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Batteries 2022, 8, 157 18 of 25 battery delivered high discharge capacities with excellent coulombic efficiency as well as stable cycling performance [123]. In addition, soft breakdown phenomena in all-solid-state symmetric batteries were pretty common because of the high electronic conductivity of solid-state electrolytes, poor interfacial solid–solid ionic contact, and uneven localized electric field. However, soft breakdown hidden in all-solid-state NMBs had been overlooked in most previous research. This abnormal phenomenom had significantly retarded the progress of improving Na metal anodes for practical engineering of all-solid-state NMBs. Sun et al. proposed a simple but effective strategy—cyclic voltammetry (CV)—to diagnose soft breakdown in all-solid-state symmetric batteries [127]. The charge carrier of an all-solid-state symmetric battery should be only ions. If an all-solid-state symmetric cell had both ion and electron transport, it was a soft breakdown. For all-solid-state symmetric batteries with soft breakdown, CV would show a mixed state of both electrochemical process and electronic conduction. Therefore, CV was a simple but effective method to diagnose the soft breakdown phenomenon in all-solid-state symmetric NMBs. It was necessary for all-solid-state NMBs to avoid arbitrary testing parameters and ignorance of soft breakdown in the future. Based on the above discussion, we summarized the electrochemical properties of mod- ified all-solid-state electrolytes for NMBs and listed some important parameters including ionic conductivity, and cycling stability of recent works, as shown in Table 3. Table 3. Electrochemical properties of different all-solid-state electrolytes in NMBs. All-Solid-State Electrolytes Na-β”-Al2 O3 BASE-CNT YSZ/BASE Sn-BASE G-NASICON NZSP-PPC-PEO NZSP/PVDF-HFP NZSP/PPE PEO-NaClO4-SiO2-Emim FSI NZSP-Na2 B4 O7 TiO2 -NZSP Ca-NZSP SnOx /Sn/NZSP SnS2 /NZSP ANs-GPE NZSP AlF3 /NZSP H-NASICON Ionic Conductivity (mS cm−1)@Temperature (◦C) 2.1@RT 0.36@58 0.46@RT 1.1@60 0.6@RT 0.12@RT 0.132@60 0.693@25 1.3@RT 1.72@RT 0.53@25 1.67@25 0.59@RT 0.42@RT 0.713@25 0.85@RT 0.2415@RT 0.07@65 Symmetrical Cell (Cycle Performance (h)@Current Density (mA cm−2)) / 1000@0.1 330@0.5 1000@0.5 1000@0.5 1000@0.1 400@0.2 200@0.05 / 2500@0.3 860@0.1 600@0.3 1500@0.1 800@0.1 300@1 1000@0.2 150@0.15 550@0.25 Full Cell (Cathode@Capacity (mAh g−1)@Current Density (C)) / Na3 V2 (PO4 )3 @100.6@0.1 O3- NaNi0.45 Cu0.05 Mn0.4 Ti0.1 O2 @110@1 PTO-PEO@180@0.5 Na3 V2 (PO4 )3 @108@1 Na3 V2 (PO4 )3 @102@1 Na3 V2 (PO4 )3 @95@0.2 Na0.67 Ni0.33 Mn0.67 O2 @112@0.1 Y-Na2 O3 Zr/C@90.5@0.05 Na3V1.5Cr0.5(PO4)3@107@30 mA g−1 Na3 V2 (PO4 )3 @103.1@0.2 NaTi2 (PO4 )3 @96.4@0.2 Na3 V2 (PO4 )3 @101.2@0.5 Na3 V2 (PO4 )3 @85.5@5 Na3 V1.5 Cr0.5 (PO4 )3 @114.6@0.2 Na3 V2 (PO4 )3 @111@1 NaTi2 (PO4 )3 @110@0.2 References [110] [111] [112] [113] [115] [52] [116] [117] [128] [118] [129] [130] [119] [120] [114] [121] [131] [96] Considering the practical application of NMBs in the future, NMBs design should not be limited to coin batteries. Currently, three major cell formats are commercially used: cylindrical, prismatic, and pouch. Among them, the pouch cells based on layered constructions allow maximum use of space and active materials and therefore are popular for large cell formats [132]. However, the excessive capacities and thicknesses of the available Na metal foils remain a critical yet unresolved challenge in practical pouch cells. Practical Na metal pouch cells require a ultra-thin Na metal foil paired with the conventional cathode to satisfy a lower negative to positive areal capacity (N/P) ratio [133]. The existing technology cannot satisfy the requirements of ultra-thin sodium metal anodes. Thus, the side reactions in the pouch cells with a high excess of Na may be intensified. New manufacturing capabilities will be needed to control the thickness of the Na metal anodes in the future. In addition, a higher CE close to 100% could be enabled by an electrolyte that produces a more stable SEI and fewer side reactions, or by an anode that allows aPDF Image | Recent Development for Sodium Metal Batteries
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