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DOI | 10.1039/c9ee01338e |
Visualization of regulated nucleation and growth of lithium sulfides for high energy lithium sulfur batteries | |
Xu Z.-L.; Kim S.J.; Chang D.; Park K.-Y.; Dae K.S.; Dao K.P.; Yuk J.M.; Kang K. | |
发表日期 | 2019 |
ISSN | 17545692 |
起始页码 | 3144 |
结束页码 | 3155 |
卷号 | 12期号:10 |
英文摘要 | The formation of lithium sulfides as discharge products imparts high specific energy density to lithium sulfur batteries (LSBs), however, the involvement of soluble intermediates in the battery reaction makes it challenging to achieve it reversibly for extended cycles. The precise understanding of phase transitions from the soluble intermediates to solid discharge products would aid in fundamentally resolving practical issues involving the intermediates, and thus allow the realization of long-lived high-energy-density LSBs. Herein, we utilize liquid in situ transmission-electron-microscopy (TEM) to probe detailed liquid-solid reaction processes. It reveals that the surface nature of the host materials of the polysulfides critically influences the growth mechanism of lithium sulfides. It is elucidated that polar hosts induce instantaneous nucleation of lithium sulfides, followed by diffusion-controlled-to-reaction-limited growth kinetics and a crystalline-to-amorphous phase transition. Moreover, it is verified that polysulfides are better immobilized in polar hosts, whereas polysulfide diffusion through nonpolar hosts is evidently observed, leading to the eventual degradation of cells. Based on these findings, an optimal host structure for sulfur is proposed, where the dual walls of polar (inner)/nonpolar (outer) spheres confine the polysulfides. The new cathode exhibits remarkable electrochemical performance, retaining a capacity of 4.3 mA h cm-2 over 400 cycles at a low electrolyte/sulfur ratio of 6.8 ml g-1, which rivals state-of-the-art LSBs. This work contributes the first liquid in situ TEM study of liquid-solid phase evolution for high energy electrode materials. © 2019 The Royal Society of Chemistry. |
英文关键词 | Cathodes; Electric discharges; Electrolytes; Growth kinetics; High resolution transmission electron microscopy; In situ processing; Liquids; Lithium batteries; Lithium compounds; Nucleation; Polysulfides; Reaction intermediates; Reaction kinetics; Structural optimization; Sulfur compounds; Crystalline-to-amorphous; Electrochemical performance; High energy densities; In situ transmission electron microscopy (TEM); Instantaneous nucleations; Liquid-solid reaction; Nucleation and growth; Specific energy density; Lithium sulfur batteries; detection method; electrochemical method; electrode; equipment; inorganic compound; lithium; performance assessment; phase transition; sulfur |
语种 | 英语 |
来源期刊 | Energy & Environmental Science
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文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/189813 |
作者单位 | Department of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul, 151-742, South Korea; Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon, 34141, South Korea; Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul National University, 1 Gwanak-ro, Gwanak-gu Seoul, 08826, South Korea; Institute of Engineering Research, Seoul National University, 1 Gwanak-ro, Gwanak-gu Seoul, 08826, South Korea |
推荐引用方式 GB/T 7714 | Xu Z.-L.,Kim S.J.,Chang D.,et al. Visualization of regulated nucleation and growth of lithium sulfides for high energy lithium sulfur batteries[J],2019,12(10). |
APA | Xu Z.-L..,Kim S.J..,Chang D..,Park K.-Y..,Dae K.S..,...&Kang K..(2019).Visualization of regulated nucleation and growth of lithium sulfides for high energy lithium sulfur batteries.Energy & Environmental Science,12(10). |
MLA | Xu Z.-L.,et al."Visualization of regulated nucleation and growth of lithium sulfides for high energy lithium sulfur batteries".Energy & Environmental Science 12.10(2019). |
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