Synergetic Effect of Li-Ion Concentration and Triple Doping on Ionic Conductivity of Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolyte

Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) is a promising and safe solid electrolyte for all-solid-state batteries. To achieve high ionic conductivity of LLZO, stabilizing the cubic phase and reducing Li loss during the sintering p...

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Main Authors: Minh Hai Nguyen, Sangbaek Park
Format: Article
Language:English
Published: MDPI AG 2022-08-01
Series:Nanomaterials
Subjects:
Online Access:https://www.mdpi.com/2079-4991/12/17/2946
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author Minh Hai Nguyen
Sangbaek Park
author_facet Minh Hai Nguyen
Sangbaek Park
author_sort Minh Hai Nguyen
collection DOAJ
description Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) is a promising and safe solid electrolyte for all-solid-state batteries. To achieve high ionic conductivity of LLZO, stabilizing the cubic phase and reducing Li loss during the sintering process is essential. Therefore, reducing the sintering temperature, which increases the sintering time for high-density pellets, is necessary. Herein, we investigate the change in the crystal structure, morphology, and Li ionic conductivity of LLZO pellets by triple doping with Al, Ga, and Ta and modulating the variation in initial Li concentrations. Interestingly, the proportion of the conductive cubic phase increased with increasing Li stoichiometry by 1.1 times, and this tendency was further accelerated by triple doping. The synergetic effects of triple doping and Li concentration also minimized Li loss during sintering. Accordingly, it provided a high-quality LLZO pellet with good ionic conductivity (3.6 × 10<sup>−4</sup> S cm<sup>−1</sup>) and high relative density (97.8%). Notably, the LLZO pellet was obtained using a very short sintering process (40 min). Considering that the most time-consuming step is the sintering process for LLZO, this study can provide guidelines for the fast production and commercialization of LLZO electrolytes with high ionic conductivity.
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spelling doaj.art-cae61c44e5514f9ab7a7ebcb8bdb697f2023-11-23T13:48:16ZengMDPI AGNanomaterials2079-49912022-08-011217294610.3390/nano12172946Synergetic Effect of Li-Ion Concentration and Triple Doping on Ionic Conductivity of Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid ElectrolyteMinh Hai Nguyen0Sangbaek Park1Department of Materials Science and Engineering, Chungnam National University, Daejeon 34134, KoreaDepartment of Materials Science and Engineering, Chungnam National University, Daejeon 34134, KoreaLi<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) is a promising and safe solid electrolyte for all-solid-state batteries. To achieve high ionic conductivity of LLZO, stabilizing the cubic phase and reducing Li loss during the sintering process is essential. Therefore, reducing the sintering temperature, which increases the sintering time for high-density pellets, is necessary. Herein, we investigate the change in the crystal structure, morphology, and Li ionic conductivity of LLZO pellets by triple doping with Al, Ga, and Ta and modulating the variation in initial Li concentrations. Interestingly, the proportion of the conductive cubic phase increased with increasing Li stoichiometry by 1.1 times, and this tendency was further accelerated by triple doping. The synergetic effects of triple doping and Li concentration also minimized Li loss during sintering. Accordingly, it provided a high-quality LLZO pellet with good ionic conductivity (3.6 × 10<sup>−4</sup> S cm<sup>−1</sup>) and high relative density (97.8%). Notably, the LLZO pellet was obtained using a very short sintering process (40 min). Considering that the most time-consuming step is the sintering process for LLZO, this study can provide guidelines for the fast production and commercialization of LLZO electrolytes with high ionic conductivity.https://www.mdpi.com/2079-4991/12/17/2946solid electrolytesLLZOLi-ion concentrationtriple dopingLi-ion conductivity
spellingShingle Minh Hai Nguyen
Sangbaek Park
Synergetic Effect of Li-Ion Concentration and Triple Doping on Ionic Conductivity of Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolyte
Nanomaterials
solid electrolytes
LLZO
Li-ion concentration
triple doping
Li-ion conductivity
title Synergetic Effect of Li-Ion Concentration and Triple Doping on Ionic Conductivity of Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolyte
title_full Synergetic Effect of Li-Ion Concentration and Triple Doping on Ionic Conductivity of Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolyte
title_fullStr Synergetic Effect of Li-Ion Concentration and Triple Doping on Ionic Conductivity of Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolyte
title_full_unstemmed Synergetic Effect of Li-Ion Concentration and Triple Doping on Ionic Conductivity of Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolyte
title_short Synergetic Effect of Li-Ion Concentration and Triple Doping on Ionic Conductivity of Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolyte
title_sort synergetic effect of li ion concentration and triple doping on ionic conductivity of li sub 7 sub la sub 3 sub zr sub 2 sub o sub 12 sub solid electrolyte
topic solid electrolytes
LLZO
Li-ion concentration
triple doping
Li-ion conductivity
url https://www.mdpi.com/2079-4991/12/17/2946
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AT sangbaekpark synergeticeffectofliionconcentrationandtripledopingonionicconductivityoflisub7sublasub3subzrsub2subosub12subsolidelectrolyte