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Batteries 2022, 8, 157 18 of 26 voids of NZSP, which avoided the immediate contact between the Na metal anode and NZSP. In addition, the NaSn alloy was also formed during the Na metal deposition, which endowed the good wettability between the Na anode and NZSP and reduced the interfa‐ cial impedance. Furthermore, the mixed‐ion‐electron conductor layer on NZSP also real‐ ized the homogeneous and rapid Na‐ion flux transfer from the interface, resulting in uni‐ form Na metal deposition. Interface modification was also another strategy to improve interface resistance be‐ tween the electrolyte and electrode [53,121]. Therefore, Wang et al. adopted a surface po‐ tential regulation strategy to mitigate the interfacial potential divergence and modify the Na/NZSP interface through the active control of the ceramic electrolyte surface micro‐ structure [121]. The surface regulation of the Na/ NZSP interface presented stability for over 4 months with the interfacial resistance of 129 Ω cm2 at 25 °C. To understand the modification of the Na3Zr2Si2PO12 interface, they conducted the in‐depth ToF‐SIMS map‐ ping of the interface after Na metal plating/stripping, as shown in Figure 7. Na metal is‐ lands (Figure 7a) and Na dendrite (Figure 7b) with tens of millimeters could be observed in the NZSP electrolyte without interface modification. With the interface modification, the Na metal anode presented uniform distribution on the surface without Na dendrite (Figure 7c,d). These results were also demonstrated in the SEM image. Figure 7. (a) Mapping of Na species and (b) overlay depth profile of Na, Zr, and Si on TS1300‐ 15/1200 after cycling; (c) mapping of Na species and (d) overlay depth profile of Na, Zr, and Si on NS1250 after cycling, reproduced with permission from Reference [121] Copyright 2021, Elsevier. Except for Na‐β”‐Al2O3 and NZSP all‐solid‐state electrolytes, the other new types of all‐solid‐state electrolytes for NMBs were also developed. Ruiz‐Martinez et al. developed NaYxNH3 (Y = I−, BF4− or BH4−)) solid‐state electrolyte with a high Na‐ion concentration (>7 M) and high specific conductivity (0.1 S cm−1) for NMBs [122]. They selected three different solid‐state electrolytes, NaI3.3NH3, NaBH4•1.5NH3, and NaBF4•2.5NH3 for comparison. It was found that all three ammonia‐based electrolytes in NMBs exhibited stability for sev‐ eral weeks and retained a CE of close to 100% and high cyclability even at a large current of 10 mA cm−2. To compare the electrochemical performance of these solid‐state electro‐ lytes in NMBs, the Cu||Na asymmetric battery in NaI3.3NH3, NaBH4•1.5NH3, and NaBF4•2.5NH3 electrolytes were also measured. A low voltage hysteresis of ±4.5 mV andPDF Image | Electrolyte Engineering for Sodium Metal Batteries
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