Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High-Energy Li-S Batteries.,Angewandte Chemie International Edition

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Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High-Energy Li-S Batteries.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-07-09 , DOI: 10.1002/anie.202007159
Chen Zhao _{1,

2} , Gui-Liang Xu ₂ , Tianshou Zhao ₁ , Khalil Amine _{2,

3,

4}

Affiliation

Electrolyte modulation simultaneously suppresses polysulfide the shuttle effect and lithium dendrite formation of lithium–sulfur (Li‐S) batteries. However, the sluggish S redox kinetics, especially under high S loading and lean electrolyte operation, has been ignored, which dramatically limits the cycle life and energy density of practical Li‐S pouch cells. Herein, we demonstrate that a rational combination of selenium doping, core–shell hollow host structure, and fluorinated ether electrolytes enables ultrastable Li stripping/plating and essentially no polysulfide shuttle as well as fast redox kinetics. Thus, high areal capacity (>4 mAh cm⁻²) with excellent cycle stability and Coulombic efficiency were both demonstrated in Li metal anode and thick S cathode (4.5 mg cm⁻²) with a low electrolyte/sulfur ratio (10 μL mg⁻¹). This research further demonstrates a durable Li‐Se/S pouch cell with high specific capacity, validating the potential practical applications.

中文翻译：

超越多硫化物穿梭和锂枝晶形成：解决实用高能锂硫电池缓慢的硫氧化还原动力学问题。

电解质调制同时抑制多硫化物的穿梭效应和锂硫（Li-S）电池的锂枝晶形成。然而，缓慢的 S 氧化还原动力学，尤其是在高 S 负载和贫电解质操作下，已被忽略，这极大地限制了实际 Li-S 软包电池的循环寿命和能量密度。在这里，我们证明了硒掺杂、核壳空心主体结构和氟化醚电解质的合理组合能够实现超稳定的锂剥离/电镀，并且基本上没有多硫化物穿梭以及快速的氧化还原动力学。因此，具有优异循环稳定性和库仑效率的高面积容量（>4 mAh cm ^-2）在锂金属负极和厚硫正极（4.5 mg cm ^-2) 具有低电解质/硫比 (10 μL mg ^-1 )。该研究进一步证明了具有高比容量的耐用 Li-Se/S 软包电池，验证了潜在的实际应用。

更新日期：2020-07-09

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