The reusability, non-volatility and non-corrosiveness of ionic liquids (ILs), as well as their ease of isolation and a large electrochemical stability window, make them an interesting choice as environmentally friendly electrolytes for metal/air batteries. ILs have been described as designer solvents as their properties and behaviour can be adjusted to suit an individual reaction need. In the framework of this study we applied a conceptually similar design approach and showed that a simple parameter such as the concentration of a Li⁺ dopant dramatically affects the reaction yields of Li/O₂ based energy storage devices. We studied the effect of Li⁺ concentration from 0.1 to 1 M in a LiTFSI:PYR₁₄TFSI ionic liquid electrolyte on the kinetics of the oxygen reduction reaction (ORR) and on the formation rate of different Li–O species at two different temperatures, finding that the discharge capacity, rates and product distribution change in a non-linear way. At 60 °C, the highest rates and up to one order of magnitude larger capacities were observed at intermediate LiTFSI concentrations, implying a complete mechanism switch from surface to volume phase mediation for Li₂O₂ precipitation. At room temperature the same evolution was observed, even if in this case the surface mediation remained predominant at all concentrations. These results suggest the possibility to optimise the ionic liquid based Li/O₂ battery performances in terms of discharge capacity and lithium use, by tuning the temperature and alkali cation concentration.

中文翻译：

---

通过Li ⁺掺杂剂浓度 调节离子液体基Li / O ₂电池中的氧还原反应。

离子液体（IL）的可重复使用性，不挥发性和非腐蚀性，以及它们的易分离性和大的电化学稳定性窗口，使其成为金属/空气电池组的环保电解质的一个有趣的选择。IL被描述为设计溶剂，因为可以调整其性质和行为以适应单个反应的需要。在这项研究的框架中，我们应用了概念上相似的设计方法，并表明简单的参数（例如Li ⁺掺杂剂的浓度）会极大地影响基于Li / O ₂的储能装置的反应产率。我们研究了LiTFSI：PYR ₁₄中Li ⁺浓度从0.1到1 M的影响TFSI离子液体电解质对氧还原反应（ORR）的动力学以及在两个不同温度下不同Li–O物种的形成速率的影响，发现放电容量，速率和产物分布呈非线性变化。在60°C时，在中等LiTFSI浓度下观察到了最高的速率和高达一个数量级的容量，这意味着Li ₂ O ₂沉淀从表面相到体积相的完全机制转换。在室温下，即使在所有浓度下，表面介导仍然占主导地位，也观察到了相同的演变。这些结果表明优化基于离子液体的Li / O ₂的可能性。 通过调节温度和碱金属阳离子浓度来确定电池在放电容量和锂用量方面的性能。