Extremely dense microstructure and enhanced ionic conductivity in hot-isostatic pressing treated cubic garnet-type solid electrolyte of Ga2O3-doped Li7La3Zr2O12

2018 ◽  
Vol 11 (02) ◽  
pp. 1850029 ◽  
Author(s):  
Shiying Qin ◽  
Xiaohong Zhu ◽  
Yue Jiang ◽  
Ming’en Ling ◽  
Zhiwei Hu ◽  
...  

A large number of pores and a low relative density that are frequently observed in solid electrolytes reduce severely their ionic conductivity and thus limit their applicability. Here, we report on the use of hot isostatic pressing (HIP) for ameliorating the garnet-type lithium-ion conducting solid electrolyte of Ga2O3-doped Li7La3Zr2O[Formula: see text] (Ga-LLZO) with nominal composition of Li[Formula: see text]Ga[Formula: see text]La3Zr2O[Formula: see text]. The Ga-LLZO pellets were conventionally sintered at 1075[Formula: see text]C for 12[Formula: see text]h, and then were followed by HIP treatment at 120[Formula: see text]MPa and 1160[Formula: see text]C under an Ar atmosphere. It is found that the HIP-treated Ga-LLZO shows an extremely dense microstructure and a significantly enhanced ionic conductivity. Coherent with the increase in relative density from 90.5% (untreated) to 97.5% (HIP-treated), the ionic conductivity of the HIP-treated Ga-LLZO reaches as high as [Formula: see text][Formula: see text]S/cm at room temperature (25[Formula: see text]C), being two times higher than that of [Formula: see text][Formula: see text]S/cm for the untreated one.


2021 ◽  
pp. 2140002
Author(s):  
Mingxia Fan ◽  
Xiangyu Deng ◽  
Anqiao Zheng ◽  
Songdong Yuan

NASICON-type Li[Formula: see text]Al[Formula: see text]Ti[Formula: see text](PO[Formula: see text] (LATP) solid electrolytes have been widely studied because of its stability in the air, low material price and high ionic conductivity. Gd-doped Li[Formula: see text]Al[Formula: see text]Gd[Formula: see text]Ti[Formula: see text](PO[Formula: see text] ([Formula: see text]= 0, 0.025, 0.05, 0.075 and 0.1) with high ionic conductivity was successfully synthesized by solvothermal method for the first time in this work. The effect of Gd doping content on the structure and electrochemical performance of solid electrolytes was systematically studied. The optimal doping content of Gd is [Formula: see text]= 0.075. With the Gd doping content of 0.075, the solid electrolyte has the highest ionic conductivity of 4.23 × 10[Formula: see text] S cm[Formula: see text] at room temperature, the lowest activation energy of 0.247 eV and the highest relative density of 94.89%. This is because the fact that when [Formula: see text]= 0.075, it is the maximum content of Gd[Formula: see text] to replace Al[Formula: see text] and can completely enter the lattice of LATP, and does not emerge too much non-lithium ion conductive GdPO4 phase.



Molecules ◽  
2021 ◽  
Vol 26 (12) ◽  
pp. 3559
Author(s):  
Jinhua Hong ◽  
Shunsuke Kobayashi ◽  
Akihide Kuwabara ◽  
Yumi H. Ikuhara ◽  
Yasuyuki Fujiwara ◽  
...  

Solid electrolytes, such as perovskite Li3xLa2/1−xTiO3, LixLa(1−x)/3NbO3 and garnet Li7La3Zr2O12 ceramic oxides, have attracted extensive attention in lithium-ion battery research due to their good chemical stability and the improvability of their ionic conductivity with great potential in solid electrolyte battery applications. These solid oxides eliminate safety issues and cycling instability, which are common challenges in the current commercial lithium-ion batteries based on organic liquid electrolytes. However, in practical applications, structural disorders such as point defects and grain boundaries play a dominating role in the ionic transport of these solid electrolytes, where defect engineering to tailor or improve the ionic conductive property is still seldom reported. Here, we demonstrate a defect engineering approach to alter the ionic conductive channels in LixLa(1−x)/3NbO3 (x = 0.1 ~ 0.13) electrolytes based on the rearrangements of La sites through a quenching process. The changes in the occupancy and interstitial defects of La ions lead to anisotropic modulation of ionic conductivity with the increase in quenching temperatures. Our trial in this work on the defect engineering of quenched electrolytes will offer opportunities to optimize ionic conductivity and benefit the solid electrolyte battery applications.



2018 ◽  
Vol 20 (34) ◽  
pp. 22134-22147 ◽  
Author(s):  
Yun Kyung Shin ◽  
Mert Y. Sengul ◽  
A. S. M. Jonayat ◽  
Wonho Lee ◽  
Enrique D. Gomez ◽  
...  

Using a ReaxFF reactive force field, we investigated the composition-dependent ionic conductivity and the Li migration behaviors in Li1+xAlxTi2−x(PO4)3 solid electrolyte.



2014 ◽  
Vol 82 (11) ◽  
pp. 938-945 ◽  
Author(s):  
Nobuyuki IMANISHI ◽  
Masaki MATSUI ◽  
Yasuo TAKEDA ◽  
Osamu YAMAMOTO


Ceramics ◽  
2021 ◽  
Vol 4 (3) ◽  
pp. 421-436
Author(s):  
Aamir Iqbal Waidha ◽  
Vanita Vanita ◽  
Oliver Clemens

Composite electrolytes containing lithium ion conducting polymer matrix and ceramic filler are promising solid-state electrolytes for all solid-state lithium ion batteries due to their wide electrochemical stability window, high lithium ion conductivity and low electrode/electrolyte interfacial resistance. In this study, we report on the polymer infiltration of porous thin films of aluminum-doped cubic garnet fabricated via a combination of nebulized spray pyrolysis and spin coating with subsequent post annealing at 1173 K. This method offers a simple and easy route for the fabrication of a three-dimensional porous garnet network with a thickness in the range of 50 to 100 µm, which could be used as the ceramic backbone providing a continuous pathway for lithium ion transport in composite electrolytes. The porous microstructure of the fabricated thin films is confirmed via scanning electron microscopy. Ionic conductivity of the pristine films is determined via electrochemical impedance spectroscopy. We show that annealing times have a significant impact on the ionic conductivity of the films. The subsequent polymer infiltration of the porous garnet films shows a maximum ionic conductivity of 5.3 × 10−7 S cm−1 at 298 K, which is six orders of magnitude higher than the pristine porous garnet film.



2016 ◽  
Vol 4 (18) ◽  
pp. 6972-6979 ◽  
Author(s):  
Beatriz Lopez-Bermudez ◽  
Wolfgang G. Zeier ◽  
Shiliang Zhou ◽  
Anna J. Lehner ◽  
Jerry Hu ◽  
...  

The development of new frameworks for solid electrolytes exhibiting fast Li-ion diffusion is critical for enabling new energy storage technologies.



2019 ◽  
Vol 31 (21) ◽  
pp. 8649-8662 ◽  
Author(s):  
Rayavarapu Prasada Rao ◽  
Haomin Chen ◽  
Stefan Adams


2019 ◽  
Vol 337 ◽  
pp. 101-106 ◽  
Author(s):  
Yuta Koizumi ◽  
Daisuke Mori ◽  
Sou Taminato ◽  
Osamu Yamamoto ◽  
Yasuo Takeda ◽  
...  


Crystals ◽  
2020 ◽  
Vol 10 (11) ◽  
pp. 987
Author(s):  
Jin Shi ◽  
Yongfei Hong ◽  
Chengfei Zhu

The beta-Al2O3 solid electrolyte doped with Chromium was synthesized via a citrate-nitrate combustion method, which started with NaNO3, LiNO3, Cr(NO3)3·9H2O, and Al(NO3)3·9H2O as the raw materials in this paper. The thermal behavior analysis, structure, and ionic conductivity of the beta-Al2O3 solid electrolyte were studied by the thermogravimetry/differential scanning calorimetry (TG/DSC), X-ray diffraction (XRD), scanning electron microscopy (SEM), and electrochemical impedance spectroscopy (EIS). Meanwhile, the relative density and bending strength of the samples were also measured. The results showed that with the appropriate Chromium doping, the calcining temperature of the precursor powders was only 1100 °C, the β″-Al2O3 phase content, bending strength, relative density, and ionic conductivity were all improved with a compact and uniform cross section micrograph. The optimized sample contained 94% of β″-Al2O3 phase and exhibited a relative density up to 98.13% of the theoretical density. In addition, it showed a good bending strength (215 MPa) and a satisficed ionic conductivity (0.110 S cm−1 at 350 °C).



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