Exploring Binder–Ionic Liquid Electrolyte Systems in Silicon Oxycarbide Negative Electrodes for Lithium-Ion Batteries

Enhancing the safety of lithium-ion batteries (LIBs) by replacing flammable electrolytes is a key challenge. Ionic liquid (IL)-based electrolytes are considered an interesting alternative due to their thermal and chemical stability, high voltage stability window, and tunable properties. This study investigates the electrochemical behavior of two newly synthesized ILs, comparing them to conventional alkyl carbonate-based electrolytes. Nitrogen-doped carbon silicon oxycarbide (NC-SiOC), used as the active material in negative electrodes, was combined with two polymeric binders: poly(acrylic acid) (PAA) and poly(acrylonitrile) (PAN). NC-SiOC/PAN electrodes exhibited a significantly higher initial charge capacity—approximately 25–30% greater than their PAA-based counterparts in the first cycle at 0.1 A g⁻¹ (850–990 mAh g⁻¹ vs. 600–700 mAh g⁻¹), and demonstrated an improved initial Coulombic efficiency (67% vs. 62%). Long-term cycling stability over 1000 cycles at 1.6 A g⁻¹ retained 75–80% of the initial 0.1 A g⁻¹ capacity. This outstanding performance is attributed to the synergistic effects of nitrogen-rich carbonaceous phases within the NC-SiOC material and the cyclized-PAN binder, which facilitate structural stability by accommodating volumetric changes and enhancing solid electrolyte interphase (SEI) stability. Notably, despite the lower ionic transport properties of the IL electrolytes, their incorporation did not compromise performance, supporting their feasibility as safer electrolyte alternatives. These findings offer one of the most promising electrochemical performances reported for SiOC materials to date.