In recent years, secondary lithium-ion batteries (LIBs) have become critical components for portable devices and large power source systems such as electric vehicles (EVs) and hybrid EVs (HEVs).[1],[2] However, conventional LIBs typically use flammable nonaqueous liquid electrolytes, posing a serious safety risk. Our previous study[3] demonstrated that one promising approach for safe LIBs involves using electrolytes based on a series of ionic liquids (ILs) with branched alkyl imidazolium cations. The introduction of bulky branched alkyl groups enhances charge delocalization in imidazolium cations, thereby improving the electrochemical reduction stability. Herein, we evaluated the compatibility and electrochemical performance of two types of ILs: branched alkyl functional and electrochemically polymerizable ILs. Moreover, binary mixture–based electrolytes based on their ILs were investigated for use in LIBs.We synthesized two types of ILs: reduction-stable and polymerizable ILs (Fig. 1). An IL-based electrolyte was mixed with various compositions of reduction-stable and polymerizable ILs, with LiFSA (LiFSA molal concentration: ca. 1.5 mol/kg) serving as the Li ion source. The characteristics of the involved battery were examined using a graphite electrode | IL–LiFSA mixture–based electrolyte | Li metal half-cell configuration. The graphite electrode sheets comprised NMC powder (86 wt%) as the active material, acetylene black (7 wt%) as an electrically conductive additive, and poly(vinylidene fluoride) (7 wt%) as a binder. The graphite electrode sheet, separator, IL–LiFSA mixture–based electrolyte, and Li were assembled into a battery cell. Performance tests for charge–discharge rates were conducted at 303 K, with the involved rates varying from 0.1 to 0.5 C.Fig. 2 shows the first charge–discharge profiles of the graphite | Li half-cells with [EPisoIm][FSA]–, [APisoIm][FSA]–, and [EPisoIm]0.8[APisoIm]0.2[FSA]–based electrolytes. During the first charge with the [APisoIm][FSA]– and [EPisoIm]0.8[APisoIm]0.2[FSA]–based electrolytes, a plateau was observed at approximately 0.5 V, attributed to the reduction decomposition and polymerization of [APisoIm] cations on graphite. The presence of [APisoIm] cations enabled the formation of a stable solid electrolyte interface, an electron-insulating, lithium-ion-conducting film.[1] M. Wakihara, “Recent developments in lithium ion batteries”, Mater. Sci. Eng., R, 33, 109 (2001).[2] D. D. Lecce, R. Verrelli, and J. Hassoun, “Lithium-ion batteries for sustainable energy storage: recent advances towards new cell configurations”, Green Chem., 19, 3442 (2017). Figure 1
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