Amorphous Chloride Solid Electrolytes with High Li-Ion Conductivity for Stable Cycling of All-Solid-State High-Nickel Cathodes

Unraveling the interfacial compatibility of ultrahigh nickel cathodes and chloride solid electrolyte for stable all-solid-state lithium batteries

“…S4, ESI†). Besides, it should be noted that the intrinsic anti-oxidation instability of chlorides with a potential over 4.43 V, as demonstrated in our recent report, 22 leading to the decomposition of chloride SEs, could also contribute to the increase in internal resistance.…”

“…S11, S12a, b, ESI†). Considering the electrochemical stable window of Li 2 TaCl 7 , which is less than 4.4 V, 22 and the release of high-activity lattice oxygen from the S-NCM92 cathode at high voltage, the observed pronounced change can be correlated to high voltage oxidation-induced degradation. In addition, the signal of TaO x − and ClO − fragments exhibited a similar increasing trend under aging at 4.3, 4.6, and 4.8 V, showing the most significant enhancement of the TaO x − signal (Fig.…”

“…Chloride SEs, such as Li 3 YCl 6 , 14 Li 2 ZrCl 6 , 15 Li 3 ScCl 6 , 16 Li 2 In x Sc 0.666− x Cl 4 , 17 Li 3− x M 1− x Zr x Cl 6 (M = In, Yb), 18,19 LiTaCl 4 O, 20 ZrO 2 –LiCl–Li 2 ZrCl 6 , 21 amorphous Li–Ta–Cl, 22 Li 2.75 (YErYb) 0.16 In 0.25 Zr 0.25 Cl 6 , 23 and Li 5/3 (CrZr) 1/3 Cl 4 24 have recently emerged as the most promising SEs because of their superionic conductivity (ranging from 1 to 12 mS cm −1 , comparable to that of liquid electrolytes), impressive anti-oxidation potential (4.3 V versus Li + /Li), and superior mechanical ductility. These outstanding achievements represent an optimal trade-off between conductivity and electrochemical stability, a balance that has yet to be accomplished in oxide and sulfide SEs.…”

Coprecipitation Strategy for Halide-Based Solid-State Electrolytes and Atmospheric-Dependent In Situ Analysis

“…Furthermore, the X-ray absorption spectroscopy (XAS) technique is employed to determine the locally coordinated environment of the selected ion throughout the bulk material. , The XAS spectra, including the X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectra, of pristine Li 3 InCl 6 and Li 3 InCl 6 exposed to ∼60% relative humidity for 3 min are shown in Figure d–f. Figure d presents the In K -edge XANES spectra of the Li 3 InCl 6 sample.…”

Critical Role of Framework Flexibility and Disorder in Driving High Ionic Conductivity in LiNbOCl4

“…or Li 2 ZrCl 6 have gained popularity as catholytes owing to their favorable mechanical properties and excellent electrochemical oxidation stability. − However, their ionic conductivity does not (yet) surpass that of sulfides. Efforts are being made to enhance conductivity by investigating new compositions and structures through theoretical and experimental approaches. , Recent success has been achieved through the discovery of a few amorphous halides such as LiTaCl 6 , where the exact mechanism of high ionic conductivity is debatable. , …”