Redox-active cathode interphases in solid-state batteries

2017 ◽  
Vol 5 (43) ◽  
pp. 22750-22760 ◽  
Author(s):  
Raimund Koerver ◽  
Felix Walther ◽  
Isabel Aygün ◽  
Joachim Sann ◽  
Christian Dietrich ◽  
...  

In situ X-ray photoelectron spectroscopy shows the redox-active chemistry of β-Li3PS4 at the cathode interface in a solid-state battery.

2020 ◽  
Author(s):  
John Lewis ◽  
Francisco Javier Quintero Cortes ◽  
Yuhgene Liu ◽  
John C. Miers ◽  
Ankit Verma ◽  
...  

<p>Despite progress in solid-state battery engineering, our understanding of the chemo-mechanical phenomena that govern electrochemical behavior and stability at solid-solid interfaces remains limited compared to solid-liquid interfaces. Here, we use <i>operando</i> synchrotron X-ray computed microtomography to investigate the evolution of lithium/solid-state electrolyte interfaces during battery cycling, revealing how the complex interplay between void formation, interphase growth, and volumetric changes determines cell behavior. Void formation during lithium stripping is directly visualized in symmetric cells, and the loss of contact at the interface between lithium and the solid-state electrolyte (Li<sub>10</sub>SnP<sub>2</sub>S<sub>12</sub>) is found to be the primary cause of cell failure. Reductive interphase formation within the solid-state electrolyte is simultaneously observed, and image segmentation reveals that the interphase is redox-active upon charge. At the cell level, we postulate that global volume changes and loss of stack pressure occur due to partial molar volume mismatches at either electrode. These results provide new insight into how chemo-mechanical phenomena can impact cell performance, which is necessary to understand for the development of solid-state batteries.</p>


Author(s):  
K. Ganesh Kumar ◽  
P. Balaji Bhargav ◽  
C. Balaji ◽  
Ahmed Nafis ◽  
K. Aravinth ◽  
...  

Abstract Owing to high lithium ion conductivity and good stability with lithium metal, Li7La3Zr2O12 (LLZO—a solid electrolyte) has emerged as a viable candidate for solid-state battery applications. In the current study, Al-substituted LLZO (Al-LLZO) powder is synthesized using a typical solid-state reaction. The pellets are made with the synthesized powder and are subjected to annealing for different durations and its effect on the structural properties of the Al-LLZO is investigated in detail. Reitveld refinement of the powder X-ray diffraction pattern reveals that the sintered Al-LLZO belong to the cubic system with the Ia-3d space group at room temperature. Morphology and microstructural properties of sintered powder are analyzed using field emission scanning electron microscopy (FESEM) and high-resolution transmission electron microscopy (HRTEM)/selected area electron diffraction (SAED), respectively. The FESEM image of LLZO pellets shows well-structured cubic grains spread evenly over on the surface after sintering. The chemical compositions of the sample are identified using energy dispersive X-ray analysis (EDAX). The surface chemistry of the prepared samples is examined by X-ray photoelectron spectroscopy (XPS), which states that the observed photoelectron signals from O 1s at about 531 eV and Li1s at 54.52 eV correspond to the Li-O bond in Al-LLZO. Raman spectra have been analyzed and the observed Raman peaks appearing at 299 cm−1, 393 cm−1, 492 cm−1, and 514 cm−1 were assigned to Eg, F2g, A1g, and F2g, respectively. Phase transformation from C-LLZO to the pyrochore LZO phase is noticed when the sample is sintered for 12 h at 1100 °C. The impedance analysis is carried out to measure the conductivity of the Al-LLZO pellet and is found to be 0.3 × 10−5 S cm−1, which is suitable for solid electrolyte applications in lithium ion batteries.


2019 ◽  
Vol 123 (16) ◽  
pp. 10487-10493 ◽  
Author(s):  
Takashi Tsuchiya ◽  
Yaomi Itoh ◽  
Yoshikazu Yamaoka ◽  
Shigenori Ueda ◽  
Yukihiro Kaneko ◽  
...  

2020 ◽  
Author(s):  
John Lewis ◽  
Francisco Javier Quintero Cortes ◽  
Yuhgene Liu ◽  
John C. Miers ◽  
Ankit Verma ◽  
...  

<p>Despite progress in solid-state battery engineering, our understanding of the chemo-mechanical phenomena that govern electrochemical behavior and stability at solid-solid interfaces remains limited compared to solid-liquid interfaces. Here, we use <i>operando</i> synchrotron X-ray computed microtomography to investigate the evolution of lithium/solid-state electrolyte interfaces during battery cycling, revealing how the complex interplay between void formation, interphase growth, and volumetric changes determines cell behavior. Void formation during lithium stripping is directly visualized in symmetric cells, and the loss of contact at the interface between lithium and the solid-state electrolyte (Li<sub>10</sub>SnP<sub>2</sub>S<sub>12</sub>) is found to be the primary cause of cell failure. Reductive interphase formation within the solid-state electrolyte is simultaneously observed, and image segmentation reveals that the interphase is redox-active upon charge. At the cell level, we postulate that global volume changes and loss of stack pressure occur due to partial molar volume mismatches at either electrode. These results provide new insight into how chemo-mechanical phenomena can impact cell performance, which is necessary to understand for the development of solid-state batteries.</p>


Sign in / Sign up

Export Citation Format

Share Document