulfur loading capacity could be prepared by facile transition metal-based anion exchange of cationic MOFs. And the sulfur embedded in Cu-Mo@NPCN was directly used as freestanding sulfur cathodes, enabling a high areal capacity, good rate performance, and cycling stability even under high sulfur loading. The freestanding Cu-Mo@NPCN/10.3S achieves high areal capacity of 9.3 mA h cm-2 and volumetric capacity of 1163 mA h cm-3 at 0.2 C with a sulfur loading of 10.3 mg cm-2. This work provides new insights into freestanding sulfur cathode engineering for high-performance Li-S batteries and would advance the development of cationic MOF-derived bimetallic catalysts in various energy storage technologies. Figure 1
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Hawes, Gillian, Christian Punckt, and Michael Pope. "Examining Sulfur Nucleation and Growth on Carbon Nanomaterials from Aqueous, Elemental Sulfur Sols for Lithium−Sulfur Batteries." ECS Meeting Abstracts MA2022-01, no. 1 (July 7, 2022): 84. http://dx.doi.org/10.1149/ma2022-01184mtgabs.
Повний текст джерелаАнотація:
With decades of engineering, lithium-ion batteries are beginning to reach their fundamental energy density limits. As such, next generation chemistries that can store significantly more energy are essential for electrification of vehicles, improved portable electronics, and increased adoption of renewable energy sources. Lithium-sulfur batteries have attracted significant research attention due to their theoretical full cell capacity (1167 mAh/g) and gravimetric energy density (2500 Wh/kg) which are both an order of magnitude higher than conventional lithium-ion batteries. Furthermore, lithium-sulfur batteries employ elemental sulfur as the cathode material, which is both widely abundant and inexpensive, and also a common waste product of the petroleum industry, making the projected cost of lithium-sulfur cells per kWh much lower than conventional lithium-ion cells that rely on costly lithium transition metal oxide-based cathodes. However, a number of challenges plague the lithium-sulfur chemistry, one of the most critical being that elemental sulfur and its final discharge product, Li2S, are insulating in nature, requiring sulfur to be intimately mixed with a conductive, lightweight carbon material in order to facilitate electron transport. Because sulfur is typically redistributed throughout the cathode during cycling due to dissolution of intermediate polysulfide species in the electrolyte, the uniform coating of sulfur onto carbon materials has not garnered significant research attention. However, uniform distribution of the sulfur within the cathode is critical for several reasons. Large, insulating sulfur particles are not electrochemically converted during cycling, limiting cell capacity, and as sulfur undergoes an 80% volume change during cycling, non-uniform sulfur distribution can result in mechanical failure of the cathode. Moreover, as the field moves toward all-solid-state batteries, in which sulfur redistribution does not occur, the initial sulfur distribution within the cathode is critical for high performance cells. Nanoscale mixing of sulfur and carbon additives is typically achieved via melt imbibition, a lengthy, high-temperature process in which sulfur is melted and then used to coat solid carbon powders. This process typically employs carbon nanomaterials as aggregated solid powders, thereby limiting the accessible surface area that can be coated by sulfur. To access the exceptional surface area of carbon nanomaterials such as graphene (~2630 m2/g), the sulfur coating process needs to occur while the carbon nanomaterials are dispersed in solvent. While this has been demonstrated previously, it is typically done with highly toxic solvents such as CS2 due to sulfur’s limited solubility, or by using more costly and inefficient sulfur precursors, known as hydrophilic sulfur sols, to form elemental sulfur in situ. We demonstrate, for the first time, the use of aqueous, hydrophobic sulfur sols to coat carbon nanomaterials in solution at room temperature. Hydrophobic sulfur sols are sub-micron, metastable sulfur particles which are formed via the rapid dilution of an organic solution of sulfur into large quantities of water. We demonstrate that due to the metastable nature of these hydrophobic sulfur sols in the aqueous system, sulfur dissolves out of the sols and can uniformly coat the surface of dispersed carbon nanomaterials such as reduced graphene oxide (rGO) via a heterogeneous nucleation and growth process. This process is simple, scalable, employs inexpensive elemental sulfur directly, and can be performed at room temperature with an aqueous system, making it an attractive method to prepare sulfur cathodes. We study how the sulfur deposition process is affected by the introduction of a surfactant into the aqueous phase and the use of different organic solvents to prepare the sol, and further demonstrate that heterogeneous sulfur nucleation occurs preferentially with rGO, while a competing, undesirable homogeneous nucleation pathway that forms large insulating sulfur crystals is observed for Ketjen black and graphene oxide. We demonstrate that via this approach, high loading (3-4 mgsulfur/cm2) rGO/sulfur cathodes can be prepared that achieve capacities of 1300 mAh/g (~4.8 mAh/cm2) at 0.1C, and capacities 7-fold higher than cells prepared via traditional melt imbibition approaches at higher C rates of 0.8C and 1C. Moreover, we demonstrate that these cells can be prepared without additional conductive additives or binder and can achieve projected energy densities of ~468 Wh/kg at 0.1C when considering all inactive components and no lithium degradation, indicating the promise of this simple, novel approach for high energy density sulfur cathodes.
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Capkova, Dominika, Tomas Kazda, Ondrej Petruš, Ján Macko, Kamil Jasso, A. Baskevich, Elena Shembel, and Andrea Strakova Fedorkova. "Pyrite as a Low-Cost Additive in Sulfur Cathode Material for Stable Cycle Performance." ECS Transactions 105, no. 1 (November 30, 2021): 191–98. http://dx.doi.org/10.1149/10501.0191ecst.
Повний текст джерелаАнотація:
Various materials have been reported as an efficient host for sulfur to suppress large volume variation and polysulfide shuttle in lithium-sulfur batteries. Carbon materials are widely used as a matrix for sulfur to improve cycle performance and confine sulfur. Addition of transition metal sulfides into cathode material can improve cycle stability due to high efficiency of chemisorption and suppressing the polysulfide diffusion. In this work, various additions of pyrite to carbon and sulfur in the cathode material were investigated. The results show that the amount of pyrite has an affect on capacity and cycle stability of the electrode. Consequently, the lithium-sulfur batteries with the composite cathodes, containing 10 % of pyrite, exhibits stable discharge capacity of 788 mAh g-1 after 60 cycles at 0.2 C. Pyrite is a promising electrocatalyst in advanced lithium-sulfur batteries in the merits of low-cost, eco-friendliness and high activity towards polysulfides conversion reaction.
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Quay, Yee-Jun, and Sheng-Heng Chung. "Structural and Surfacial Modification of Carbon Nanofoam as an Interlayer for Electrochemically Stable Lithium-Sulfur Cells." Nanomaterials 11, no. 12 (December 9, 2021): 3342. http://dx.doi.org/10.3390/nano11123342.
Повний текст джерелаАнотація:
Electrochemical lithium-sulfur batteries engage the attention of researchers due to their high-capacity sulfur cathodes, which meet the increasing energy-density needs of next-generation energy-storage systems. We present here the design, modification, and investigation of a carbon nanofoam as the interlayer in a lithium-sulfur cell to enable its high-loading sulfur cathode to attain high electrochemical utilization, efficiency, and stability. The carbon-nanofoam interlayer features a porous and tortuous carbon network that accelerates the charge transfer while decelerating the polysulfide diffusion. The improved cell demonstrates a high electrochemical utilization of over 80% and an enhanced stability of 200 cycles. With such a high-performance cell configuration, we investigate how the battery chemistry is affected by an additional polysulfide-trapping MoS2 layer and an additional electron-transferring graphene layer on the interlayer. Our results confirm that the cell-configuration modification brings major benefits to the development of a high-loading sulfur cathode for excellent electrochemical performances. We further demonstrate a high-loading cathode with the carbon-nanofoam interlayer, which attains a high sulfur loading of 8 mg cm−2, an excellent areal capacity of 8.7 mAh cm−2, and a superior energy density of 18.7 mWh cm−2 at a low electrolyte-to-sulfur ratio of 10 µL mg−1.
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Kang, Jukyoung, and Yongju Jung. "Free-Standing Sulfur-Carbon Nanotube Electrode with a Deposited Sulfur Layer for High-Energy Lithium-Sulfur Batteries." Journal of Nanoscience and Nanotechnology 20, no. 8 (August 1, 2020): 5019–23. http://dx.doi.org/10.1166/jnn.2020.17847.
Повний текст джерелаАнотація:
To obtain a high S-loading cathode for a Li–S battery, we propose a free-standing carbon nanotube (CNT)-based S cathode, which consists of two layers: a pure S deposition layer with a thickness of 20 μm, and a S-containing CNT film (S-CNT). Based on scanning electron microscopic (SEM) studies, it was observed that the S layer completely vanished when the cell with the S/S-CNT cathode was discharged to 2.1 V after cell assembly, indicating that the thick sulfur film dissolved in the form of polysulfide intermediates during discharge. The proposed S/S-CNT cathode delivered double the areal capacity with good capacity retention of 83% after 100 cycles, compared with that of the control cathode (S-CNT). Thus, we believe that our new cathode design will be useful in developing stable, high-energy Li–S batteries.
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Song, Wenming, Changmeng Xu, Mai Li, Zhi Cheng, Yunjie Liu, Peng Wang, and Zhiming Liu. "Cobalt Nanocluster-Doped Carbon Micro-Spheres with Multilevel Porous Structure for High-Performance Lithium-Sulfur Batteries." Energies 16, no. 1 (December 26, 2022): 247. http://dx.doi.org/10.3390/en16010247.
Повний текст джерелаАнотація:
Lithium-Sulfur batteries (Li-S batteries) have gained great interest in next-generation energy storage systems due to their high energy density and low-cost sulfur cathodes. There is, however, a serious obstacle in the commercial application of Li-S batteries due to the poor kinetics of the redox process at the sulfur cathode and the “shuttle effect” caused by lithium polysulfide (LiPSs). Herein, we report the synthesis of a sulfur cathode host material that can drastically inhibit the “shuttle effect” and catalyze the conversion of LiPSs by a simple electrostatic spray technique, namely, cobalt (Co) nanoclusters doped with N-containing porous carbon spheres (Co/N-PCSs). The results show that Co/N-PCSs has catalytic activity for the transformation of liquid LiPSs to solid Li2S and alleviates the notorious “shuttle effect.” This new sulfur cathode exhibits stable running for 300 cycles accompanied by a capacity of 650 mAh g−1 at a current density of 1 C, a capacity fading rate of 0.051% per cycle, and a Coulombic efficiency maintained at close to 100%. The results demonstrate that Co/N-PCSs offers the possibility of practical applications for high-performance Li-S batteries.
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Marangon, Vittorio, Daniele Di Lecce, Fabio Orsatti, Dan J. L. Brett, Paul R. Shearing, and Jusef Hassoun. "Investigating high-performance sulfur–metal nanocomposites for lithium batteries." Sustainable Energy & Fuels 4, no. 6 (2020): 2907–23. http://dx.doi.org/10.1039/d0se00134a.
Повний текст джерелаАнотація:
X-ray tomography and electrochemistry shed light on a novel approach to prepare high-performance cathodes for lithium–sulfur batteries. Metal nanoparticles promote beneficial microstructural reorganizations in the cathode during the cycling process.
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Kalutara Koralalage, Milinda, Varun Shreyas, William Richard Arnold, Sharmin Akter, Arjun Thapa, Jacek Bogdan Jasinski, Gamini Sumanasekera, Hui Wang, and Badri Narayanan. "Quasi-Solid-State Lithium-Sulfur Batteries Consist of Super P – Sulfur Composite Cathode." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 541. http://dx.doi.org/10.1149/ma2022-024541mtgabs.
Повний текст джерелаАнотація:
Lithium-Sulfur (Li-S) batteries stand out to be one of the most promising candidates to meet the current energy storage requirement, with its natural abundance of materials, high theoretical capacity of 1672 mAhg-1, high energy density of 2600 Whkg-1, and low cost and lower environmental impact. Sulfur itself (S8), Li2S2 and Li2S formed during the discharge process, are electrical insulators and hence reduce the active material utilization and the electronic conductivity of the cathode affecting the battery performance. Combining of Carbon Super P (SP) with sulfur in cathode formulation is used to overcome these issues. In Liquid electrolyte batteries, polysulfides formed while charging and discharging, easily dissolve in liquid electrolyte and the resulting polysulfide shuttling leads to poor coulombic efficiency and cyclability. Liquid electrolytes used in the conventional Li-S batteries are easy to flow and become flammable. Further, Lithium dendrites piercing through separator causing short circuit paths leads to safety concerns. Replacement of the liquid electrolyte by a solid-state electrolyte (SSE) proves to be a strategy to overcome above mentioned issues. Sulfide based solid electrolytes have received greater attention due to their higher ionic conductivity, compatible interface with sulfur-based cathodes, and lower grain boundary resistance. Novel Li6PS5F0.5Cl0.5 due to its remarkable ionic conductivity of 3.5 x 10-4 S cm-1 makes it an excellent candidate for use in a Li-S solid state battery. However, the interface between SSEs and cathodes has become a challenge to be addressed in all solid-state Li-S batteries due to the rigidity of the participating surfaces. A hybrid electrolyte containing of SSE coupled with a small amount of ionic liquid at the interface, has been employed to improve the interface contact of the SSE with the electrodes. Cathode formulation consisting of sulfur as the active material, Super P as the conductive carbon black, acetylene carbon black as conductive carbon additive, with water based carboxymethyl cellulose (CMC) solution and Styrene butadiene rubber (SBR) as the binder was successfully developed. Thermo gravimetric analysis (TGA) studies of the cathode were carried out by the thermo gravimetric analyzer TA 2050 under N2 gas flow of 100 ml/min. Cathode surface morphology was characterized using the Field emission gun scanning electron microscope (FEI), TESCAN scanning electron microscope with energy dispersive X-ray spectroscopy (EDAX). Using a solvent-based process, Li6PS5F0.5Cl0.5 and Li6PS5F0.5Cl2 SSE were synthesized via the introduction of LiF into the argyrodite crystal structure, which enhances both the ionic conductivity and interface-stabilizing properties of the SSE. Relevant Ionic Liquids (IL) were prepared using Lithium bis(trifluoromethyl sulfonyl)imide (LiTFSI) as salt, with premixed pyrrolidinium bis(trifluoromethyl sulfonyl)imide (PYR) as solvent and 1,3-dioxolane (DOL) as diluent. SP-S cathode with 0.70 mgcm-2 sulfur loading was punched into disks of 2.0 cm2. SSE was pressed into 150 mg pellets using a stainless-steel tank. During the assembly, SSE was wetted with total of 40 μl of IL (LiTFSI dissolved in PYR and DOL solution) from both ends using a micropipette. 2032 type coin cells of Quasi-solid-state Li-S batteries (QSSLSB) consisting of SP-S based composite cathodes, Li anodes and novel Li6PS5F0.5Cl0.5 SSE were tested with an ionic liquid wetting both electrode-SSE interfaces. All the QSSLSB were cycled at 30 °C between 1.0 V and 2.8 V using an 8 channel Arbin battery testing system. Effect of IL dilution, co-solvent amount, LiTFSI concentration and C rate at which the batteries are tested, were systematically studied and optimized to develop a QSSLSB with higher capacity retention and cyclability. Optimum batteries had initial discharge capacity >1100 mAh/g and discharge capacity >400 mAh/g after 100 cycles at the C rate of C/10 with a significant coulombic efficiency. 40 μl of LiTFSI (2M) dissolved in PYR:DOL(1:1) IL was found to be optimum for high performance QSSEBs with low sulfur loading of 0.7 mg/cm2. From the C rate performance study QSSEBs have shown improved stability with the higher current rates. Next, cathodes with higher sulfur loading were studied and for sulfur loading > 4 mgcm-2, initial discharge capacity >950 mAh/g and 400 mAh/g after 60 cycles at C/20 rate were achieved with 40 μl of IL consisting of LiTFSI (3M) dissolved in PYR:DOL(1:3) for the SSE Li6PS5F0.5Cl2. Further testing is underway to improve the performance at high C rate for higher loading by incorporating SSE in the cathode to realize QSSLSB with higher capacity with improved cycle retention.
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Ma, Shao Wu, Dong Lin Zhao, Ning Na Yao, and Li Xu. "Graphene/Sulfur Nanocomposite for High Performance Lithium-Sulfur Batteries." Advanced Materials Research 936 (June 2014): 369–73. http://dx.doi.org/10.4028/www.scientific.net/amr.936.369.
Повний текст джерелаАнотація:
The graphene/sulfur nanocomposite has been synthesized by heating a mixture of graphene sheets and elemental sulfur. The morphology, structure and electrochemical performance of graphene/sulfur nanocomposite as cathode material for lithium-sulfur batteries were systematically investigated by field-emission scanning electron microscope, X-ray diffraction and a variety of electrochemical testing techniques. The graphene/sulfur nanocomposite cathodes display a high reversible capacity of 800-1200 mAh g-1, and stable cycling for more than 100 deep cycles at 0.1 C. The graphene sheets have good conductivity and an extremely high surface area, and provide a robust electron transport network. The graphene network also accommodates the volume change of the electrode during the Li-S electrochemical reaction.
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Nagai, Erika, Timothy S. Arthur, Patrick Bonnick, Koji Suto, and John Muldoon. "The Discharge Mechanism for Solid-State Lithium-Sulfur Batteries." MRS Advances 4, no. 49 (2019): 2627–34. http://dx.doi.org/10.1557/adv.2019.255.
Повний текст джерелаАнотація:
AbstractThe electrochemical discharge mechanism is reported for all-solid lithium sulfur batteries. Upon milling with carbon fibers, the solid electrolyte used within the cathode composite becomes electrochemically active. Analysis with Raman spectroscopy and XPS revealed the importance of bridging S-S bond formation and breaking in lithium polysulfidophosphates during electrochemical lithiation of the active solid electrolyte. Remarkably, when sulfur is introduced as an active material in the cathode composite, lithium polysulfides are formed as an intermediate product before full lithiation into lithium sulfide. The synthesis of materials based on bridging S-S bonds is an important avenue to the design of new cathodes for all-solid batteries.
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Zhu, Sheng, and Yan Li. "Carbon-metal oxide nanocomposites as lithium-sulfur battery cathodes." Functional Materials Letters 11, no. 06 (December 2018): 1830007. http://dx.doi.org/10.1142/s1793604718300074.
Повний текст джерелаАнотація:
In rechargeable lithium-sulfur (Li-S) batteries, the conductive carbon materials with high surface areas can greatly enhance the electrical conductivity of sulfur cathode, and metal oxides can restrain the dissolution of lithium polysulfides within the electrolyte through strong chemical bindings. The rational design of carbon-metal oxide nanocomposite cathodes has been considered as an effective solution to increase the sulfur utilization and improve cycling performance of Li-S batteries. Here, we summarize the recent progresses in the carbon-metal oxide composites for Li-S battery cathodes. Some insights are also offered on the future directions of carbon-metal oxide hybrid cathodes for high performance Li-S batteries.
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Manjum, Marjanul, Saheed Adewale Lateef, William Earl Mustain, and Golareh Jalilvand. "Cycle-Induced Structural Evolution of Sulfur Cathodes in Lithium-Sulfur Batteries." ECS Meeting Abstracts MA2022-02, no. 2 (October 9, 2022): 136. http://dx.doi.org/10.1149/ma2022-022136mtgabs.
Повний текст джерелаАнотація:
Lithium (Li) ion batteries (LIBs) have been the predominant and fastest growing energy storage technology over the past few decades. A significant amount of LIB research has been carried out and remarkable improvements in the technology have been achieved. As a result, state-of-the-art LIBs offer superior cyclability, high efficiency, and high specific energy relative to competitors [1]. However, the desire for long-range electric vehicles (EVs) and grid-level energy storage and delivery is increasing the demands for batteries with very high gravimetric energy density (e.g. > 500 Wh/kg) [2]. This is simply much higher than what LIB electrode materials can practically offer (~ 260 Wh/kg). Therefore, alternative chemistries are needed at both electrodes. One material that has received significant attention recently as a replacement cathode material in Li-based batteries is sulfur (S). S has 5 times the theoretical specific energy than conventional LIB cathodes and can offer a practical energy density of > 500 Wh/kg when coupled with commercially available lithiated graphite or Li metal anodes [3]. S is also non-toxic, low-cost, and has high natural abundance. These properties make S a promising candidate for next-generation cathodes in Li battery systems. Yet, the path to achieving near theoretical capacity and long cycle life for S cathodes has proven difficult due to numerous unsolved scientific and technical issues including: i) the insulating nature of Sulfur (S8) and its discharged product (Li2S); ii) undesired solubility of the S products in the liquid electrolyte, resulting in the degrading so-called Li polysulfides “shuttling”, and iii) structural change of the S cathode during charge and discharge due to the large volume variation between the fully charged and discharged products [4]. Several approaches have been reported to address these challenges and improve the Li-S battery performance and durability. Despite these efforts, the advances have been mostly limited to a small number of cycles, or the need for complex structures and that would lead to expensive synthesis costs at the manufacturing scale. In fact, it is not truly known if such complex structures are even necessary as the literature lacks a truly systematic investigation into i) the influence of the S structure on its behavior; and ii) how the S structure evolves as a result of charging and discharging the cell. It is also likely that complex structures would not be reformed upon deep charging/discharging – making their possible advantages only temporary. Hence, there are a limited number of truly practical S cathodes that can be rationally developed [3, 4]. In this work, new insights are presented regarding the structural evolution of S cathodes throughout cycling. The structural changes experienced by the S cathodes were investigated by scanning electron microscopy (SEM) during charge and discharge (at C/10) over the lifetime of the cell (10’s to 100’s of cycles) for multiple cells. Cycling was done with Li-S coin cells that were made using a Li metal anode and a S cathode. The S cathode was prepared using commercially available S powder, a through low-cost, simple, and scalable electrode recipe and production techniques. Drastic microstructural and compositional transformations were observed in the S cathodes as a consequence of charging and discharging. Results suggest that there was a reversible swelling transfiguration of the support structure (conductive carbon plus binder) during each discharge and charge step. It was also observed that the location and distribution of S was changed, and new structures were formed. These results are expected to cast light on a fairly unknown area in the Li-S battery technology, which can help with future scale-up and manufacturing of these cells. References [1] G. E. Blomgren, “The development and future of lithium ion batteries,” Journal of The Electrochemical Society, vol. 164, no. 1, p. A5019, 2016. [2] B. Zhu, X. Wang, P. Yao, J. Li, and J. Zhu, “Towards high energy density lithium battery anodes: silicon and lithium,” Chemical science, vol. 10, no. 30, pp. 7132–7148, 2019. [3] Z. Lin and C. Liang, “Lithium–sulfur batteries: from liquid to solid cells,” Journal of Materials Chemistry A, vol. 3, no. 3, pp. 936–958, 2015. [4] ZW. She, Y. Sun, Q. Zhang, and Y. Cui. “Designing high-energy lithium–sulfur batteries” Chemical society reviews, vol. 45, no. 20, pp. 5605-5634, 2016.
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Shi, Changmin, Saya Takeuchi, Joseph Dura, and Eric Wachsman. "(Digital Presentation) High Energy Density Stable Lithium-Sulfur Batteries Enabled By 3D Bilayer Garnet Electrolytes." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2614. http://dx.doi.org/10.1149/ma2022-0272614mtgabs.
Повний текст джерелаАнотація:
The cubic-garnet (Li7La3Zr2O12, LLZO) Lithium-Sulfur battery (GLSB) shows great promise in the pursuit of achieving high energy densities. The sulfur used in the cathodes are abundant and inexpensive and possess high specific capacity. As well, LLZO displays excellent chemical stability with Li metal. By using unique porous/dense/porous LLZO “trilayer” and dense/porous LLZO “bilayer” architectures developed by our group, an exceptionally high areal current density of 10 mA/cm2 in Li-Li symmetric cells without applied pressure was achieved. However, instability in the sulfur cathode/LLZO interface can cause cell performance issues. Therefore, it is critical to resolve the sulfur cathode/LLZO interfacial challenge to achieve stable cycling. Here, we created an innovative gel polymer (GPE) buffer layer to stabilize the sulfur cathode/LLZO interface. With a thin bilayer LLZO architecture as a solid electrolyte, stable cycling was achieved with a high initial discharge capacity of 1542 mAh/g corresponding to an energy density of 223 Wh/kg and 769 Wh/L under a discharge current density of 0.87 mA/cm2 without applied pressure. Moreover, the addition of the GPE interlayer also allowed the GLSB cells to maintain an average discharge capacity of 1218 mAh/g over 265 cycles with 80% capacity retention at discharge current density of 1.74 mA/cm2 under a sulfur loading of 5.2 mg/cm2 at 22 (Figure 1). Achieving such stability is a major step in the development of commercial garnet lithium sulfur batteries. Figure 1
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Kuroda, Masato, Morihiko Okuno, Daisuke Okuda, and Masashi Ishikawa. "Improvement of Sulfur Cathode Reversibility by Specific Chemical Lithium Pre-doping Method." ECS Meeting Abstracts MA2022-02, no. 64 (October 9, 2022): 2312. http://dx.doi.org/10.1149/ma2022-02642312mtgabs.
Повний текст джерелаАнотація:
1.Intoroduction Recently, lithium-ion batteries (LIBs) have been required in terms of a high energy density for large-scale applications such as power supplies for electric vehicles. Lithium-sulfur (Li-S) batteries are, therefore, expected as next generation batteries because of their high energy density. Sulfur is utilized as cathode material for Li-S batteries because of a high specific capacity. However, sulfur has a low electric conductivity and a risk of dissolution into an electrolyte during a charge-discharge process [1]. L. Nazar et al. applied activated carbon as substrate for sulfur to help electric conduction and prevent dissolution of sulfur [2]. The activated carbon allows Li-S batteries to show high specific capacity with high reversibility. Even if these problems are solved, however, Li-S batteries have a further problem of excessive initial irreversible capacity during the first discharge process. Li pre-doping is a useful technique to cancel the large irreversible capacity in actual LIBs. Abe et al. reported a chemical lithium pre-doping method for a graphite using lithium naphthalenide [3]. Studies have been reported on the use of such pre-doping to improve the performance of Li-S batteries, for instance, with a sulfur-Ketjenblack composite cathode [4]. In our previous study, we have applied that method to a sulfur cathode composed of microporous activated carbon and sulfur before cell assembly and developed a Li2S cathode that suppressed the initial irreversible capacity during the first discharge process. However, the Li2S cathode showed an unignorable initial irreversible capacity and poor cycle life [5]. This work attempts to improve the reversible capacity of the Li2S cathode by a specialized chemical lithium pre-doping method. Our report would lead to the proposal of novel cathode and anode options in Li-S batteries. Method 2-1. Fabrication of lithium naphthalenide solution As Li metal and Li2S are both sensitive to moisture in air, all the following synthesis processes were carried out in an Ar-filled glove box. Lithium naphthalenide, a dark green solution was prepared by mixing an equal mol amount of Li metal with naphthalene in a cyclic ether solvent. 2-2. Fabrication of Li2S-AC cathodes Each sulfur cathode was prepared by mixing the S-AC (a composite of microporous activated carbon and sulfur), acetylene black, carboxymethyl cellulose, and styrene butadiene rubber at a respective weight ratio of 93: 3: 2: 2 and coating the resulting aqueous slurry on a carbon paper. The 1M lithium naphthalenide solution was dropped on the sulfur cathode. After 20 min reaction, the cathode was rinsed several times with 2–dimethoxyethane (DME) to remove the residues of reagents. The cathode was then dried under reduced pressure for 12 h. After that, the resulting Li2S cathode was impregnated with a mixture of vinylene carbonate (VC) and fluoroethylene carbonate (FEC) (VC: FEC = 1: 1 by weight). After 20 min impregnation, the cathode was dried under reduced pressure for 12 h. 2-3. Assembling of cells Cells were assembled with the Li2S electrode and Li metal foil as an anode. Lithium bis(trifluorosulfonyl)imide (LiTFSI): tetraglyme (G4): 1,1,2,2–tetrafluoroethyl–2,2,3,3–tetrafluoropropyl ether (D2) at a respective ratio of 10: 8: 40 (by mol) was used as the electrolyte. 3.Major results and discussion The Li2S cathode without the VC/FEC impregnation showed an initial charge capacity of 1791 mAh g-1 and an initial discharge capacity of 1298 mAh g-1, indicating a large irreversible capacity. In contrast, the Li2S cathode with the VC/FEC impregnation showed 1446 mAh g-1 and 1422 mAh g-1, respectively. Thus, the impregnation with VC/FEC reduced the initial irreversible capacity and improved the initial charge capacity. According to these results, Li remaining in the sulfur cathode would be partially consumed to form a film by the impregnation with VC/FEC. In addition, the capacity retention of the Li2S cathode with and without the VC/FEC impregnation was 73 % and 64 % at the 30th cycle, respectively. This suggests that the Li2S cathode with the film leads to better cycle performance than that without the film. We will also report the results of surface composition analysis of the Li2S cathode with and without the VC/FEC impregnation by Hard X-ray Photoelectron Spectroscopy (HAXPES). References [1] M. Wild et al., Energy & Environ. Sci., 8 (2015) 3477. [2] X. Ji et al., Nat. Mater., 8 (2009) 500. [3] T. Abe et al., J. Power Sources, 68 (1997) 216. [4] Y. Wu et al., J. Power Sources, 366 (2017) 65. [5] M. Okuno et al., The 60th Battery Symposium in Japan (2019) Abstract [3D01].
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Yan, Yinglin, Jiaming Lin, Shiyu Chen, Shaoxiong Zhang, Rong Yang, Yunhua Xu, and Tong Han. "Investigation on the Electrochemical Properties of Antimony Tin Oxide Nanoparticle-Modified Graphene Aerogel as Cathode Matrix in Lithium–Sulfur Battery." Journal of Nanoscience and Nanotechnology 20, no. 11 (November 1, 2020): 7027–33. http://dx.doi.org/10.1166/jnn.2020.18825.
Повний текст джерелаАнотація:
Lithium-sulfur (Li–S) batteries are considered the most appealing secondary batteries attributed to the ultrahigh theoretical specific capacity as 1675 mA·h·g−1 for elemental sulfur cathode. Nevertheless, there are still several disadvantages (sulfur insulation, insoluble lithium polysulfide, shuttle effect, etc.) impeding the commercial application of Li–S batteries. Recent studies have discovered that nanosized metal oxides can effectively modify the electrochemical properties of composite cathodes in Li–S batteries. In this paper, graphene aerogels (GA) loaded with different mass fractions of antimony tin oxide (ATO) nanoparticles were incorporated with sulfur and utilized as cathode materials for Li–S batteries. The sample (GA/ATO-3) loaded with 3 wt.% ATO nanoparticles showed the best electrochemical performance. For example, the specific discharge capacity of first cycle reached 1210 mA·h·g−1 under a current of 0.1 C. The reversible discharge capacity was reduced to 545 mA·h·g−1 after 50 cycles, namely, the corresponding capacity retention rate was approximately 50%. However, the coulombic efficiency was still near 100%. Potential modification mechanism was considered to be a combination between the GA with excellent conductivity, which effectively improved the internal conductivity of the cathode material, and the ATO nanoparticles, which improved the distribution uniformity of the solid sulfur and its sulfurized product because the ATO nanoparticles acted as heterogeneous nucleation points. Furthermore, the ATO nanoparticles with strong polarity possessed a strong capture ability on the soluble polysulfide ions. For the above reasons, the ATO-loaded GA cathode could effectively inhibit the “shuttle effect,” thereby, improved the electrochemical performance of Li–S batteries.
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Xu, Yong Gang, Xiang Yu Yan, Jing Xiang, Han Wen Ou, and Wen Yao Yang. "Characterization of Sulfur/Graphitized Mesocarbon Microbeads Composite Cathodes for Li-S Batteries." Advanced Engineering Forum 44 (January 17, 2022): 87–94. http://dx.doi.org/10.4028/www.scientific.net/aef.44.87.
Повний текст джерелаАнотація:
Cathode optimization is vital for improving the performance of Li-S batteries. Various carbon materials with special morphologies have been proposed and verified to form optimized sulfur/carbon (S/C) cathodes owning high cycling and rate performances. However, the high cost and complexity of material preparation processes hinder their commercialization. Herein, graphitized mesocarbon microbeads (g-MCMB) were used to form sulfur/carbon cathodes for Li-S battery. By simply dry-mixing sulfur powder with g-MCMB, S/g-MCMB cathodes were formed and characterized by galvanostatic charge-discharge tests, electrochemical impedance spectroscopy and scanning electron microscopy. Compared with S/C cathodes using acetylene black, S/g-MCMB cathodes show better cycling performance, but worse rate performance, which can be attributed to the size and morphologies of g-MCMB particles.
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Mukkabla, Radha, and Michael R. Buchmeiser. "Cathode materials for lithium–sulfur batteries based on sulfur covalently bound to a polymeric backbone." Journal of Materials Chemistry A 8, no. 11 (2020): 5379–94. http://dx.doi.org/10.1039/c9ta12619h.
Повний текст джерелаАнотація:
Polymeric cathode materials for lithium–sulfur batteries in which the sulfur is covalently bound to the polymer are summarized; differences in electrochemical performance to cathode materials in which the sulfur is physically confined are outlined.
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Jeong, Sang Sik, Young Jin Choi, and Ki Won Kim. "Effects of Multiwalled Carbon Nanotubes on the Cycle Performance of Sulfur Electrode for Li/S Secondary Battery." Materials Science Forum 510-511 (March 2006): 1106–9. http://dx.doi.org/10.4028/www.scientific.net/msf.510-511.1106.
Повний текст джерелаАнотація:
Lithium sulfur cells were prepared by composing with sulfur cathode, 0.5M LiCF3SO3 in tetra ethylene glycol dimethyl ether (TEGDME) solution and lithium anode. Multiwalled carbon nanotubes (MWNTs) were used to form the high electric network and prevent the dissolution of lithium polysulfides in sulfur cathode. The effects of additive contents were investigated by discharge test. The morphology of cathode with MWNTs (20wt.%) has rough and submicro porous. The initial discharge capacity of lithium sulfur cell using multiwalled carbon nanotubes (MWNTs) was 1,200mAh/g-sulfur, which was better than those of acetylene black (AB). The cycle performance of lithium sulfur cell was remarkably improved by the the addition of MWNTs.
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Hu, Xianfei, Kaitong Leng, Cuijuan Zhang, and Jiayan Luo. "Crumpled graphene-encapsulated sulfur for lithium–sulfur batteries." RSC Advances 8, no. 33 (2018): 18502–7. http://dx.doi.org/10.1039/c8ra03255f.
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Pang, Zhiyuan, Linglong Kong, Hongzhou Zhang, Bin Deng, Dawei Song, Xixi Shi, Yue Ma, and Lianqi Zhang. "The Optimization of a Carbon Paper/MnO2 Composite Current Collector for Manufacturing a High-Performance Li–S Battery Cathode." Crystals 12, no. 11 (November 9, 2022): 1596. http://dx.doi.org/10.3390/cryst12111596.
Повний текст джерелаАнотація:
High theoretical energy density endows lithium–sulfur batteries to be a promising candidate of the secondary batteries. Numerous studies have been implemented relying on exploring efficient host materials or separator modifying layers to solve the problematic shuttling and insufficient conversion of soluble polysulfides, whereas few studies have focused on the modification of the cathode collector. Herein, a high-performance sulfur cathode is manufactured with carbon paper/MnO2 as the cathode collector and liquid lithium polysulfides as the electrode material. The interface of carbon paper/MnO2 is proposed to afford fast electronic transport, strong chemical adsorption, and effective electrocatalysis to confine the diffusion of lithium polysulfides and facilitate their conversion during the charge/discharge process. More importantly, with no conductive additives and binders assisting, the gravimetric energy density of the sulfur cathode could be largely improved. Specifically, lithium–sulfur batteries using carbon paper/MnO2 as a cathode collector could stably circulate for 200 cycles at 0.2 C with a capacity of 664 mAh g−1, which is higher than that of carbon paper as a cathode collector (486 mAh g−1). This work may provide a new perspective to enhance the electrochemical performance of lithium–sulfur batteries by optimizing the cathode collector.
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Park, Jong Won, Hyean-Yeol Park, Jukyoung Kang, Seok Kim, and Yongju Jung. "Carbon Nanotube-Based Sulfur Cathode with a Mesoporous Carbon-Silica Composite for Long Cycle Life Li–S Batteries." Journal of Nanoscience and Nanotechnology 20, no. 8 (August 1, 2020): 4949–54. http://dx.doi.org/10.1166/jnn.2020.17851.
Повний текст джерелаАнотація:
The use of carbon nanotube (CNT) films as a sulfur host is a promising approach to improve the sulfur loading and energy density of Li–S batteries. However, the inability to durably incorporate polysulfides within the cathode structure results in a limited cycle life. Herein, we propose a CNTbased sulfur cathode with carbon-coated ordered mesoporous silica (c-OMS) to overcome the cycle performance issue. Scanning electron microscopy and X-ray diffraction studies on the c-OMS prepared in this work revealed that the wall surface of OMS was evenly coated with an extremely thin carbon layer. The sulfur-CNT cathode with c-OMS retained a remarkably improved capacity (942 mAh g−1) with excellent cycling stability (91%) after 100 cycles as well as significantly high sulfur utilization in the first cycle compared with the sulfur-CNT cathode with OMS. This result may stem from the surface property of c-OMS with high chemical affinity towards electrolyte solvents.
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Gao, Xiaosi, Changyang Zheng, Yiqi Shao, Shuo Jin, Jin Suntivich, and Yong Lak Joo. "Lithium Iron Phosphate Reconstruction Facilitates Kinetics in High-Areal-Capacity Sulfur Composite Cathodes." ECS Meeting Abstracts MA2022-01, no. 1 (July 7, 2022): 35. http://dx.doi.org/10.1149/ma2022-01135mtgabs.
Повний текст джерелаАнотація:
Lithium-sulfur (Li-S) batteries have been recognized as one of the most promising choices beyond lithium-ion batteries (LIB), because of its low cost and high theoretical specific energy (~2510 Wh/kg or ~10 times of LIB). However, Li-S batteries still face a few challenges, including large volume expansion, poor conductivity, low active material loading, inert end products, and polysulfide crossover called the “shuttle effect”, etc. To address these challenges, we have incorporated lithium iron phosphate (LFP) into our sulfur composite cathode. The addition of LFP enabled a more uniform slurry rheology, which allowed mass loading to double the amount of typical sulfur cathodes. Meanwhile, LFP can effectively adsorb polysulfides, which restricted the shuttle effects common in high-sulfur-loading batteries. Our LFP-hybrid Li-S batteries showed high areal capacity for 300 cycles under both low- and high-current charge-discharge cycles. More importantly, our characterizations demonstrated that LFP in Li-S batteries can reconstruct into Fe2P during cycling. We propose that Fe2P is an effective electrocatalyst for anchoring polysulfides. To unveil the role of Fe2P, we have directly incorporated these materials into the sulfur composite cathode. Using a hydrothermal synthesis, we showed that Fe2P nanoparticles can be directly anchored on the sulfur-carbon composite. This approach caused minimal phase separation and enabled a uniform morphology. We presented the analysis of the cathodes by scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and thermogravimetric analysis (TGA). These results allow us to develop a mechanistic hypothesis and a comparison between Fe2P and LFP in terms of the electrochemical performances.
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Gerle, Martina, Norbert Wagner, Joachim Häcker, Maryam Nojabaee, and Kasper Andreas Friedrich. "Identification of the Underlying Processes in Impedance Response of Sulfur/Carbon Composite Cathodes at Different SOC." Journal of The Electrochemical Society 169, no. 3 (March 1, 2022): 030505. http://dx.doi.org/10.1149/1945-7111/ac56a4.
Повний текст джерелаАнотація:
For lithium-sulfur batteries, porous carbon/sulfur composite cathodes are the primary solution to compensate the non-conductive nature of sulfur. The composition and structure of this class of cathodes are crucial to the electrochemical performance, achieved energy density and the stability of the cell. Electrochemical impedance spectroscopy is employed to investigate and correlate the electrochemical performance of lithium-sulfur batteries to the composition and microstructure of differently fabricated carbon/sulfur composite cathodes. A transmission line model is applied to identify different underlying electrochemical processes appearing in the impedance response of a range of porous carbon/sulfur cathodes. The integration of a lithium ring serving as a counter electrode coupled with advanced wiring has allowed an artifact-free recording of the cathode impedance at different states of charge with the aim to investigate the evolution of impedance during discharge/charge and the kinetics of charge transfer depending on the infiltration method and the utilized carbon host. It is shown that impedance response of this class of cathodes is highly diverse and the plausible underlying processes are discussed in details. To this end, quasi-solid-state and various polysulfide-based charge transfer mechanisms are identified and their time constants are reported.
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Chen, Shu-Yu, and Sheng-Heng Chung. "Advanced Current Collectors with Carbon Nanofoams for Electrochemically Stable Lithium—Sulfur Cells." Nanomaterials 11, no. 8 (August 17, 2021): 2083. http://dx.doi.org/10.3390/nano11082083.
Повний текст джерелаАнотація:
An inexpensive sulfur cathode with the highest possible charge storage capacity is attractive for the design of lithium-ion batteries with a high energy density and low cost. To promote existing lithium–sulfur battery technologies in the current energy storage market, it is critical to increase the electrochemical stability of the conversion-type sulfur cathode. Here, we present the adoption of a carbon nanofoam as an advanced current collector for the lithium–sulfur battery cathode. The carbon nanofoam has a conductive and tortuous network, which improves the conductivity of the sulfur cathode and reduces the loss of active material. The carbon nanofoam cathode thus enables the development of a high-loading sulfur cathode (4.8 mg cm−2) with a high discharge capacity that approaches 500 mA·h g−1 at the C/10 rate and an excellent cycle stability that achieves 90% capacity retention over 100 cycles. After adopting such an optimal cathode configuration, we superficially coat the carbon nanofoam with graphene and molybdenum disulfide (MoS2) to amplify the fast charge transfer and strong polysulfide-trapping capabilities, respectively. The highest charge storage capacity realized by the graphene-coated carbon nanofoam is 672 mA·h g−1 at the C/10 rate. The MoS2-coated carbon nanofoam features high electrochemical utilization attaining the high discharge capacity of 633 mA·h g−1 at the C/10 rate and stable cyclability featuring a capacity retention approaching 90%.
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Zukalová, Markéta, Monika Vinarčíková, Milan Bouša, and Ladislav Kavan. "Nanocrystalline TiO2/Carbon/Sulfur Composite Cathodes for Lithium–Sulfur Battery." Nanomaterials 11, no. 2 (February 20, 2021): 541. http://dx.doi.org/10.3390/nano11020541.
Повний текст джерелаАнотація:
This paper evaluates the influence of the morphology, surface area, and surface modification of carbonaceous additives on the performance of the corresponding cathode in a lithium–sulfur battery. The structure of sulfur composite cathodes with mesoporous carbon, activated carbon, and electrochemical carbon is studied by X-ray diffraction, nitrogen adsorption measurements, and Raman spectroscopy. The sulfur cathode containing electrochemical carbon with the specific surface area of 1606.6 m2 g−1 exhibits the best electrochemical performance and provides a charge capacity of almost 650 mAh g−1 in cyclic voltammetry at a 0.1 mV s−1 scan rate and up to 1300 mAh g−1 in galvanostatic chronopotentiometry at a 0.1 C rate. This excellent electrochemical behavior is ascribed to the high dispersity of electrochemical carbon, enabling a perfect encapsulation of sulfur. The surface modification of carbonaceous additives by TiO2 has a positive effect on the electrochemical performance of sulfur composites with mesoporous and activated carbons, but it causes a loss of dispersity and a consequent decrease of the charge capacity of the sulfur composite with electrochemical carbon. The composite of sulfur with TiO2-modified activated carbon exhibited the charge capacity of 393 mAh g−1 in cyclic voltammetry and up to 493 mAh g−1 in galvanostatic chronopotentiometry. The presence of an additional Sigracell carbon felt interlayer further improves the electrochemical performance of cells with activated carbon, electrochemical carbon, and nanocrystalline TiO2-modified activated carbon. This positive effect is most pronounced in the case of activated carbon modified by nanocrystalline TiO2. However, it is not boosted by additional coverage by TiO2 or SnO2, which is probably due to the blocking of pores.
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Cheng, J. J., Y. Pan, J. A. Pan, H. J. Song, and Z. S. Ma. "Sulfur/bamboo charcoal composites cathode for lithium–sulfur batteries." RSC Advances 5, no. 1 (2015): 68–74. http://dx.doi.org/10.1039/c4ra12509f.
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Wang, Fan, Xinqi Liang, Minghua Chen, and Xinhui Xia. "Synthesis of carbon nanoflake/sulfur arrays as cathode materials of lithium-sulfur batteries." Functional Materials Letters 11, no. 06 (December 2018): 1840001. http://dx.doi.org/10.1142/s1793604718400015.
Повний текст джерелаАнотація:
It is of great importance to develop high-quality carbon/sulfur cathode for lithium-sulfur batteries (LSBs). Herein, we report a facile strategy to embed sulfur into interconnected carbon nanoflake matrix forming integrated electrode. Interlinked carbon nanoflakes have dual roles not only as a highly conductive matrix to host sulfur, but also act as blocking barriers to suppress the shuttle effect of intermediate polysulfides. In the light of these positive characteristics, the obtained carbon nanoflake/S cathode exhibit good LSBs performances with high capacities (1117[Formula: see text]mAh[Formula: see text]g[Formula: see text] at 0.2[Formula: see text]C, and 741[Formula: see text]mAh[Formula: see text]g[Formula: see text] at 0.6[Formula: see text]C) and good high-rate cycling performance. Our synthetic method provides a novel way to construct enhanced carbon/sulfur cathode for LSBs.
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Weng, Wei, Shengwen Yuan, Nasim Azimi, Zhang Jiang, Yuzi Liu, Yang Ren, Ali Abouimrane, and Zhengcheng Zhang. "Improved cyclability of a lithium–sulfur battery using POP–Sulfur composite materials." RSC Adv. 4, no. 52 (2014): 27518–21. http://dx.doi.org/10.1039/c4ra02589j.
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Pandey, Gaind P., Kobi Jones, and Lamartine Meda. "CNFs/S1-xSex Composites as Promising Cathode Materials for High-Energy Lithium-Sulfur Batteries." MRS Advances 4, no. 14 (2019): 821–28. http://dx.doi.org/10.1557/adv.2019.144.
Повний текст джерелаАнотація:
ABSTRACTHigh-energy lithium-sulfur (Li-S) batteries still suffer from poor rate capability and short cycle life caused by the polysulfides shuttle and insulating nature of S (and the discharge product, Li2S). Selenium disulfide (SeS2), with a theoretical specific capacity of 1342 mAh g−1, is a promising cathode material as it has better conductivity compared to sulfur. The electrochemical reaction kinetics of CNFs-S/SeS2 composites (denoted as CNFs/S1-xSex, where x ≤ 0.1) are expected to be remarkably improved because of the better conductivity of SeS2 compared to sulfur. Here, a high-performance composite cathode material of CNFs/S1-xSex for novel Li-S batteries is reported. The CNFs/S1-xSex composites combine the higher conductivity and higher density of SeS2 with high specific capacity of sulfur. The CNFs/S1-xSex electrode shows good initial discharge capacity of ∼1050 mAh g−1 at 0.05 C rate with high mass loading of materials (∼6-7 mg cm−2 of composites) and > 97% initial coulombic efficiency. The CNFs/S1-xSex electrode shows more than 600 mAh g-1 specific capacity after 50 charge-discharge cycles at 0.5C rate, much higher compared to the CNFs/S cathodes.
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Tripathi, Balram, Rajesh K. Katiyar, Gerardo Morell, Ambesh Dixit, and Ram S. Katiyar. "BiFeO3 Coupled Polysulfide Trapping in C/S Composite Cathode Material for Li-S Batteries as Large Efficiency and High Rate Performance." Energies 14, no. 24 (December 11, 2021): 8362. http://dx.doi.org/10.3390/en14248362.
Повний текст джерелаАнотація:
We demonstrated the efficient coupling of BiFeO3 (BFO) ferroelectric material within the carbon–sulfur (C-S) composite cathode, where polysulfides are trapped in BFO mesh, reducing the polysulfide shuttle impact, and thus resulting in an improved cyclic performance and an increase in capacity in Li-S batteries. Here, the built-in internal field due to BFO enhances polysulfide trapping. The observation of a difference in the diffusion behavior of polysulfides in BFO-coupled composites suggests more efficient trapping in BFO-modified C-S electrodes compared to pristine C-S composite cathodes. The X-ray diffraction results of BFO–C-S composite cathodes show an orthorhombic structure, while Raman spectra substantiate efficient coupling of BFO in C-S composites, in agreement with SEM images, showing the interconnected network of submicron-size sulfur composites. Two plateaus were observed at 1.75 V and 2.1 V in the charge/discharge characteristics of BFO–C-S composite cathodes. The observed capacity of ~1600 mAh g−1 in a 1.5–2.5 V operating window for BFO30-C10-S60 composite cathodes, and the high cyclic stability substantiate the superior performance of the designed cathode materials due to the efficient reduction in the polysulfide shuttle effect in these composite cathodes.
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Wang, Jing, Riwei Xu, Chengzhong Wang, and Jinping Xiong. "Lamellar Polypyrene Based on Attapulgite–Sulfur Composite for Lithium–Sulfur Battery." Membranes 11, no. 7 (June 29, 2021): 483. http://dx.doi.org/10.3390/membranes11070483.
Повний текст джерелаАнотація:
We report on the preparation and characterization of a novel lamellar polypyrrole using an attapulgite–sulfur composite as a hard template. Pretreated attapulgite was utilized as the carrier of elemental sulfur and the attapulgite–sulfur–polypyrrole (AT @400 °C–S–PPy) composite with 50 wt.% sulfur was obtained. The structure and morphology of the composite were characterized with infrared spectroscopy (IR), thermogravimetric analysis (TGA), and scanning electron microscopy (SEM). An AT @400 °C–S–PPy composite was further utilized as the cathode material for lithium–sulfur batteries. The first discharge specific capacity of this kind of battery reached 1175 mAh/g at a 0.1 C current rate and remained at 518 mAh/g after 100 cycles with capacity retention close to 44%. In the rate test, compared with the polypyrrole–sulfur (PPy–S) cathode material, the AT @400 °C–S–PPy cathode material showed lower capacity at a high current density, but it showed higher capacity when the current came back to a low current density, which was attributed to the “recycling” of pores and channels of attapulgite. Therefore, the lamellar composite with special pore structure has great value in improving the performance of lithium–sulfur batteries.
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Chen, Liang, Zhongxue Chen, Zheng Huang, Yingfei Wang, Haihui Zhou, and Yafei Kuang. "A nitrogen-doped unzipped carbon nanotube/sulfur composite as an advanced cathode for lithium–sulfur batteries." New Journal of Chemistry 39, no. 11 (2015): 8901–7. http://dx.doi.org/10.1039/c5nj01803j.
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Liu, Run Ru, De Jun Wang, and Leng Jing. "Effect of SO2 on the Performance of LSCF Cathode." Advanced Materials Research 902 (February 2014): 41–44. http://dx.doi.org/10.4028/www.scientific.net/amr.902.41.
Повний текст джерелаАнотація:
Sulfur poisoning effect on the electrochemical performance and long-term durability of SOFC cathode has been investigated for La0.6Sr0.4Co0.2Fe0.8O3(LSCF) by Galvanic Current Interruption (GCI) technology. Cell performance was measured supplying with SO2-containing air to the cathode under a constant current density of 200 mA cm-2. At 800 °C, LSCF cathode showed low tolerance to the sulfur poisoning. SO2tends to react with strontium in LSCF material resulting in the formation of SrSO4in the cathode. This reaction gave rise to microstructural change in the cathode and caused gradual degradation of cell performance.
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Lasetta, Kyriakos, Joseph Paul Baboo, and Constantina Lekakou. "Modeling and Simulations of the Sulfur Infiltration in Activated Carbon Fabrics during Composite Cathode Fabrication for Lithium-Sulfur Batteries." Journal of Composites Science 5, no. 3 (February 25, 2021): 65. http://dx.doi.org/10.3390/jcs5030065.
Повний текст джерелаАнотація:
During the manufacture of a composite cathode for lithium-sulfur (Li-S) batteries it is important to realize homogeneous infiltration of a specified amount of sulfur, targeted to be at least 5 mg cm−2 to achieve good battery performance in terms of high energy density. A model of the sulfur infiltration is presented in this study, taking into account the pore size distribution of the porous cathode host, phase transitions in sulfur, and formation of different sulfur allotropes, depending on pore size, formation energy and available thermal energy. Simulations of sulfur infiltration into an activated carbon fabric at a hot-plate temperature of 175 °C for two hours predicted a composite cathode with 41 wt% sulfur (8.3 mg cm−2), in excellent agreement with the experiment. The pore size distribution of the porous carbon host proved critical for both the extent and form of retained sulfur, where pores below 0.4 nm could not accommodate any sulfur, pores between 0.4 and 0.7 nm retained S4 and S6 allotropes, and pores between 0.7 and 1.5 nm contained S8.
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Gong, Zhijie, Qixing Wu, Fang Wang, Xu Li, Xianping Fan, Hui Yang, and Zhongkuan Luo. "PEDOT-PSS coated sulfur/carbon composite on porous carbon papers for high sulfur loading lithium–sulfur batteries." RSC Advances 5, no. 117 (2015): 96862–69. http://dx.doi.org/10.1039/c5ra18567j.
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Zhang, Yuxuan, Thomas Kivevele, Han Wook Song, and Sunghwan Lee. "(Digital Presentation) Accelerating the Conversion Process of Polysulfides in High Mass Loading Sulfur Cathode for the Longevity Li-S Battery." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 383. http://dx.doi.org/10.1149/ma2022-012383mtgabs.
Повний текст джерелаАнотація:
Conventional lithium-ion batteries are unable to meet the increasing demands for high-energy storage systems, because of their limited theoretical capacity.1 In recent years, intensive attention has been paid to enhancing battery energy storage capability to satisfy the increasing energy demand in modern society and reduce the average energy capacity cost. Among the candidates for next generation high energy storage systems, the lithium sulfur battery is especially attractive because of its high theoretical specific energy (around 2600 W h kg-1) and potential cost reduction. In addition, sulfur is a cost effective and environmentally friendly material due to its abundance and low-toxicity. 2 Despite all of these advantages, the practical application of lithium sulfur batteries to date has been hindered by a series of obstacles, including low active material loading, poor cycle life, and sluggish sulfur conversion kinetics.3 Achieving high mass loading cathode in the traditional 2D planar thick electrode has been challenged. The high distorsion of the traditional planar thick electrodes for ion/electron transfer leads to the limited utilization of active materials and high resistance, which eventually results in restricted energy density and accelerated electrode failure.4 Furthermore, of the electrolyte to pores in the cathode and utilization ratio of active materials. Catalysts such as MnO2 and Co dopants were employed to accelerate the sulfur conversion reaction during the charge and discharge process.5 However, catalysts based on transition metals suffer from poor electronic conductivity. Other catalysts such as transition metal dopants are also limited due to the increased process complexities. . In addition, the severe shuttle effects in Li-S batteries may lead to fast failures of the battery. Constructing a protection layer on the separator for limiting the transmission of soluble polysulfides is considered an effective way to eliminate the shuttle phenomenon. However, the soluble sulfides still can largely dissolve around the cathode side causing the sluggish reaction condition for sulfur conversion.5 To mitigate the issues above, herein we demonstrate a novel sulfur electrode design strategy enabled by additive manufacturing and oxidative vapor deposition (oCVD). Specifically, the electrode is strategically designed into a hierarchal hollow structure via stereolithography technique to increase sulfur usage. The active material concentration loaded to the battery cathode is controlled precisely during 3D printing by adjusting the number of printed layers. Owing to its freedom in geometry and structure, the suggested design is expected to improve the Li ions and electron transport rate considerably, and hence, the battery power density. The printed cathode is sintered at 700 °C at N2 atmosphere to achieve carbonization of the cathode during which intrinsic carbon defects (e.g., pentagon carbon) as catalytic defect sites are in-situ generated on the cathode. The intrinsic carbon defects equipped with adequate electronic conductivity. The sintered 3D cathode is then transferred to the oCVD chamber for depositing a thin PEDOT layer as a protection layer to restrict dissolutions of sulfur compounds in the cathode. Density functional theory calculation reveals the electronic state variance between the structures with and without defects, the structure with defects demonstrates the higher kinetic condition for sulfur conversion. To further identify the favorable reaction dynamic process, the in-situ XRD is used to characterize the transformation between soluble and insoluble polysulfides, which is the main barrier in the charge and discharge process of Li-S batteries. The results show the oCVD coated 3D printed sulfur cathode exhibits a much higher kinetic process for sulfur conversion, which benefits from the highly tailored hierarchal hollow structure and the defects engineering on the cathode. Further, the oCVD coated 3D printed sulfur cathode also demonstrates higher stability during long cycling enabled by the oCVD PEDOT protection layer, which is verified by an absorption energy calculation of polysulfides at PEDOT. Such modeling and analysis help to elucidate the fundamental mechanisms that govern cathode performance and degradation in Li-S batteries. The current study also provides design strategies for the sulfur cathode as well as selection approaches to novel battery systems. References: Bhargav, A., (2020). Lithium-Sulfur Batteries: Attaining the Critical Metrics. Joule 4, 285-291. Chung, S.-H., (2018). Progress on the Critical Parameters for Lithium–Sulfur Batteries to be Practically Viable. Advanced Functional Materials 28, 1801188. Peng, H.-J.,(2017). Review on High-Loading and High-Energy Lithium–Sulfur Batteries. Advanced Energy Materials 7, 1700260. Chu, T., (2021). 3D printing‐enabled advanced electrode architecture design. Carbon Energy 3, 424-439. Shi, Z., (2021). Defect Engineering for Expediting Li–S Chemistry: Strategies, Mechanisms, and Perspectives. Advanced Energy Materials 11. Figure 1
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Pai, Rahul, Varun Natu, Maxim Sokol, Michael Carey, Michel W. Barsoum, and Vibha Kalra. "Surface Functionalization of Two-Dimensional MXene Nanosheets to Tailor Sulfur-Host Architecture for Metal-Sulfur Batteries." ECS Meeting Abstracts MA2022-01, no. 1 (July 7, 2022): 37. http://dx.doi.org/10.1149/ma2022-01137mtgabs.
Повний текст джерелаАнотація:
Practicality of lithium-sulfur batteries is severely hindered by the notorious polysulfide-shuttle phenomenon, leading to rapid capacity fade. This issue is aggravated with increase in sulfur loading, causing low-coulombic efficiency and cycle life. Herein, we present a facile strategy to combine hydrophobic sulfur and hydrophilic, conductive Ti3C2Tz-MXene via one-step surface functionalization using di(hydrogenated tallow) benzylmethyl ammonium chloride (DHT). The latter renders the Ti3C2Tz surface hydrophobic, making it readily dispersible in sulfur dissolved in a carbon disulfide (CS2) solvent. By evaporating the solvent, we conformally coat the DHT-Ti3C2Tz (DMX) with sulfur. The developed composite, with higher available active area, enables effective trapping of lithium polysulfides (LiPs) on the electroactive sites within the cathode, leading to improvement in electrochemical performance at higher sulfur loadings. The DMX/S cathodes function with high sulfur loading of ∼10.7 mg·cm−2 and deliver a stable areal capacity of ∼7 mAh·cm−2 for 150 cycles in the standard ether electrolyte. Moreover, a DMX/S cathode in a pouch-cell configuration retains ∼770 mAh·g−1 after ∼200 cycles at 0.2C (85.5% retention). Postmortem spectroscopic studies elucidate the nature of the LiPs-MXene interaction and the effect of surface functionalization towards improved performance. To further demonstrate the applicability of such uniquely functionalized MXene sheets, we study them as a host to confine sulfur (S8) triggering a quasi-solid state redox mechanism enabling the use of commercialization-friendly carbonate electrolyte in metal-sulfur batteries. We demonstrate that the multilayer MXene structure provides tunable spacing for S8 confinement and its unique interlayer spacing prevents adverse polysulfide-carbonate reactions resulting in stable battery cycling.
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Zukalova, Marketa, Monika Vinarcikova, Barbora Pitna Laskova, and Ladislav Kavan. "The TiO2-Modified Separator Improving the Electrochemical Performance of Lithium-Sulfur Battery." ECS Transactions 105, no. 1 (November 30, 2021): 183–89. http://dx.doi.org/10.1149/10501.0183ecst.
Повний текст джерелаАнотація:
Electrochemical performance of activated carbon/sulfur composite cathode in the Li-S cell with standard and TiO2-modified separator is evaluated by cyclic voltammetry and galvanostatic chronopotentiometry. The modification of the separator by TiO2 impregnation has beneficial effect on the charge capacity of the activated carbon/sulfur cathode in the Li-S cell. The specific capacity of the cathode in the cell with TiO2-modified separator is 632 mAh g-1 (calculated from cyclic voltammetry) and 673 mAh g-1 (determined from galvanostatic chronopotentiometry). Facile impregnation of the separator with nanocrystalline TiO2 results in the 10-20 % stable increase of the charge capacity of corresponding activated carbon/sulfur cathode as compared to its electrochemical performance in the system with non-modified separator.
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Li, Bin. "Unlocking Failure Mechanisms and Improvement of Practical Li-S Pouch Cells through in Operando Pressure Study." ECS Meeting Abstracts MA2022-01, no. 1 (July 7, 2022): 109. http://dx.doi.org/10.1149/ma2022-011109mtgabs.
Повний текст джерелаАнотація:
Lithium-sulfur (Li-S) batteries have been considered a promising candidate for next-generation high-energy density storage technology due to their low cost and high theoretical capacity. However, since 2017, more and more attentions have been paid to the gap of lab cell characterization (coin cell) and prototype cell (pouch cell) development since misinterpretations and false expectations are frequently reported: material property impacts are often over-interpreted, while parameters with indirect impact (e.g., electrode and separator porosity, tortuosity, and pressure on cell stack) are neglected. In order to accelerate Li-S battery commercialization, the rapid transfer of material-related concept discovered in coin cells to a pouch cell level is essential, as some problems ignored or deemed minimal at the smaller level could have a greater effect on the performance of the larger pouch cell. The issues existing in practical pouch cell should be discovered, which would shed light on further battery materials development, or inspire the novel approaches to identify cell failure and improve cell performances at the pouch cell level. Considering the gap between practical pouch cells and coin cells, in addition to the noticeable difference in electrode size (e.g., the electrode size of practical pouch cell is usually >100 times of that of coin cell), a much higher stack pressure (> 1Mpa) is usually applied inside the coin cell. It was taken for granted that stack pressure was playing a critical role, leading to inconsistent performance between pouch cells and coin cells. Furthermore, with increasing size of the cells (especially for multi-layer pouch cells), the electrolyte wettability needs to be taken seriously. Otherwise, the sulfur utilization would be largely reduced as ionic conduction pathways was significantly affected. Herein, we rationally designed two kinds of cathode: Non-calendared sulfur electrode (NCSE) and Calendared sulfur electrode (CSE). The former’s porosity (ε) and tortuosity (τ) were proven to change with stack pressures while the latter’s do not change by simulations based on micro-XCT results with in-situ pressure applied. These two sulfur cathodes provide preconditions to distinguish the effects of stack pressure and porosity/tortuosity on Li-S pouch cell performances. For the first time, through in-situ monitoring of pressure applied onto Li-S pouch cells, the failure mechanisms of Li-S pouch cells were deeply understood, and the approaches to improve Li-S pouch cell performances were identified. It is found that highly porous structures of cathodes/separators and slow electrolyte diffusion through cathodes/separators can both lead to poor initial wetting. Additionally, Li-metal anode dominates the thickness variation of the whole pouch cell, which is verified by in situ measured pressure variation. Consequently, a real-time approach that combined normalized pressure with dP/dV analysis is proposed and validated to diagnose the morphology evolution of Li-metal anode. Moreover, applied pressure and porosity/tortuosity ratio of the cathode are both identified as independent factors that influence anode performance. In addition to stabilizing anodes, high pressure is proven to improve the cathode connectivity and avoid cathode cracking over cycling, which improves the possibility of developing cathodes with high sulfur mass loading. This work provides insights into Li-S pouch cell design (e.g., cathode and separator) and highlights pathways to improve cell capacity and cycling performance with applied and monitored pressure. Figure 1