Phase formation of a garnet-type lithium-ion conductor Li7−3Al La3Zr2O12

Matsuda, Yasuaki; Sakamoto, K.; Matsui, Masaki; Yamamoto, Osamu; Takeda, Yasuo; Imanishi, Nobuyuki

doi:10.1016/j.ssi.2015.04.011

Cited by 67 publications

(49 citation statements)

References 28 publications

(51 reference statements)

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“…In this specific case a bulk conductivity of 3.3 × 10 −4 S cm −1 results. This is within the range typically found for such LLZO samples stabilized with aluminium [8,13,[27][28][29][30][31]. However, literature data reveal a large scattering of bulk or total conductivities, and in a separate paper we will show that a substantial variation also exists between numerous nominally identical samples prepared in our labs.…”

Section: Macroelectrode Measurementssupporting

confidence: 80%

Microelectrodes for local conductivity and degradation measurements on Al stabilized Li7La3Zr2O12 garnets

et al. 2016

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The attractiveness of Li 7 La 3 Zr 2 O 12 (LLZO) cubic based garnets lies in their high ionic conductivity and the combination of thermal and electrochemical stability. However, relations between composition and conductivity as well as degradation effects are still not completely understood.In this contribution we demonstrate the applicability of microelectrodes (Ø = 20-300 μm) for electrochemical impedance spectroscopy (EIS) studies on LLZO garnets. Microelectrodes allow to obtain local information on the ionic conductivity. A comparison between the overall performance of the sample (3.3 × 10 −4 S cm −1 ) and local measurements revealed differences in conductivity with a maximum of the locally measured values of 6.3 × 10 −4 S cm −1 and a minimum of 2.6 × 10 −4 S cm −1 . One reason behind these conductivity variations is most probably a compositional gradient in the sample. In addition, microelectrodes are very sensitive to conductivity changes near to the surface. This was used to investigate the effect of moisture in ambient air on the conductivity variations of LLZO. Substantial changes of the measured Li-ion transport resistance were found, particularly for smaller microelectrodes which probe sample volumes close to the surface.

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Section: Macroelectrode Measurementssupporting

confidence: 80%

Microelectrodes for local conductivity and degradation measurements on Al stabilized Li7La3Zr2O12 garnets

et al. 2016

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“…In the literature, a wide variety of transition temperatures ranging from 373 to 923 K was reported. [45][46][47][48][49] Literature results and our previous work suggest that such variation could be attributed to intentional or inadvertent impurity (e.g. Al)/dopant incorporation, H2O or CO2 exposure, all of which reduces the transition temperature.…”

Section: Phase Characterizationmentioning

confidence: 91%

“…Al)/dopant incorporation, H2O or CO2 exposure, all of which reduces the transition temperature. 45,49,50 Thus we chose experimental data with the highest transition temperatures, i.e. works of Larraz et al 47 and…”

Section: Phase Characterizationmentioning

confidence: 99%

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Finite-size effects on the molecular dynamics simulation of fast-ion conductors: A case study of lithium garnet oxide Li7La3Zr2O12

Klenk

Lai

2016

Solid State Ionics

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A useful tool to study ionic conduction mechanisms in fast-ion conductors is the molecular dynamics (MD) simulation performed on finite simulation cells with periodic boundary conditions. While there have been many studies of the effect of cell size on the thermodynamics and kinetics of simple liquids, the finite-size effect in fast-ion conductors remains elusive. This work presents a case study to investigate the finite-size effect on the phase transition, self-diffusivity, ionic conductivity, Haven ratio, thermodynamic factor, and Fickian diffusivity using lithium garnet oxide Li7La3Zr2O12 as a model material. It was found that cell sizes influence extracted thermodynamic and kinetic characteristics in different ways with magnitude ranging from weak to strong. For Li7La3Zr2O12, reliable properties can be obtained with a 3×3×3 (5184 atoms) cell.

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“…The Al 3+ substitution of Li + sites in LLZ (Al-doping) is an effective way to improve the stability of cubic phase at room temperature. For example, Li6.25Al0.25La3Zr2O12 (x = 0.25 in Li7-3xAlxLa3Zr2O12) has been known as a stable cubic LLZ (Matsuda et al, 2015). These kinds of Al-doped LLZs are usually denoted as LLZAls and show a relatively high bulk ionic conductivity such as 3.1 × 10 −4 S cm −1 at 25°C in Li6.25Al0.25La3 Zr2O12.…”

mentioning

confidence: 99%

Fabrication of All-Solid-State Lithium-Ion Cells Using Three-Dimensionally Structured Solid Electrolyte Li7La3Zr2O12 Pellets

2016

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All-solid-state lithium-ion batteries using Li + -ion conducting ceramic electrolytes have been focused on as attractive future batteries for electric vehicles and renewable energy conversion systems because high safety can be realized due to non-flammability of ceramic electrolytes. In addition, a higher volumetric energy density than that of current lithium-ion batteries is expected since the all-solid-state lithium-ion batteries can be made in bipolar cell configurations. However, the special ideas and techniques based on ceramic processing are required to construct the electrochemical interface for all-solidstate lithium-ion batteries since the battery development has been done so far based on liquid electrolyte system over 100 years. As one of the promising approaches to develop practical all-solid-state batteries, we have been focusing on three-dimensionally (3D) structured cell configurations such as an interdigitated combination of 3D pillars of cathode and anode, which can be realized by using solid electrolyte membranes with hole-array structures. The application of such kinds of 3D structures effectively increases the interface between solid electrode and solid electrolyte per unit volume, lowering the internal resistance of all-solid-state lithium-ion batteries. In this study, Li6.25Al0.25La3Zr2O12 (LLZAl), which is a Al-doped Li7La3Zr2O12 (LLZ) with Li + -ion conductivity of ~10 -4 S ⋅cm −1 at room temperature and high stability against lithium-metal, was used as a solid electrolyte, and its pellets with 700 μm depth holes in 700 μm × 700 μm area were fabricated to construct 3D-structured all-solid-state batteries with LiCoO2/LLZAl/lithium-metal configuration. It is expected that the LiCoO2-LLZAl interface is formed by point-to-point contact even when the LLZAl pellet with 3D hole-array structure is applied. Therefore, Li3BO3, which is a mechanically soft solid electrolyte with a low melting point at around 700°C was also applied as a supporting Li + -ion conductor to improve the LiCoO2-LLZAl interface.

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Phase formation of a garnet-type lithium-ion conductor Li7−3Al La3Zr2O12

Cited by 67 publications

References 28 publications

Microelectrodes for local conductivity and degradation measurements on Al stabilized Li7La3Zr2O12 garnets

Microelectrodes for local conductivity and degradation measurements on Al stabilized Li7La3Zr2O12 garnets

Finite-size effects on the molecular dynamics simulation of fast-ion conductors: A case study of lithium garnet oxide Li7La3Zr2O12

Fabrication of All-Solid-State Lithium-Ion Cells Using Three-Dimensionally Structured Solid Electrolyte Li7La3Zr2O12 Pellets

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