Versatility of Sb-doping enabling argyrodite electrolyte with superior moisture stability and Li metal compatibility towards practical all-solid-state Li metal batteries

Li-argyrodite solid-state electrolytes with lithium compatibility and air stability for all-solid-state batteries

“…It has been shown that the presence of such impurity phases severely affects ion transport in the electrolyte. 36,38 The peaks at 2 θ ≈ 18° were assigned to Kapton tape and were masked by the tape due to the low intensity of the two peaks at 15°–20°, which was confirmed by XRD Rietveld refinement of the maps (Fig. 1e, S1†).…”

“…S8b†), indicating the decomposition of the electrolyte structure under the effect of moisture. 36 However, no significant changes were observed in the Raman spectrum of the Li 6.05 P 0.95 Zr 0.05 S 4.9 O 0.1 Cl electrolyte exposed to wet air. This confirmed that the structure of the ZrO 2 -doped Li 6.05 P 0.95 Zr 0.05 S 4.9 O 0.1 Cl electrolyte was not disrupted.…”

“…After this, the value of CCD started to decrease gradually with the increase in doping amount, which may be related to the large decrease in ionic conductivity. 36,50 It is noteworthy that the CCD (Fig. S14a and b†) of Li 6+ x P 1− x Zr x S 5−2 x O 2 x Cl ( x = 0.01, 0.03) were both higher than that of pristine Li 6 PS 5 Cl, but the ionic conductivity lacks of both were lower than that of Li 6 PS 5 Cl.…”

“…32 Therefore, acids with softer central atoms (In 3+ , Bi 3+ , Sn 4+ , Sb 5+ , etc. ) can be chosen to partially replace the strong acid P 5+ in order to design Li-argyrodite-type SSEs with higher air stability, 33–36 since the soft acid prefers to combine with the soft base S rather than the hard base O. More importantly, this large-size soft acid substitution will increase the cell volume, thus promoting ion transport.…”

Enhanced Air Stability and Li Metal Compatibility of Li‐Argyrodite Electrolytes Triggered by In2O3 Co‐Doping for All‐Solid‐State Li Metal Batteries

“…Only four characteristic peaks belonging to PS 4 3− unit is observed at ≈197, 272, 418, and 564 cm −1 for five electrolytes. [19] Furthermore, no other groups (such as InS 4 5− and PS 3 O 4− ) are detected at the detection limit of the Raman spectrum. In addition, the low-speed scanning XRD patterns and Rietveld refinement of Li 6 PS 5 Cl and Li 6.16 P 0.92 In 0.08 S 4.88 O 0.12 Cl electrolytes were tested to illustrate the crystal phase changes caused by the doping of In 2 O 3 in detail (Figure 1e,f).…”