Sol–gel synthesis and lithium ion conductivity of Li7La3Zr2O12 with garnet-related type structure

Kokal, Ilkin; Somer, M.; Notten, Phl Peter; Hintzen, Htjm Bert

doi:10.1016/j.ssi.2011.01.002

Cited by 241 publications

(159 citation statements)

References 20 publications

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“…In fact, at high temperature, the grain-boundary contribution is very small and cannot be differentiated from the bulk response. The actual capacitance (C) can be calculated 3,8,12,[18][19][20][21][22][23] from CPE and resistance (R) using the formula:…”

Section: Resultsmentioning

confidence: 99%

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X-ray Photoelectron Spectroscopy and AC Impedance Spectroscopy Studies of Li-La-Zr-O Solid Electrolyte Thin Film/LiCoO₂Cathode Interface for All-Solid-State Li Batteries

Zarabian

Bartolini

Pereira‐Almao

et al. 2017

J. Electrochem. Soc.

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Li ion half-cell electrode-based configuration was prepared by spin-coating using precursor of Li-stuffed garnet with intended composition of Li 7 La 3 Zr 2 O 12 on LiCoO 2 . The main goal of this study was lowering the heat-treatment to 400 • C, which is well below the chemical reaction temperature of these phases. Liquid precursor of the nominal compound was prepared and spin-coated on the top surface of MgO(100) and LiCoO 2 pellets until the appropriate thickness was obtained. Electrochemical impedance spectroscopy (EIS) was used to understand the resistance and capacitance behavior of the electrolyte and electrolyte-electrode interface. The ac impedance of half-cell shows semicircles, corresponding to the response from bulk electrolyte, second phase and interface. The interfacial region between LiCoO 2 and Li-La-Zr-O film was deeply studied with X-ray photoelectron spectroscopy (XPS) depth profile analysis. XPS results show that Co diffuses from the substrate toward the solid electrolyte; Li depletes in the interface region, and moves to the top surface, which changes the electronic structure of Co to a multiplicity of reduced forms. The present study shows that even at 400 • C, the Li-stuffed garnet precursor and LiCoO 2 cathode seem to form reaction products, suggesting that is critical for applications to develop protecting layers between the cathodes and Li-stuffed garnet electrolytes. Switching from an organic polymer-based Li ion electrolyte to a ceramic Li ion electrolyte in conventional Li ion batteries is expected to allow for higher energy density, improve safety and prolong lifetime. These, all-solid-state Li batteries can also be miniaturized, which will streamline the packing design and save cargo space. A solid electrolyte has to have several criteria to be able to use in the Li ion batteries such as high ionic conductivity at room temperature, high Li + ion transference number, chemical stability versus the Li cathodes and the Li anodes during preparation and battery operation, sustainability and economic feasibility.1-3 Although all-solid-state batteries offer lots of advantages over conventional liquid and polymer based batteries, the widespread applications of currently developed solid-state (ceramic) Li ion electrolytes have been postponed by low conductivity and or high reactivity with the electrodes which impede reaching high power density required for electric vehicles. 4,5 Li-stuffed garnet is a promising type of solid electrolyte offering an advantage of very high electrochemical stability window (∼6 V versus Li/Li + for Zr and Ta-based garnets), which opens up the possibility of using alternative cathodes and anodes for high voltage applications. It solely allows Li ions to move, and reduces the chance of capacity fading by unwanted reactions and or self-discharging. It is benign and resistant to Li dendrite electroplating.6-8 Interfacial resistance of Li stuffed garnet with Li metal and LiCoO 2 has been the scope of some recent studies targeting developing high performance battery f...

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Section: Resultsmentioning

confidence: 99%

“…techniques. 3,8,12,[18][19][20][21][22][23] Li ion conductivity at room temperature is estimated 1 × 10 −6 Scm −1 . This value is about two orders of magnitude lower than the reported value for bulk Li 7 La 3 Zr 2 O 12 (LLZO) sample; however, it is comparable to the reported garnet LLZO thin film prepared at much higher temperature.…”

Section: Resultsmentioning

confidence: 99%

X-ray Photoelectron Spectroscopy and AC Impedance Spectroscopy Studies of Li-La-Zr-O Solid Electrolyte Thin Film/LiCoO₂Cathode Interface for All-Solid-State Li Batteries

Zarabian

Bartolini

Pereira‐Almao

et al. 2017

J. Electrochem. Soc.

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“…However, there have been several reports of Al-free cubic LLZO produced at lower temperatures. For example, cubic LLZO has been produced by sol-gel synthesis at 700°C [10,11]. The lattice parameters of these low temperature cubic phases are larger than the values reported for nominally Al-free cubic phases produced at high temperatures (Table 1) [3,12].…”

Section: Introductionmentioning

confidence: 89%

Effect of microstructure and surface impurity segregation on the electrical and electrochemical properties of dense Al-substituted Li₇La₃Zr₂O₁₂

et al. 2014

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Al-substituted Li 7 La 3 Zr 2 O 12 (LLZO) pellets with a grain size of 100-200 µm and a relative density of 94% were prepared by conventional solid-state processing at a sintering temperature of 1100° C, 130°C lower than previously reported. Morphological features and the presence of impurities were evaluated by X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy dispersive x-ray spectroscopy (EDS). Femtosecond Laser Induced Breakdown Spectroscopy (LIBS) was used to visualize the distribution of impurities. The results suggest that chemical composition of the powder cover strongly affects morphology and impurity formation, and that particle size control is critical to densification. These properties, in turn, strongly affect total ionic conductivity and interfacial resistance of the sintered pellets.3

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“…Conductivity of the cubic phase (10 −4 S cm −1 , room temperature) is about two orders of magnitude higher than that of the tetragonal phase (Kokal et al, 2011;Tietz et al, 2013). Therefore, the challenge has been to stabilize the cubic phase, which can be achieved by doping.…”

Section: Garnet-type Electrolytesmentioning

confidence: 99%

Recent Advances in Inorganic Solid Electrolytes for Lithium Batteries

et al. 2014

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The review presents an overview of the recent advances in inorganic solid lithium ion conductors, which are of great interest as solid electrolytes in all-solid-state lithium batteries. It is focused on two major categories: crystalline electrolytes and glass-based electrolytes. Important systems such as thio-LISICON Li 10 SnP 2 S 12 , garnet Li 7 La 3 Zr 2 O 12 , perovskite Li 3x La (2/3) x TiO 3 , NASICON Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 , and glass-ceramic xLi 2 S·(1 − x )P − 2 S 5 and their progress are described in great detail. Meanwhile, the review discusses different ongoing strategies on enhancing conductivity, optimizing electrolyte/electrode interface, and improving cell performance.

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Sol–gel synthesis and lithium ion conductivity of Li7La3Zr2O12 with garnet-related type structure

Cited by 241 publications

References 20 publications

X-ray Photoelectron Spectroscopy and AC Impedance Spectroscopy Studies of Li-La-Zr-O Solid Electrolyte Thin Film/LiCoO₂Cathode Interface for All-Solid-State Li Batteries

X-ray Photoelectron Spectroscopy and AC Impedance Spectroscopy Studies of Li-La-Zr-O Solid Electrolyte Thin Film/LiCoO₂Cathode Interface for All-Solid-State Li Batteries

Effect of microstructure and surface impurity segregation on the electrical and electrochemical properties of dense Al-substituted Li₇La₃Zr₂O₁₂

Recent Advances in Inorganic Solid Electrolytes for Lithium Batteries

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Sol–gel synthesis and lithium ion conductivity of Li7La3Zr2O12 with garnet-related type structure

Cited by 241 publications

References 20 publications

X-ray Photoelectron Spectroscopy and AC Impedance Spectroscopy Studies of Li-La-Zr-O Solid Electrolyte Thin Film/LiCoO2Cathode Interface for All-Solid-State Li Batteries

X-ray Photoelectron Spectroscopy and AC Impedance Spectroscopy Studies of Li-La-Zr-O Solid Electrolyte Thin Film/LiCoO2Cathode Interface for All-Solid-State Li Batteries

Effect of microstructure and surface impurity segregation on the electrical and electrochemical properties of dense Al-substituted Li7La3Zr2O12

Recent Advances in Inorganic Solid Electrolytes for Lithium Batteries

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Product

Resources

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X-ray Photoelectron Spectroscopy and AC Impedance Spectroscopy Studies of Li-La-Zr-O Solid Electrolyte Thin Film/LiCoO₂Cathode Interface for All-Solid-State Li Batteries

X-ray Photoelectron Spectroscopy and AC Impedance Spectroscopy Studies of Li-La-Zr-O Solid Electrolyte Thin Film/LiCoO₂Cathode Interface for All-Solid-State Li Batteries

Effect of microstructure and surface impurity segregation on the electrical and electrochemical properties of dense Al-substituted Li₇La₃Zr₂O₁₂