Improving the Ionic Conductivity of the LLZO–LZO Thin Film through Indium Doping

A solid-state electrolyte with an ionic conductivity comparable to that of a liquid electrolyte is demanded of all-solid-state lithium-ion batteries. Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) is considered to be a promising candid...

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Main Authors: Zongkai Yan, Yu Song, Shuai Wu, Yongmin Wu, Shipai Song, Xinyu Wang, Yanlin Zhu, Junsong Chen, Rui Guo, Yong Xiang
Format: Article
Language:English
Published: MDPI AG 2021-04-01
Series:Crystals
Subjects:
Online Access:https://www.mdpi.com/2073-4352/11/4/426
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author Zongkai Yan
Yu Song
Shuai Wu
Yongmin Wu
Shipai Song
Xinyu Wang
Yanlin Zhu
Junsong Chen
Rui Guo
Yong Xiang
author_facet Zongkai Yan
Yu Song
Shuai Wu
Yongmin Wu
Shipai Song
Xinyu Wang
Yanlin Zhu
Junsong Chen
Rui Guo
Yong Xiang
author_sort Zongkai Yan
collection DOAJ
description A solid-state electrolyte with an ionic conductivity comparable to that of a liquid electrolyte is demanded of all-solid-state lithium-ion batteries. Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) is considered to be a promising candidate due to its good thermal stability, high ionic conductivity, and wide electrochemical window. However, the synthesis of a stable cubic-phase LLZO thin film with enhanced densification at a relatively low thermal treatment temperature is yet to be developed. Indium is predicted to be a possible dopant to stabilize the cubic-phase LLZO (c-LLZO). Herein, via a nanolayer stacking process, a LLZO–Li<sub>2</sub>CO<sub>3</sub>–In<sub>2</sub>O<sub>3</sub> multilayer solid electrolyte precursor was obtained. After thermal annealing at different temperatures, the effects of indium doping on the formation of c-LLZO and the ionic conductivities of the prepared LLZO–LZO thin film were systematically investigated. The highest ionic conductivity of 9.6 × 10<sup>−6</sup> S·cm<sup>–1</sup> was obtained at an annealing temperature of 800 °C because the incorporation of indium promoted the formation of c-LLZO and the highly conductive LLZO–LZO interfaces. At the end, a model of LLZO–LZO interface-enhancing ionic conductivity was proposed. This work provides a new approach for the development of low-temperature LLZO-based, solid-state thin-film batteries.
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spelling doaj.art-54e8b2adc84f42cd8cdac71831c4b52e2023-11-21T15:41:14ZengMDPI AGCrystals2073-43522021-04-0111442610.3390/cryst11040426Improving the Ionic Conductivity of the LLZO–LZO Thin Film through Indium DopingZongkai Yan0Yu Song1Shuai Wu2Yongmin Wu3Shipai Song4Xinyu Wang5Yanlin Zhu6Junsong Chen7Rui Guo8Yong Xiang9School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, ChinaSchool of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, ChinaHunan Aerospace Huanyu Communication Technology Co., LTD., Changsha 410006, ChinaState Key Laboratory of Space Power-Sources Technology, Shanghai Institute of Space Power-Sources, Shanghai 200245, ChinaSchool of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, ChinaSchool of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, ChinaShenzhen Clean Energy Research Institute, Shenzhen 518045, ChinaSchool of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, ChinaState Key Laboratory of Space Power-Sources Technology, Shanghai Institute of Space Power-Sources, Shanghai 200245, ChinaSchool of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, ChinaA solid-state electrolyte with an ionic conductivity comparable to that of a liquid electrolyte is demanded of all-solid-state lithium-ion batteries. Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) is considered to be a promising candidate due to its good thermal stability, high ionic conductivity, and wide electrochemical window. However, the synthesis of a stable cubic-phase LLZO thin film with enhanced densification at a relatively low thermal treatment temperature is yet to be developed. Indium is predicted to be a possible dopant to stabilize the cubic-phase LLZO (c-LLZO). Herein, via a nanolayer stacking process, a LLZO–Li<sub>2</sub>CO<sub>3</sub>–In<sub>2</sub>O<sub>3</sub> multilayer solid electrolyte precursor was obtained. After thermal annealing at different temperatures, the effects of indium doping on the formation of c-LLZO and the ionic conductivities of the prepared LLZO–LZO thin film were systematically investigated. The highest ionic conductivity of 9.6 × 10<sup>−6</sup> S·cm<sup>–1</sup> was obtained at an annealing temperature of 800 °C because the incorporation of indium promoted the formation of c-LLZO and the highly conductive LLZO–LZO interfaces. At the end, a model of LLZO–LZO interface-enhancing ionic conductivity was proposed. This work provides a new approach for the development of low-temperature LLZO-based, solid-state thin-film batteries.https://www.mdpi.com/2073-4352/11/4/426LLZOindium dopingsolid electrolytes thin film
spellingShingle Zongkai Yan
Yu Song
Shuai Wu
Yongmin Wu
Shipai Song
Xinyu Wang
Yanlin Zhu
Junsong Chen
Rui Guo
Yong Xiang
Improving the Ionic Conductivity of the LLZO–LZO Thin Film through Indium Doping
Crystals
LLZO
indium doping
solid electrolytes thin film
title Improving the Ionic Conductivity of the LLZO–LZO Thin Film through Indium Doping
title_full Improving the Ionic Conductivity of the LLZO–LZO Thin Film through Indium Doping
title_fullStr Improving the Ionic Conductivity of the LLZO–LZO Thin Film through Indium Doping
title_full_unstemmed Improving the Ionic Conductivity of the LLZO–LZO Thin Film through Indium Doping
title_short Improving the Ionic Conductivity of the LLZO–LZO Thin Film through Indium Doping
title_sort improving the ionic conductivity of the llzo lzo thin film through indium doping
topic LLZO
indium doping
solid electrolytes thin film
url https://www.mdpi.com/2073-4352/11/4/426
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