Minimizing the Abnormal High-Potential Discharge Process Related to Redox Mediators in Lithium–Oxygen Batteries,The Journal of Physical Chemistry Letters

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Minimizing the Abnormal High-Potential Discharge Process Related to Redox Mediators in Lithium–Oxygen Batteries
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2018-11-13 00:00:00 , DOI: 10.1021/acs.jpclett.8b02899
Shichao Wu ₁ , Yu Qiao ₁ , Han Deng ₁ , Yibo He ₁ , Haoshen Zhou _{1,

2}

Affiliation

Nonaqueous lithium–oxygen batteries can achieve a reduced charge potential when an available redox mediator is introduced. However, there are accompanying problems, such as the shuttle effect and the abnormal high-potential discharge process (>2.96 V) after the first cycle. The shuttle effect can be addressed by developing a blocking separator or resistant solid electrolyte interphase on the anode. No attention has been paid to the abnormal discharge process. Here, we unravel the underlying mechanism causing the undesired abnormal phenomenon. Our results show that the slow reaction rate between the discharged lithium peroxide and redox mediator and the low yield of lithium peroxide should take primary responsibility for the abnormal discharge issue. The sluggish reaction kinetics results from the formed byproducts covering lithium peroxide. We propose developing redox mediator-containing hydrate-melt lithium–oxygen batteries. The lithium hydroperoxide intermediator shows high reaction activity with the redox mediator and improves battery charge ability, thus solving the abnormal discharge problem. This work sheds light on the further design of lithium–oxygen batteries using a redox mediator.

中文翻译：

最大限度地减少锂氧电池中与氧化还原介体有关的异常高电势放电过程

当引入可用的氧化还原介体时，非水锂氧电池可以降低充电电位。但是，伴随着一些问题，例如在第一个循环后出现飞梭效应和异常的高电势放电过程（> 2.96 V）。穿梭效应可以通过在阳极上形成阻挡隔板或电阻性固体电解质相来解决。尚未注意异常放电过程。在这里，我们揭示了导致不希望的异常现象的潜在机制。我们的结果表明，放电的过氧化锂与氧化还原介体之间的反应速度较慢，而过氧化锂的收率较低，这是造成异常放电问题的主要原因。反应动力学迟缓是由覆盖过氧化锂的副产物形成的。我们建议开发包含氧化还原介体的水合物熔体锂氧电池。氢过氧化物锂介体与氧化还原介体表现出高反应活性，并提高了电池充电能力，从而解决了异常放电问题。这项工作为使用氧化还原介体的锂氧电池的进一步设计提供了启示。

更新日期：2018-11-13

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