Chemical compatibility between garnet-like solid state electrolyte Li6.75La3Zr1.75Ta0.25O12 and major commercial lithium battery cathode materials

Ren, Yaoyu; Liu, Ting; Shen, Yang; Lin, Yuanhua; Chen, Nan

doi:10.1016/j.jmat.2016.04.003

Cited by 109 publications

(135 citation statements)

References 51 publications

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“…It is worth here to compare our experimental finding to the previously reported computational and experimental studies 50,[58][59][60]63 La2Zr2O7 as a result of reactions between LCO and LLZO was proposed by those earlier works, which was also found by the XRD and XAS in this study. Formation of a La-Co-O phase was not predicted computationally, but has been suggested in several experimental papers 49,50,63 . In this work, we conclude that LaCoO3 is the more likely La-Co-O phase, rather than La2CoO4, due to the O K-edge XAS data and XRD.…”

Section: Discussionsupporting

confidence: 87%

“…The cross-diffusion of La and Co, and EXAFS and XRD signatures, strongly suggest the emergence of a La-Co-O phase. Previous studies of LCO|LLZO interface reactions indicated the formation of La-Co-O phases such as La2CoO4 and LaCoO3 49,50,63 . Zr shows negligible, if any, reactivity with LCO for the annealing conditions studied in this report.…”

Section: Discussionmentioning

confidence: 98%

“…The LaCoO3 (214) peak at 59.10⁰ (30.9% intensity) was not accessible due to the angular limit in the synchrotron XRD setup. Similar peak overlap issues have hindered the identification of secondary phases in cathode/LLZO powder mixtures previously 63 . Similar measurements were conducted with a laboratory XRD system using thicker LCO layers.…”

Section: D) Secondary Phase Formation At the Lco|llzo Interfacesmentioning

confidence: 93%

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Structure, Chemistry, and Charge Transfer Resistance of the Interface between Li₇La₃Zr₂O₁₂ Electrolyte and LiCoO₂ Cathode

et al. 2018

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All-solid-state batteries promise significant safety and energy density advantages over liquid-electrolyte batteries. The interface between the cathode and the solid electrolyte is an important contributor to charge transfer resistance. Strong bonding of solid oxide electrolytes and cathodes requires sintering at elevated temperatures. Knowledge of the temperature dependence of the composition and charge transfer properties of this interface is important for determining the ideal sintering conditions. To understand the interfacial decomposition processes and their onset temperatures, model systems of LiCoO2 (LCO) thin films deposited on cubic Al-doped Li7La3Zr2O12 (LLZO) pellets were studied as a function of temperature using interface-sensitive techniques. X-ray photoelectron spectroscopy (XPS), secondary ion mass spectroscopy (SIMS), and energy-dispersive X-ray spectroscopy (EDS) data indicated significant cation interdiffusion and structural changes starting at temperatures as low as 300⁰C. La2Zr2O7 and Li2CO3 were identified as 2 decomposition products after annealing at 500°C by synchrotron X-ray diffraction (XRD). X-ray absorption spectroscopy (XAS) results indicate the presence of also LaCoO3, in addition to La2Zr2O7 and Li2CO3. Based on electrochemical impedance spectroscopy, and depth profiling of the Li distribution upon potentiostatic hold experiments on symmetric LCO|LLZO|LCO cells, the interfaces exhibited significantly increased impedance, up to 8 times that of the as-deposited samples after annealing at 500 o C. Our results indicate that lower-temperature processing conditions, shorter annealing time scales, and CO2-free environments are desirable for obtaining ceramic cathode-electrolyte interfaces that enable fast Li transfer and high capacity.

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Section: Discussionsupporting

confidence: 87%

Section: Discussionmentioning

confidence: 98%

Section: D) Secondary Phase Formation At the Lco|llzo Interfacesmentioning

confidence: 93%

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Structure, Chemistry, and Charge Transfer Resistance of the Interface between Li₇La₃Zr₂O₁₂ Electrolyte and LiCoO₂ Cathode

et al. 2018

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“…Although Li-stuffed garnet-type oxide is a good candidate for SE in a solid-state battery, high-temperature sintering at 1000–1200 °C is generally needed for densification [7,11,12,13,14,15,16,17,18,19,20,21] and this temperature is too high to suppress the undesired side reaction between the majority of electrode active materials and SE and the formation of impurity phases [22]. Li + conducting Li 3 BO 3 with a low melting point (~700 °C) has been applied to form the interface between LiCoO 2 and garnet-type SE by a co-sintering process [23,24], but the conductivity for Li 3 BO 3 is low (10 −7 –10 −6 S cm −1 at room temperature) and there are currently limited electrode materials that can be used for solid-state batteries with garnet-type SEs developed by the co-sintering process.…”

Section: Introductionmentioning

confidence: 99%

Properties of Lithium Trivanadate Film Electrodes Formed on Garnet-Type Oxide Solid Electrolyte by Aerosol Deposition

et al. 2018

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We fabricated lithium trivanadate LiV3O8 (LVO) film electrodes for the first time on a garnet-type Ta-doped Li7La3Zr2O12 (LLZT) solid electrolyte using the aerosol deposition (AD) method. Ball-milled LVO powder with sizes in the range of 0.5–2 µm was used as a raw material for LVO film fabrication via impact consolidation at room temperature. LVO film (thickness = 5 µm) formed by AD has a dense structure composed of deformed and fractured LVO particles and pores were not observed at the LVO/LLZT interface. For electrochemical characterization of LVO film electrodes, lithium (Li) metal foil was attached on the other end face of a LLZT pellet to comprise a LVO/LLZT/Li all-solid-state cell. From impedance measurements, the charge transfer resistance at the LVO/LLZT interface is estimated to be around 103 Ω cm2 at room temperature, which is much higher than at the Li/LLZT interface. Reversible charge and discharge reactions in the LVO/LLZT/Li cell were demonstrated and the specific capacities were 100 and 290 mAh g−1 at 50 and 100 °C. Good cycling stability of electrode reaction indicates strong adhesion between the LVO film electrode formed via impact consolidation and LLZT.

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“…Li + /Li 0 ). There are other cathode materials under development which provide even higher potentials, however, examples are described in literature where they react chemically even more severely with LLZ-based garnet materials than LCO due to the additional transition metals [10,11,12].…”

Section: Introductionmentioning

confidence: 99%

Cathode-electrolyte material interactions during manufacturing of inorganic solid-state lithium batteries

et al. 2016

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Solid-state lithium batteries comprising a ceramic electrolyte instead of a liquid one enable safer highenergy batteries. Their manufacturing usually requires a high temperature heat treatment to interconnect electrolyte, electrodes, and if applicable, further components like current collectors. Tantalum-substituted Li 7 La 3 Zr 2 O 12 as electrolyte and LiCoO 2 as active material on the cathode side were chosen because of their high ionic conductivity and energy density, respectively. However, both materials react severely with each other at temperatures around 1085 °C thus leading to detrimental secondary phases. Thin-film technologies open a pathway for manufacturing compounds of electrolyte and active material at lower processing temperatures. Two of them are addressed in this work to manufacture thin electrolyte layers of the aforementioned materials at low temperatures: physical vapor deposition and coating technologies with liquid precursors. They are especially applicable for electrolyte layers since electrolytes require a high density while at the same time their thickness can be as thin as possible, provided that the separation of the electrodes is still guaranteed.

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Chemical compatibility between garnet-like solid state electrolyte Li6.75La3Zr1.75Ta0.25O12 and major commercial lithium battery cathode materials

Cited by 109 publications

References 51 publications

Structure, Chemistry, and Charge Transfer Resistance of the Interface between Li₇La₃Zr₂O₁₂ Electrolyte and LiCoO₂ Cathode

Structure, Chemistry, and Charge Transfer Resistance of the Interface between Li₇La₃Zr₂O₁₂ Electrolyte and LiCoO₂ Cathode

Properties of Lithium Trivanadate Film Electrodes Formed on Garnet-Type Oxide Solid Electrolyte by Aerosol Deposition

Cathode-electrolyte material interactions during manufacturing of inorganic solid-state lithium batteries

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Chemical compatibility between garnet-like solid state electrolyte Li6.75La3Zr1.75Ta0.25O12 and major commercial lithium battery cathode materials

Cited by 109 publications

References 51 publications

Structure, Chemistry, and Charge Transfer Resistance of the Interface between Li7La3Zr2O12 Electrolyte and LiCoO2 Cathode

Structure, Chemistry, and Charge Transfer Resistance of the Interface between Li7La3Zr2O12 Electrolyte and LiCoO2 Cathode

Properties of Lithium Trivanadate Film Electrodes Formed on Garnet-Type Oxide Solid Electrolyte by Aerosol Deposition

Cathode-electrolyte material interactions during manufacturing of inorganic solid-state lithium batteries

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Structure, Chemistry, and Charge Transfer Resistance of the Interface between Li₇La₃Zr₂O₁₂ Electrolyte and LiCoO₂ Cathode

Structure, Chemistry, and Charge Transfer Resistance of the Interface between Li₇La₃Zr₂O₁₂ Electrolyte and LiCoO₂ Cathode