Carbon materials together with various redox electrolytes have been developed intensively in recent years to assemble large-capacitance and high-rate supercapacitors. However, the weak interactions between carbon electrodes and redox electrolytes result in the severe shuttle of redox ions in electrolytes, causing critical self-discharge performance. Here we report a functional interface to establish strong adhesion of redox ions on the liquid side towards carbon nanotube arrays, leading to efficient confinement of redox ions around carbon electrode and enhanced electronic transfer between the electrode and redox electrolyte. Benefiting from the interface, the coupling carbon nanotube arrays-K₃Fe(CN)₆ system exhibits a substantially boosted self-discharge rate with no decay after 32 h under the open-circuit stage, as well as a large areal capacitance up to 3.048 F cm⁻². The introduction of functionalized interface suggests a general and versatile concept for carbon-based electrodes to achieve battery-like charge storage with reliable features.

近年来，碳材料与各种氧化还原电解质一起得到了广泛的开发，以组装大容量和高速率的超级电容器。然而，碳电极与氧化还原电解质之间的弱相互作用导致电解质中氧化还原离子的严重穿梭，从而导致严重的自放电性能。在这里，我们报告了一个功能界面，该界面建立了氧化还原离子在液体侧对碳纳米管阵列的牢固粘附，从而有效地限制了碳电极周围的氧化还原离子，并增强了电极与氧化还原电解质之间的电子传递。得益于该界面，偶联的碳纳米管阵列-K ₃ Fe（CN）₆该系统表现出了显着提升的自放电速率，在开路状态下经过32h后没有衰减，以及高达3.048 F cm ^-2的大面积电容。功能化界面的引入为碳基电极提出了通用且通用的概念，以实现具有可靠功能的类似电池的电荷存储。