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REPORT OF THE BASIC RESEARCH NEEDS WORKSHOP conductivity of ~10-6 S/cm.18 Because its conductivity is relatively low compared to fast-ion conductors (also three orders of magnitude lower than conventional liquid Li-ion electrolytes), it must be made relatively thin (~1 mm), which is easily achievable through thin-film deposition processing. These commercially available batteries demonstrated unprecedented energy density at the cell level, very long cycle life (> 20,000 cycles), and high- rate cycling stability; perhaps most importantly, they showed that the Li metal interface could be successfully stabilized with a solid electrolyte.18 Note, however, that the thin film format employs fabrication techniques (e.g., physical vapor deposition) foreign to conventional, large-scale commercial battery manufacturing, with consequences in material and architectural characteristics that invite a new set of scientific questions. Consequently, fabricating large-format batteries would benefit from the development of solid electrolytes manufactured using traditional bulk-scale synthesis and manufacturing techniques. Presumably, the same or similar processes could be used to fabricate solid-state batteries. Given the myriad properties and manufacturability of solid electrolytes, a series of radar plots can be used to compare the properties of the common material classes, as shown in Figure 3.5.1.8 Three specific classes of materials—sulfides, oxides, and polymers—are discussed below. a. Oxide Ion Reduction selectivity stability Electronic ASR Ionic ASR Device integration Oxidation stability Chemical stability Thermal stability b. Sulfide Ion Reduction selectivity stability Electronic ASR Ionic ASR Device integration Oxidation stability Chemical stability Thermal stability c. Hydride Ion Reduction selectivity stability Electronic Oxidation ASR stability cost d. Halide properties cost e. Thin film properties Electronic ASR Ionic ASR Device integration Oxidation stability Chemical stability Thermal stability Electronic ASR Ionic ASR Device integration Oxidation stability Chemical stability Thermal stability Electronic Oxidation ASR stability Processing Mechanical Processing Mechanical Ion selectivity stability Reduction Processing Mechanical cost properties Processing Mechanical cost properties Reduction Ion selectivity stability Nature Reviews | Materials Figure 3.5.1. Radar plots comparing the properties of several common classes of solid lithium ion conductors. From Ref. 8. Inorganic/Ceramic Solid Electrolytes: The last decade also saw the resurgence in discovery of solid-state electrolyte materials, notably Li-ion-conducting sulfides and oxides. For example, Kamaya et al.21 and Mizuno et al.22 discovered crystalline Li10GeP2S12 and glass Li2S-P2S5, both exhibiting Li-ionic conductivities comparable to liquid electrolytes. Compared to oxides that typically require high temperature densification, the sulfide electrolytes can be densified at room temperature. Recently, Kato et al. demonstrated that bulk-scale solid- state batteries can be fabricated at ambient temperature, with specific energies of several hundred Wh/kg while cycling at relatively high rates for hundreds of cycles.23 A solid-sulfide electrolyte was used owing to its high ionic conductivities and ease of consolidation at ambient temperature under relatively high pressure (> 100 MPa) (Figure 3.5.2).23 Undoubtedly, the ionic conductivities and ease of processing offered by the sulfides mark an important milestone in solid-state battery development. Another important discovery occurred in 2007, when Weppner et al. reported a new oxide bulk-scale Li-ion conductor based on the garnet mineral structure, Li7La3Zr2O12 (aka LLZO).24 When doped with Al or Ta to stabilize the cubic polymorph, LLZO is one of the few bulk-scale electrolytes to simultaneously exhibit stability against metallic Li, fast-ion conductivity, and Li electrode/electrolyte interfacial resistance (at 25°C) comparable to liquid- based cells.24-26 130 PANEL 5 REPORT Ionic ASR Device integration Processing Mechanical cost properties f. Polymer Ion Reduction selectivity stability Chemical stability Thermal stability Ionic ASR Device integration Processing Mechanical cost properties Chemical stability Thermal stabilityPDF Image | Next Generation Electrical Energy Storage
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