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Gels 2022, 8, 193 8 of 13 The result suggests that the migration of the ions in B8-BMPTFSI and B8-BMPTFSI-NaTFSI gels is similar to that of a viscous liquid [25]. The ionic conductivity of the B8-BMPTFSI-NaTFSI ionogel still achieved 10−3 S/m, albeit less than that of B8-BMPTFSI ionogel. To evaluate the chemical stability of the B8-BMPTFSI-NaTFSI ionogel, aging exper- iments were performed on the ionogel; therefore, sodium metal was immersed into the ionogel and then placed in an inert environment at 50 ◦C for 30 days. After the B8- BMPTFSI-NaTFSI ionogel was in contact with the sodium metal at 50 / for 30 days, no clear color change was observed, and its state was not significantly different from that of the newly prepared ionogel (Figure S5a). In addition, 1H- NMR data indicated that the signals of the main functional groups of BMPTFSI and B8 of the aged ionogel do not change (Figure S5b–e), illustrating the excellent chemical stability of the B8-BMPTFSI-NaTFSI ionogel. Furthermore, electrochemical impedance spectroscopy (EIS) was employed to measure the TNa+ of the B8-BMPTFSI-NaTFSI gel (4% B8, w/v, 0.3 M NaTFSI) using a symmetrical Na/electrolyte/Na cell. Figure 5B represents the Nyquist plots for the ionogel electrolyte before and after polarization; a model equivalent circuit manifested from the Nyquist plots is shown as Figure 5C, in which R0 and R1 denotes the resistances to ionic and electronic transport, respectively [51]. The calculated TNa+ value of the ionogel was 0.1835, a satisfactory value [30]. Thus, a multifunctional ionogel electrolyte suitable for NIBs has been successfully developed. The performance parameters, including ionic conductivity, self-healing, and TNa+, of our ionogel electrolyte were compared with those of other ionogel electrolytes for NIBs (from 2010 to present, as shown in Table S2), the ionogel electrolyte of this work is the only self-healing ionogel electrolyte reported for Na batteries with high room temperature conductivity and good TNa+. However, a lot of work needs to be carried out before a high-performance sodium-ion battery can be successfully produced based on our ionogel, such as the compatibility study of the ionogel with different electrodes, the stability and efficiency study of the ionogel at different temperatures, etc. 3. Conclusions In this study, a novel supramolecular ionogel electrolyte based on the D-gluconic acetal- based gelator with a favorable ionic conductivity, satisfactory Na+ transference number (TNa+), high mechanical strength, chemical stability, thixotropy, and rapid self-healing property was prepared. The introduction of NaTFSI induced a denser microstructure of the ionogel, leading to the decreased conductivity of the ionogel electrolyte; however, the resultant B8-BMPTFSI-NaTFSI ionogel still exhibited high conductivity. The B8-BMPTFSI- NaTFSI ionogel electrolyte exhibited excellent chemical stability to Na metal, which is a potentially safe electrolyte material for Na batteries. The thixotropic ionogel electrolyte effectively resisted external mechanical stimulation and prevented electrolyte leakage, thus prolonging the service life of the electrolyte material. In addition, the application of thixotropic nature to the electrolyte will realize its free molding in accordance to the shape of the conduction interface, which is difficult for several electrolytes. The self-assembly and thixotropic mechanisms of ionogel were also examined and described in detail. However, more work needs to be carried out to study the effect of ions on the self-assembly of organic low-molecular-weight gelators, so as to develop gelators with self-assembly ability in the presence of Li+ and Mg2+, and expand the application range of supramolecular ionogels in the field of metal-ion batteries. In total, the multifunctional thixotropic B8-BMPTFSI-NaTFSI ionogel developed exhibited immense potential for application in high-performance Na batteries, and our studies on self-assembly and thixotropic mechanism provided a direction for the future design of more functionalized supramolecular ionogel electrolytes. 4. Materials and Methods 4.1. Materials D-Gluconic acid, 3, 4-dichlorobenzaldehyde, 1, 6-hexanediamine, and 4-dimethylaminopyridine (DMAP) were purchased from Aladdin Bio-Chem Technology Co., Ltd. (Shanghai, China). OctylPDF Image | Thixotropic Ionogel Electrolyte for Sodium Batteries
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