Altering Mechanical Properties to Improve Electrode Contacts by Organic Modification of Silica‐Based Ionogel Electrolytes for Sodium‐Ion Batteries

Abstract Sodium‐ion batteries (SIBs) are a possible candidate to create safe, sustainable, and cost‐effective batteries. Solid sodium‐ion conducting organically modified ionogel electrolytes are investigated. Silica‐based ionogels typically consist of an ionic liquid electrolyte (ILE) confined within a silica matrix and possess high thermal stability, good ionic conductivity, safety, and good electrochemical stability. However, they readily deteriorate when stress is applied, decreasing the electrolyte's and battery's overall performance. The mechanical characteristics of silica can be improved using organic moieties, creating Ormosils®. Silica‐based ionogels with phenyl‐modified silanes improve the mechanical characteristics by a reduction of their Young's modulus (from 29 to 6 MPa). This is beneficial to the charge‐transfer resistance, which decreases after implementing the electrolyte in half cells, demonstrating the improved interfacial contact. Most importantly, the phenyl groups change the interacting species at the silica interface. Cationic imidazolium species pi‐stacked to the phenyl groups of the silica matrix, pushing the anions to the bulk of the ILE, which affects the ionic conductivity and electrochemical stability, and might affect the quality of the SEI in half cells. In essence, the work at hand can be used as a directory to improve mechanical characteristics and modify and control functional properties of ionogel electrolytes.