Ion transport limitations in all-solid-state lithium battery electrodes containing a sulfide-based electrolyte

Kaiser, Nico; Spannenberger, Stefan; Schmitt, Markus; Cronau, Marvin; Kato, Yoshifumi; Roling, Bernhard

doi:10.1016/j.jpowsour.2018.05.095

Cited by 78 publications

(110 citation statements)

References 21 publications

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“…The gradient of lithiation is due to the energy loss of ionic transport in solid electrolyte across the electrode (ohmic limit). Under this condition, the battery performance can be improved by electrode engineering such as (i) increasing the ionic conductivity of the solid electrolyte, (ii) designing the tortuosity factor for ion transport, and/or (iii) find a comprise between energy/power and thickness of the WE …”

Section: Resultsmentioning

confidence: 99%

Operando Visualization of Morphological Dynamics in All‐Solid‐State Batteries

Billaud

Jerjen

et al. 2019

Advanced Energy Materials

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materials generates volume changes. [2,3] In conventional lithium-ion batteries (LiBs) employing liquid electrolytes, volume expansion dissipates in the electrode matrix (carbon/binder) and depends only on the intrinsic properties of the active material. [4,5] The mechanical fracture of the active material particles and mechanical disintegration of the electrode might be even more severe for all-solid-state batteries (SSBs) as the battery needs to maintain its mechanical integrity for proper cycling.Research in the field of SSBs is motivated by their promised high power and energy density on the cell level compared to conventional LiBs. [6] In particular, inorganic glassy and ceramic solid electrolyte (SE), for example, the thio-LiSICON family [6][7][8] and garnet-type (Li 5 La 3 M 2 O 12 ) conductors, [9] with high room-temperature ionic conductivity up to 10 mS cm −1 , moved the performance of SSBs close to and beyond that of the state-of-the-art LiB. [6] Among all superionic conductors, amorphous Li 2 S-P 2 S 5 (LPS) stands out due to its low Young's modulus (E = 18.5 GPa) [10] and its ability to be well densified by cold pressing. [11] Theoretically, the elasticity of LPS is beneficial for accommodating the stress caused by the volume change of the active material during cycling. However, All-solid-state batteries (SSBs) are considered as attractive options for next-generation energy storage owing to the favorable properties (unit transference number and thermal stabilities) of solid electrolytes. However, there are also serious concerns about mechanical deformation of solid electrolytes leading to the degradation of the battery performance. Therefore, understanding the mechanism underlying the electromechanical properties in SSBs is essentially important. Here, 3D and time-resolved measurements of an all-solid-state cell using synchrotron radiation X-ray tomographic microscopy are shown. The gradient of the electrochemical reaction and the morphological evolution in the composite layer can be clearly observed. Volume expansion/compression of the active material (Sn) is strongly oriented along the thickness of the electrode. While this results in significant deformation (cracking) in the solid electrolyte region, organized cracking patterns depending on the particle size and their arrangements is also found. This study based on operando visualization therefore opens the door toward rational design of particles and electrode morphology for all-solid-state batteries. BatteriesThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.

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Section: Resultsmentioning

confidence: 99%

Operando Visualization of Morphological Dynamics in All‐Solid‐State Batteries

Billaud

Jerjen

et al. 2019

Advanced Energy Materials

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“…The loading level of each composite electrode was controlled at 15.2 mg/cm 2 , and the corresponding composite thickness was ~63 μm. As shown in Figure B, these samples did not show any charge transfer reaction, so the approximation without Faradaic reactions can be used to describe our composite electrode . The three samples with mixing conditions of 300, 650, and 1000 rpm exhibited similar profiles, but the other samples were different.…”

Section: Resultsmentioning

confidence: 94%

“…To determine the ionic transport properties of the composite electrodes, composite symmetric cells were used (Figure A). In a full‐cell configuration with different anodes and cathodes, the impedance can be measured, but in this case, the reaction complexity of individual electrodes generally makes precise analysis difficult . To circumvent this issue, symmetric cells with identical electrodes at each end of the solid electrolyte layer can be used.…”

Section: Resultsmentioning

confidence: 99%

“…According to the transmission line model (TLM) without Faradaic reactions, the impedance of the composite electrode in the composite symmetric cell, Z composite , is given by

Z_{composite} = R_{electrolyte} + \sqrt{\frac{R_{ion}}{i ω C_{dl}}} \coth \sqrt{R_{ion} i ω C_{dl}},

where ω is the angular frequency, R electrolyte is the bulk ion transport resistance of the middle solid electrolyte layer, R ion is the total ion transport resistance within the composite electrodes, and C dl is the total double‐layer capacitance at the interface between the active material and the solid electrolyte. The capacitances can be replaced by constant phase elements.…”

Section: Resultsmentioning

confidence: 99%

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Efficient cell design and fabrication of concentration‐gradient composite electrodes for high‐power and high‐energy‐density all‐solid‐state batteries

et al. 2019

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All‐solid‐state batteries are promising energy storage devices in which high‐energy‐density and superior safety can be obtained by efficient cell design and the use of nonflammable solid electrolytes, respectively. This paper presents a systematic study of experimental factors that affect the electrochemical performance of all‐solid‐state batteries. The morphological changes in composite electrodes fabricated using different mixing speeds are carefully observed, and the corresponding electrochemical performances are evaluated in symmetric cell and half‐cell configurations. We also investigate the effect of the composite electrode thickness at different charge/discharge rates for the realization of all‐solid‐state batteries with high‐energy‐density. The results of this investigation confirm a consistent relationship between the cell capacity and the ionic resistance within the composite electrodes. Finally, a concentration‐gradient composite electrode design is presented for enhanced power density in thick composite electrodes; it provides a promising route to improving the cell performance simply by composite electrode design.

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“…The electrode was prepared by mortar hand mixing of TiS 2 with the solid electrolyte (SE) in the TiS 2 :SE ratio 30:70 wt.%. For both active materials, the electrolyte volume fraction was set around 0.8, ensuring that the ion transport pathways would not be a limiting factor in these composite electrodes [ 28 ].…”

Section: Methodsmentioning

confidence: 99%

Solid-State Li-Ion Batteries Operating at Room Temperature Using New Borohydride Argyrodite Electrolytes

et al. 2020

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Using a new class of (BH4)− substituted argyrodite Li6PS5Z0.83(BH4)0.17, (Z = Cl, I) solid electrolyte, Li-metal solid-state batteries operating at room temperature have been developed. The cells were made by combining the modified argyrodite with an In-Li anode and two types of cathode: an oxide, LixMO2 (M = ⅓ Ni, ⅓ Mn, ⅓ Co; so called NMC) and a titanium disulfide, TiS2. The performance of the cells was evaluated through galvanostatic cycling and Alternating Current AC electrochemical impedance measurements. Reversible capacities were observed for both cathodes for at least tens of cycles. However, the high-voltage oxide cathode cell shows lower reversible capacity and larger fading upon cycling than the sulfide one. The AC impedance measurements revealed an increasing interfacial resistance at the cathode side for the oxide cathode inducing the capacity fading. This resistance was attributed to the intrinsic poor conductivity of NMC and interfacial reactions between the oxide material and the argyrodite electrolyte. On the contrary, the low interfacial resistance of the TiS2 cell during cycling evidences a better chemical compatibility between this active material and substituted argyrodites, allowing full cycling of the cathode material, 240 mAhg−1, for at least 35 cycles with a coulombic efficiency above 97%.

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Ion transport limitations in all-solid-state lithium battery electrodes containing a sulfide-based electrolyte

Cited by 78 publications

References 21 publications

Operando Visualization of Morphological Dynamics in All‐Solid‐State Batteries

Operando Visualization of Morphological Dynamics in All‐Solid‐State Batteries

Efficient cell design and fabrication of concentration‐gradient composite electrodes for high‐power and high‐energy‐density all‐solid‐state batteries

Solid-State Li-Ion Batteries Operating at Room Temperature Using New Borohydride Argyrodite Electrolytes

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