The electric double-layer capacitor (EDLC), which utilizes porous activated carbon and ionic liquid electrolytes, is a promising energy storage technology due to its fast charge-discharge capability, excellent cycle stability, and wide voltage window. Understanding the energy storage mechanism in ionic liquids, particularly how the structural characteristics of anions and cations affect the capacitance of activated carbon, is crucial for optimizing EDLC performance. By revealing these microscopic interactions, researchers can better select suitable ionic liquids and design high-performance EDLCs.
Recently, a research team from the Institute of Clean Energy Chemistry and Materials at the Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, made significant progress in studying the energy storage mechanisms of ionic liquids in EDLCs. They developed four types of nano-silica-grafted ionic liquids, allowing separate analysis of cations and anions by exploiting the fact that only one type of ion can freely enter and exit the activated carbon pores during charging and discharging.
In this study, the structure of the silica-grafted ionic liquid was designed so that one ion (such as BMIM+, NBu4+, NTf2–, or PF6–) could move freely, while the counter-ion remained fixed. For example, trifluoromethanesulfonimide anion (NTf2–) and methylimidazolium cation (MIM+) were covalently attached to 7 nm silica nanoparticles. Since most activated carbons used in the study have pore sizes less than 4 nm, the silica-bound ions are blocked, allowing only the free ions (BMIM+, NBu4+, NTf2–, or PF6–) to enter the pores. This setup enables a straightforward electrochemical test to quantify ion insertion, with the cyclic voltammetry curve directly reflecting the contribution of each ion to the overall capacitance.
Using commercial activated carbon YP-50F as the electrode, the team successfully characterized the capacity contributions of individual cations (BMIM+ and NBu4+) and anions (NTf2– and PF6–), along with their respective voltage windows. Through quartz crystal microbalance (EQCM) measurements, they further explored the energy storage behavior of YP-50F in the ionic liquid BMIM-NTf2, combining electrochemical data to provide a deeper understanding of the underlying mechanisms.
These findings were published in *Nature Communications* and supported by the National Natural Science Foundation of China and the Lanzhou Institute of Chemical Industry’s “13th Five-Year Plan†initiative. The work offers a new strategy for investigating the role of ionic liquid ions in EDLCs and paves the way for future advancements in high-performance energy storage systems.
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