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Poly(ethylene oxide) (PEO)-based composite electrolytes (PCEs) are considered as promising candidates for next-generation lithium-metal batteries (LMBs) due to their high safety, easy fabrication, and good electrochemical stability. Here, we utilize operando grazing-incidence small-angle and wide-angle X-ray scattering to probe the correlation of electrochemically induced changes and the buried morphology and crystalline structure of the PCE. Results show that the two irreversible reactions, PEO-Li+ reduction and TFSI- decomposition, cause changes in the crystalline structure, array orientation, and morphology of the PCE. In addition, the reversible Li plating/stripping process alters the inner morphology, especially the PEO-LiTFSI domain radius and distance between PEO-LiTFSI domains, rather than causing crystalline structure and orientation changes. This work provides a new path to monitor a working battery in real time and to a detailed understanding of the Li+ diffusion mechanism, which is essential for developing highly transferable and interface-stable PCE-based LMBs.

Glass and glass-ceramic NASICON-type electrolytes of Li1.5Al0.5Ge1.5(PO4)3 composition were obtained by melt quenching and glass crystallization, respectively. The stability of the solid electrolytes to molten metallic Li was studied by immersing the samples and holding them at 230 °C for 72 h. Li|glass|Li and Li|glass-ceramics|Li electrochemical cells were assembled and their resistance was measured by impedance spectroscopy at 200 °C for 9 days. It was established that, unlike the glass, the glass-ceramics did not change in its phase composition and molecular structure after the tests. It is shown that Li1.5Al0.5Ge1.5(PO4)3 glass-ceramics is chemically stable in contact with metallic Li. © 2019 Elsevier B.V.

In bulk-type all-solid-state lithium batteries with sulfide-based solid electrolytes, composite electrodes, in which an active material, a solid electrolyte, and a conductive additive are mixed, have been used to enhance lithium-ion diffusion and electronic conductivity. However, the addition of electrolytes and electron-conductive additives to the composite electrodes decreases the amount of active materials in the batteries. In the present study, FePS3 was employed as the electrode in an all-solid-state lithium secondary battery, without mixing the solid electrolytes and conductive additives. The all-solid-state cell using the FePS3 electrode exhibited reversible charge-discharge behavior for more than 30 cycles under a constant current density of 0.13 mA cm (2) at room temperature. The discharge capacity of the cell was 107 mAh g (1) at the 30th cycle. This behavior was comparable to that of a cell with an electrode including a solid electrolyte and/or a conductive additive, indicating that the FePS3 electrode had sufficient paths of lithium ions and of electron conduction. These results suggest that FePS3 is an attractive iron-based electrode for an all-solid-state battery using a sulfide-based solid electrolyte. (C) 2017 Elsevier Ltd. All rights reserved.

In bulk-type all-solid-state lithium batteries with sulfide-based solid electrolytes, composite electrodes, in which an active material, a solid electrolyte, and a conductive additive are mixed, have been used to enhance lithium-ion diffusion and electronic conductivity. However, the addition of electrolytes and electron-conductive additives to the composite electrodes decreases the amount of active materials in the batteries. In the present study, FePS3 was employed as the electrode in an all-solid-state lithium secondary battery, without mixing the solid electrolytes and conductive additives. The all-solid-state cell using the FePS3 electrode exhibited reversible charge-discharge behavior for more than 30 cycles under a constant current density of 0.13 mA cm (2) at room temperature. The discharge capacity of the cell was 107 mAh g (1) at the 30th cycle. This behavior was comparable to that of a cell with an electrode including a solid electrolyte and/or a conductive additive, indicating that the FePS3 electrode had sufficient paths of lithium ions and of electron conduction. These results suggest that FePS3 is an attractive iron-based electrode for an all-solid-state battery using a sulfide-based solid electrolyte. (C) 2017 Elsevier Ltd. All rights reserved.