“…Recently, a solid electrolyte in which LiBH 4 was dispersed in a Li 2 S-P 2 S 5 glass matrix, realized a high lithium-ionic conductivity of log(σ/S cm −1 ) = −2.8 at 298 K. 28) In addition, the crystalline phase of 90LiBH 4 -10P 2 S 5 , with a nominal composition, exhibited a lithium-ionic conductivity of log(σ/S cm −1 ) = −3.0 at 300 K. 29) These materials do not include a phase transition, as seen in LiBH 4 , at least above room temperature; hence, the assembly of batteries that allowed for room temperature operation was possible. In other reports, high lithium [30][31][32][33] and sodium 30,[32][33][34][35] , have been discovered.…”
We have operated a 4V-class bulk-type, all-solid-state LiCoO 2 /Li battery at room temperature. The battery consisted of a Li 4 (BH 4 ) 3 I complex hydride electrolyte as the electrolyte layer, and a 80Li 2 S 20P 2 S 5 sul de glass as an electrolyte in the positive electrode layer. The assembled battery exhibited a 92 mAh g −1 initial discharge capacity at 298 K and 0.1 C. The discharge capacity for the 20 th cycle remained as high as 83 mAh g −1 , corresponding to a capacity retention ratio of nearly 90%.
“…Recently, a solid electrolyte in which LiBH 4 was dispersed in a Li 2 S-P 2 S 5 glass matrix, realized a high lithium-ionic conductivity of log(σ/S cm −1 ) = −2.8 at 298 K. 28) In addition, the crystalline phase of 90LiBH 4 -10P 2 S 5 , with a nominal composition, exhibited a lithium-ionic conductivity of log(σ/S cm −1 ) = −3.0 at 300 K. 29) These materials do not include a phase transition, as seen in LiBH 4 , at least above room temperature; hence, the assembly of batteries that allowed for room temperature operation was possible. In other reports, high lithium [30][31][32][33] and sodium 30,[32][33][34][35] , have been discovered.…”
We have operated a 4V-class bulk-type, all-solid-state LiCoO 2 /Li battery at room temperature. The battery consisted of a Li 4 (BH 4 ) 3 I complex hydride electrolyte as the electrolyte layer, and a 80Li 2 S 20P 2 S 5 sul de glass as an electrolyte in the positive electrode layer. The assembled battery exhibited a 92 mAh g −1 initial discharge capacity at 298 K and 0.1 C. The discharge capacity for the 20 th cycle remained as high as 83 mAh g −1 , corresponding to a capacity retention ratio of nearly 90%.
“…Recent interest in utilizing LiBH 4 as a solid-state electrolyte was established through the work of Orimo [4], who demonstrated that the ionic conductivity of lithium can be greater than 1 mS/cm at temperatures above the orthorhombic to hexagonal phase transition that occurs at 380 K [5]. This work has been expanded to achieve high conductivity in LiBH 4 based solid electrolytes through the addition of Li halide salts [6][7][8], nanoconfinement [9][10][11][12], nanoionic destabilization [13,14], ion substitution [15][16][17][18][19][20][21], and eutectic formation [22].…”
Abstract:In this study, we analyze and compare the physical and electrochemical properties of an all solid-state cell utilizing LiBH 4 as the electrolyte and aluminum as the active anode material. The system was characterized by galvanostatic lithiation/delithiation, cyclic voltammetry (CV), X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDS), Raman spectroscopy, electrochemical impedance spectroscopy (EIS), and scanning electron microscopy (SEM). Constant current cycling demonstrated that the aluminum anode can be reversibly lithiated over multiple cycles utilizing a solid-state electrolyte. An initial capacity of 895 mAh/g was observed and is close to the theoretical capacity of aluminum. Cyclic voltammetry of the cell was consistent with the constant current cycling data and showed that the reversible lithiation/delithiation of aluminum occurs at 0.32 V and 0.38 V (vs. Li + /Li) respectively. XRD of the aluminum anode in the initial and lithiated state clearly showed the formation of a LiAl (1:1) alloy. SEM-EDS was utilized to examine the morphological changes that occur within the electrode during cycling. This work is the first example of reversible lithiation of aluminum in a solid-state cell and further emphasizes the robust nature of the LiBH 4 electrolyte. This demonstrates the possibility of utilizing other high capacity anode materials with a LiBH 4 based solid electrolyte in all-solid-state batteries.
“…Argyrodite-type crystals with the stoichiometry Li 6 PS 5 X (X = Cl, Br, or I) also have high ionic conductivity (>10 −3 S/cm) (Deiseroth et al, 2008;Rao and Adams, 2011;Boulineau et al, 2012). In addition, the conductivities of some glasses, including 30Li 2 S-26B 2 S 3 -44LiI (Wada et al, 1983), 50Li 2 S-17P 2 S 5 -33LiBH 4 (Yamauchi et al, 2013), and 63Li 2 S-36SiS 2 -1Li 3 PO 4 (Aotani et al, 1994), have been reported to be as high as 1.5-1.7 × 10 −3 S/cm. The focus of this study was on the binary Li 2 S-P 2 S 5 system.…”
Lithium thiophosphate-based materials are attractive as solid electrolytes in all-solidstate lithium batteries because glass or glass-ceramic structures of these materials are associated with very high conductivity. In this work, we modeled lithium thiophosphates with amorphous structures and investigated Li + mobilities by using molecular dynamics calculations based on density functional theory (DFT-MD). The structures of xLi 2 S-(100 − x)P 2 S 5 (x = 67, 70, 75, and 80) were created by randomly identifying appropriate compositions of Li + , PS The implication is that these amorphous structures are metastable. There was good agreement between calculated and experimental structure factors determined from X-ray scattering. The differences between the structure factors of amorphous structures were small, except for the first sharp diffraction peak, which was affected by the environment between Li and S atoms. Li + diffusion coefficients obtained from DFT-MD calculations at various temperatures for picosecond simulation times were on the order of 10 −3 -10 −5 Å 2 /ps. Ionic conductivities evaluated by the Nernst-Einstein relationship at 298.15 K were on the order of 10 −5 S/cm. The ionic conductivity of the amorphous structure with x = 75 was the highest among the amorphous structures because there was a balance between the number density and diffusibility of Li + . The simulations also suggested that isolated S atoms suppress Li + migration.
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