Separation of the bulk and grain boundary contributions to the total conductivity of solid lithium-ion conducting electrolytes

Braun, Philipp; Uhlmann, Christian; Weber, André; Störmer, Heike; Gerthsen, D.; Ivers-Tiffée, Ellen

doi:10.1007/s10832-016-0061-y

Cited by 43 publications

(32 citation statements)

References 20 publications

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“…The intercept at high frequency reflects ohmic resistance, whereas the diameters of the semicircles at medium and low frequency reflect the ionic grain boundary transportation resistance and charge-transfer resistance, respectively [37,38]. An equivalent circuit mode LR Ω (R a Z a )((R b Z b )(R c Z c ) (Figure 7b) is still employed to fit the EIS data.…”

Section: Resultsmentioning

confidence: 99%

Semiconductor-Ionic Nanocomposite La0.1Sr0.9MnO3−δ-Ce0.8Sm0.2O2−δ Functional Layer for High Performance Low Temperature SOFC

Wang

et al. 2018

Materials

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A novel composite was synthesized by mixing La0.1Sr0.9MnO3−δ (LSM) with Ce0.8Sm0.2O2−δ (SDC) for the functional layer of low temperature solid oxide fuel cell (LT-SOFC). Though LSM, a highly electronic conducting semiconductor, was used in the functional layer, the fuel cell device could reach OCVs higher than 1.0 V without short-circuit problem. A typical diode or rectification effect was observed when an external electric force was supplied on the device under fuel cell atmosphere, which indicated the existence of a junction that prevented the device from short-circuit problem. The optimum ratio of LSM:SDC = 1:2 was found for the LT-SOFC to reach the highest power density of 742 mW·cm−2 under 550 °C The electrochemical impedance spectroscopy data highlighted that introducing LSM into SDC electrolyte layer not only decreased charge-transfer resistances from 0.66 Ω·cm2 for SDC to 0.47–0.49 Ω·cm2 for LSM-SDC composite, but also decreased the activation energy of ionic conduction from 0.55 to 0.20 eV.

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Section: Resultsmentioning

confidence: 99%

Semiconductor-Ionic Nanocomposite La0.1Sr0.9MnO3−δ-Ce0.8Sm0.2O2−δ Functional Layer for High Performance Low Temperature SOFC

Wang

et al. 2018

Materials

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“…grain interior) and grain boundary conductivities. Typically, the ionic conductivities are measured by impedance spectroscopy over a wide frequency range to resolve their various contributions, whereas the bulk and grain boundary conductivities are verified by adequate equivalent-circuit models [ 2 , 3 ]. Lilley et al and Breuer et al reported that at temperatures well below room temperature (~173 K) the bulk conductivity contributions are easily separated from the grain boundary response [ 2 , 4 ].…”

Section: Introductionmentioning

confidence: 99%

“…An example is the tetragonal–cubic transition in sintered Li 7 La 3 Zr 2 O 12 [ 16 , 17 ]. Microstructures such as the secondary phase, grain size distribution and short-circuited grain boundaries [ 2 ] are thought to cause inhomogeneous conduction paths of the grain boundaries across polycrystalline samples, which explicitly depend on the experimental conditions such as the sintering temperature [ 3 ]. Meanwhile, additives affect the sintered density and suppress the secondary phases by tuning the additive content, thus changing the ionic conductivities [ 18 ].…”

Section: Introductionmentioning

confidence: 99%

Essential structural and experimental descriptors for bulk and grain boundary conductivities of Li solid electrolytes

Tanaka

Komori

et al. 2020

Science and Technology of Advanced Materials

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We present a computational approach for identifying the important descriptors of the ionic conductivities of lithium solid electrolytes. Our approach discriminates the factors of both bulk and grain boundary conductivities, which have been rarely reported. The effects of the interrelated structural (e.g. grain size, phase), material (e.g. Li ratio), chemical (e.g. electronegativity, polarizability) and experimental (e.g. sintering temperature, synthesis method) properties on the bulk and grain boundary conductivities are investigated via machine learning. The data are trained using the bulk and grain boundary conductivities of Li solid conductors at room temperature. The important descriptors are elucidated by their feature importance and predictive performances, as determined by a nonlinear XGBoost algorithm: (i) the experimental descriptors of sintering conditions are significant for both bulk and grain boundary, (ii) the material descriptors of Li site occupancy and Li ratio are the prior descriptors for bulk, (iii) the density and unit cell volume are the prior structural descriptors while the polarizability and electronegativity are the prior chemical descriptors for grain boundary, (iv) the grain size provides physical insights such as the thermodynamic condition and should be considered for determining grain boundary conductance in solid polycrystalline ionic conductors.

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“…To date, a sintered body of the ionic conductor has been used for oxide solid electrolytes. However, the σ of a solid electrolyte obtained using powder decreases with the presence of grain boundary resistance [21,22]. By contrast, a solid electrolyte based on a single crystal has no grain boundary and high σ is expected.…”

Section: Introductionmentioning

confidence: 99%

Crystal growth of La _{2/3-
x} Li _{3
x} TiO ₃ by the TSFZ method

et al. 2018

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Double-perovskite-type La2/3-xLi3xTiO3 (LLT) crystals were grown by the travelling solvent floating zone (TSFZ) method. When the floating zone (FZ) crystal growth method was applied, the La2Ti2O7 phase was deposited as an inclusion in the initial growth region. Using the TSFZ crystal growth method, however, inclusion-free LLT crystals were obtained for a 10 mol% La2Ti2O7-poor composition solvent relative to the stoichiometric LLT crystals. The molten zone was initially unstable as a result of habit plane formation during the crystal growth; however, the molten zone was stably maintained for a long period of time by decreasing the feed rate compared with the growth rate. Hence, LLT crystals of approximately 5 mmφ and 37 mm in length were obtained. The anisotropic ionic conductivity of the crystals annealed in air was σ[110]/σ[001] ≈ 3, with σ[110] = 1.64 × 10−3 S cm−1 and σ[001] = 5.26 × 10−4 S cm−1. LLT single crystals are candidates for high-performance solid-state electrolytes in all-solid-state Li ion batteries.

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Separation of the bulk and grain boundary contributions to the total conductivity of solid lithium-ion conducting electrolytes

Cited by 43 publications

References 20 publications

Semiconductor-Ionic Nanocomposite La0.1Sr0.9MnO3−δ-Ce0.8Sm0.2O2−δ Functional Layer for High Performance Low Temperature SOFC

Semiconductor-Ionic Nanocomposite La0.1Sr0.9MnO3−δ-Ce0.8Sm0.2O2−δ Functional Layer for High Performance Low Temperature SOFC

Essential structural and experimental descriptors for bulk and grain boundary conductivities of Li solid electrolytes

Crystal growth of La _{2/3-
x} Li _{3
x} TiO ₃ by the TSFZ method

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Separation of the bulk and grain boundary contributions to the total conductivity of solid lithium-ion conducting electrolytes

Cited by 43 publications

References 20 publications

Semiconductor-Ionic Nanocomposite La0.1Sr0.9MnO3−δ-Ce0.8Sm0.2O2−δ Functional Layer for High Performance Low Temperature SOFC

Semiconductor-Ionic Nanocomposite La0.1Sr0.9MnO3−δ-Ce0.8Sm0.2O2−δ Functional Layer for High Performance Low Temperature SOFC

Essential structural and experimental descriptors for bulk and grain boundary conductivities of Li solid electrolytes

Crystal growth of La 2/3- x Li 3 x TiO 3 by the TSFZ method

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Crystal growth of La _{2/3-
x} Li _{3
x} TiO ₃ by the TSFZ method