scholarly journals Expansion-tolerant architectures for stable cycling of ultrahigh-loading sulfur cathodes in lithium-sulfur batteries

2020 ◽  
Vol 6 (1) ◽  
pp. eaay2757 ◽  
Author(s):  
Mahdokht Shaibani ◽  
Meysam Sharifzadeh Mirshekarloo ◽  
Ruhani Singh ◽  
Christopher D. Easton ◽  
M. C. Dilusha Cooray ◽  
...  

Lithium-sulfur batteries can displace lithium-ion by delivering higher specific energy. Presently, however, the superior energy performance fades rapidly when the sulfur electrode is loaded to the required levels—5 to 10 mg cm−2— due to substantial volume change of lithiation/delithiation and the resultant stresses. Inspired by the classical approaches in particle agglomeration theories, we found an approach that places minimum amounts of a high-modulus binder between neighboring particles, leaving increased space for material expansion and ion diffusion. These expansion-tolerant electrodes with loadings up to 15 mg cm−2 yield high gravimetric (>1200 mA·hour g−1) and areal (19 mA·hour cm−2) capacities. The cells are stable for more than 200 cycles, unprecedented in such thick cathodes, with Coulombic efficiency above 99%.

2019 ◽  
Vol 7 (13) ◽  
pp. 7644-7653 ◽  
Author(s):  
Jingyi Wu ◽  
Na You ◽  
Xiongwei Li ◽  
Hongxia Zeng ◽  
Shuai Li ◽  
...  

The synergistic effect of the SiO2@MoS2 core–shell nanocomposite simultaneously facilitates Li+ diffusion and provides triple confinement of polysulfides.


2019 ◽  
Vol 7 (2) ◽  
pp. 315-323 ◽  
Author(s):  
Chaoqun Niu ◽  
Jie Liu ◽  
Tao Qian ◽  
Xiaowei Shen ◽  
Jinqiu Zhou ◽  
...  

Abstract Lithium–sulfur batteries have great potential for high-performance energy-storage devices, yet the severe diffusion of soluble polysulfide to electrolyte greatly limits their practical applications. To address the above issues, herein we design and synthesize a novel polymer binder with single lithium-ion channels allowing fast lithium-ion transport while blocking the shuttle of unnecessary polysulfide anions. In situ UV–vis spectroscopy measurements reveal that the prepared polymer binder has effective immobilization to polysulfide intermediates. As expected, the resultant sulfur cathode achieves an excellent specific capacity of 1310 mAh g−1 at 0.2 C, high Coulombic efficiency of 99.5% at 0.5 C after 100 cycles and stable cycling performance for 300 cycles at 1 C (1 C = 1675 mA g−1). This study reports a new avenue to assemble a polymer binder with a single lithium-ion channel for solving the serious problem of energy attenuation of lithium–sulfur batteries.


2019 ◽  
Author(s):  
Yu-Chuan Chien ◽  
Ruijun Pan ◽  
Ming-Tao Lee ◽  
Leif Nyholm ◽  
Daniel Brandell ◽  
...  

This work aims to address two major roadblocks in the development of lithium-sulfur (Li-S) batteries: the inefficient deposition of Li on the metallic Li electrode and the parasitic "polysulfide redox shuttle". These roadblocks are here approached, respectively, by the combination of a cellulose separator with a cathode-facing conductive porous carbon interlayer, based on their previously reported individual benefits. The cellulose separator increases cycle life by 33%, and the interlayer by a further 25%, in test cells with positive electrodes with practically relevant specifications and a relatively low electrolyte/sulfur (E/S) ratio. Despite the prolonged cycle life, the combination of the interlayer and cellulose separator increases the polysulfide shuttle current, leading to reduced Coulombic efficiency. Based on XPS analyses, the latter is ascribed to a change in the composition of the solid electrolyte interphase (SEI) on Li. Meanwhile, electrolyte decomposition is found to be slower in cells with cellulose-based separators, which explains their longer cycle life. These counterintuitive observations demonstrate the complicated interactions between the cell components in the Li-S system and how strategies aiming to mitigate one unwanted process may exacerbate another. This study demonstrates the value of a holistic approach to the development of Li-S chemistry.<br>


Author(s):  
Maru Dessie Walle ◽  
You-Nian Liu

AbstractThe lithium–sulfur (Li–S) batteries are promising because of the high energy density, low cost, and natural abundance of sulfur material. Li–S batteries have suffered from severe capacity fading and poor cyclability, resulting in low sulfur utilization. Herein, S-DHCS/CNTs are synthesized by integration of a double-hollow carbon sphere (DHCS) with carbon nanotubes (CNTs), and the addition of sulfur in DHCS by melt impregnations. The proposed S-DHCS/CNTs can effectively confine sulfur and physically suppress the diffusion of polysulfides within the double-hollow structures. CNTs act as a conductive agent. S-DHCS/CNTs maintain the volume variations and accommodate high sulfur content 73 wt%. The designed S-DHCS/CNTs electrode with high sulfur loading (3.3 mg cm−2) and high areal capacity (5.6 mAh mg cm−2) shows a high initial specific capacity of 1709 mAh g−1 and maintains a reversible capacity of 730 mAh g−1 after 48 cycles at 0.2 C with high coulombic efficiency (100%). This work offers a fascinating strategy to design carbon-based material for high-performance lithium–sulfur batteries.


2021 ◽  
Vol 10 (1) ◽  
pp. 20-33
Author(s):  
Lian Wu ◽  
Yongqiang Dai ◽  
Wei Zeng ◽  
Jintao Huang ◽  
Bing Liao ◽  
...  

Abstract Fast charge transfer and lithium-ion transport in the electrodes are necessary for high performance Li–S batteries. Herein, a N-doped carbon-coated intercalated-bentonite (Bent@C) with interlamellar ion path and 3D conductive network architecture is designed to improve the performance of Li–S batteries by expediting ion/electron transport in the cathode. The interlamellar ion pathways are constructed through inorganic/organic intercalation of bentonite. The 3D conductive networks consist of N-doped carbon, both in the interlayer and on the surface of the modified bentonite. Benefiting from the unique structure of the Bent@C, the S/Bent@C cathode exhibits a high initial capacity of 1,361 mA h g−1 at 0.2C and achieves a high reversible capacity of 618.1 m Ah g−1 at 2C after 500 cycles with a sulfur loading of 2 mg cm−2. Moreover, with a higher sulfur loading of 3.0 mg cm−2, the cathode still delivers a reversible capacity of 560.2 mA h g−1 at 0.1C after 100 cycles.


2002 ◽  
Vol 149 (11) ◽  
pp. A1437 ◽  
Author(s):  
Sang-Eun Cheon ◽  
Ji-Hoon Cho ◽  
Ki-Seok Ko ◽  
Chang-Wee Kwon ◽  
Duck-Rye Chang ◽  
...  

CrystEngComm ◽  
2021 ◽  
Author(s):  
Guiying Xu ◽  
Yongying Li ◽  
Hui Cheng ◽  
Guan Liu ◽  
Ziyang Yang ◽  
...  

The dissolution of polysulfides (LiPSs) always leads to low Coulombic efficiency, dramatic capacity decay, and short cycle life, which hinders the practical application of lithium-sulfur (Li-S) batteries. In this study,...


2015 ◽  
Author(s):  
◽  
Donald A. Dornbusch

[ACCESS RESTRICTED TO THE UNIVERSITY OF MISSOURI AT REQUEST OF AUTHOR.] The following dissertation investigates different aspects of lithium-sulfur batteries. Lithium-sulfur batteries have a higher theoretical capacity than current lithium-ion chemistries. First, a study on the lithium-metal electrode and the formation of dendrites investigates how flow impacts the failure from dendrites of these electrodes. Second, a study relying on charging to avoid the soluble intermediates generated through charge/discharge of sulfur-cathodes which are the primary cause of capacity fade in these systems. Third, sulfur is polymerized through radical polymerization with diene comonomers in order to reduce the solubility and mobility of the intermediates generated during cycling. Using Brunauer-Emmett-Teller (BET) theory, the surface area and pore volume can be observed before and after cycling demonstrating the amount of mobility the active material has during cycling. Finally, a study on the conduction phenomena in convection batteries is studied through a literature review and COMSOL simulation.


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