The development of new electrolyte and electrode designs and compositions has led to advances in electrochemical energy-storage (EES) devices over the past decade. However, focusing on either the electrode or electrolyte separately is insufficient for developing safer and more efficient EES devices in various working environments, as the energy-storage ability is determined by the ion arrangement and charge and/or electron transfer at the electrode–electrolyte interface. In this Review, we assess the fundamental physicochemical and electrochemical properties at the electrode–electrolyte interfaces in Li-ion batteries and supercapacitors using safe and electrochemically stable ionic-liquid electrolytes. Key reactions and interactions at the electrode–electrolyte interface, as well as geometric constraints and temperature effects, are highlighted. Building on the fundamental understanding of interfacial processes, we suggest potential strategies for designing stable and efficient ionic-liquid-based EES devices with emerging electrode materials.

在过去的十年中，新的电解质和电极设计和成分的发展已导致电化学储能（EES）装置的发展。但是，单独关注电极或电解质不足以在各种工作环境下开发出更安全，更高效的EES装置，因为能量存储能力取决于离子排列以及电极-电解质界面处的电荷和/或电子转移。在本综述中，我们使用安全和电化学稳定的离子液体电解质评估了锂离子电池和超级电容器中电极-电解质界面的基本物理化学和电化学性质。重点介绍了电极-电解质界面上的关键反应和相互作用，以及几何约束和温度效应。