Improvement of the Interface between the Lithium Anode and a Garnet-Type Solid Electrolyte of Lithium Batteries Using an Aluminum-Nitride Layer

The next generation of all-solid-state batteries can feature battery safety that is unparalleled among conventional liquid batteries. The garnet-type solid-state electrolyte Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO), in particular...

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Main Authors: Wen Jiang, Lingling Dong, Shuanghui Liu, Bing Ai, Shuangshuang Zhao, Weimin Zhang, Kefeng Pan, Lipeng Zhang
Format: Article
Language:English
Published: MDPI AG 2022-06-01
Series:Nanomaterials
Subjects:
Online Access:https://www.mdpi.com/2079-4991/12/12/2023
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author Wen Jiang
Lingling Dong
Shuanghui Liu
Bing Ai
Shuangshuang Zhao
Weimin Zhang
Kefeng Pan
Lipeng Zhang
author_facet Wen Jiang
Lingling Dong
Shuanghui Liu
Bing Ai
Shuangshuang Zhao
Weimin Zhang
Kefeng Pan
Lipeng Zhang
author_sort Wen Jiang
collection DOAJ
description The next generation of all-solid-state batteries can feature battery safety that is unparalleled among conventional liquid batteries. The garnet-type solid-state electrolyte Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO), in particular, is widely studied because of its high Li-ion conductivity and stability in air. However, the poor interface-contact between Li and the electrolyte (garnet) severely limits the development of solid electrolytes. In this study, we synthesize cubic phase Li<sub>6.4</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> (LLZTO) using a secondary sintering method. In addition, a thin aluminum nitride (AlN) layer is introduced between the metal (Li) and the solid electrolyte. Theoretical calculations show that AlN has a high affinity for Li. Furthermore, it is shown that the AlN coating can effectively reduce the interface impedance between Li and the solid electrolyte and improve the lithium-ion transport. The assembled symmetric Li cells can operate stably for more than 3600 h, unlike the symmetric cells without AlN coating, which short-circuited after only a few cycles. The hybrid solid-state battery with a modified layer, which is assembled using LiFePO<sub>4</sub> (LFP), still has a capacity of 120 mAh g<sup>−1</sup> after 200 cycles, with a capacity retention rate of 98%. This shows that the introduction of an AlN interlayer is very helpful to obtain a stable Li/solid-electrolyte interface, which improves the cycling stability of the battery.
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spelling doaj.art-3b32ad66768745518831ead558b2b8c52023-11-23T18:16:15ZengMDPI AGNanomaterials2079-49912022-06-011212202310.3390/nano12122023Improvement of the Interface between the Lithium Anode and a Garnet-Type Solid Electrolyte of Lithium Batteries Using an Aluminum-Nitride LayerWen Jiang0Lingling Dong1Shuanghui Liu2Bing Ai3Shuangshuang Zhao4Weimin Zhang5Kefeng Pan6Lipeng Zhang7School of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255049, ChinaSchool of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255049, ChinaSchool of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255049, ChinaSchool of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255049, ChinaSchool of Materials and New Energy, South China Normal University, Shanwei 516600, ChinaSchool of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255049, ChinaSchool of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255049, ChinaSchool of Materials and New Energy, South China Normal University, Shanwei 516600, ChinaThe next generation of all-solid-state batteries can feature battery safety that is unparalleled among conventional liquid batteries. The garnet-type solid-state electrolyte Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO), in particular, is widely studied because of its high Li-ion conductivity and stability in air. However, the poor interface-contact between Li and the electrolyte (garnet) severely limits the development of solid electrolytes. In this study, we synthesize cubic phase Li<sub>6.4</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> (LLZTO) using a secondary sintering method. In addition, a thin aluminum nitride (AlN) layer is introduced between the metal (Li) and the solid electrolyte. Theoretical calculations show that AlN has a high affinity for Li. Furthermore, it is shown that the AlN coating can effectively reduce the interface impedance between Li and the solid electrolyte and improve the lithium-ion transport. The assembled symmetric Li cells can operate stably for more than 3600 h, unlike the symmetric cells without AlN coating, which short-circuited after only a few cycles. The hybrid solid-state battery with a modified layer, which is assembled using LiFePO<sub>4</sub> (LFP), still has a capacity of 120 mAh g<sup>−1</sup> after 200 cycles, with a capacity retention rate of 98%. This shows that the introduction of an AlN interlayer is very helpful to obtain a stable Li/solid-electrolyte interface, which improves the cycling stability of the battery.https://www.mdpi.com/2079-4991/12/12/2023LLZTOsolid-state electrolyteslithium/electrolyte interfaceanode interfacelithium-ion battery
spellingShingle Wen Jiang
Lingling Dong
Shuanghui Liu
Bing Ai
Shuangshuang Zhao
Weimin Zhang
Kefeng Pan
Lipeng Zhang
Improvement of the Interface between the Lithium Anode and a Garnet-Type Solid Electrolyte of Lithium Batteries Using an Aluminum-Nitride Layer
Nanomaterials
LLZTO
solid-state electrolytes
lithium/electrolyte interface
anode interface
lithium-ion battery
title Improvement of the Interface between the Lithium Anode and a Garnet-Type Solid Electrolyte of Lithium Batteries Using an Aluminum-Nitride Layer
title_full Improvement of the Interface between the Lithium Anode and a Garnet-Type Solid Electrolyte of Lithium Batteries Using an Aluminum-Nitride Layer
title_fullStr Improvement of the Interface between the Lithium Anode and a Garnet-Type Solid Electrolyte of Lithium Batteries Using an Aluminum-Nitride Layer
title_full_unstemmed Improvement of the Interface between the Lithium Anode and a Garnet-Type Solid Electrolyte of Lithium Batteries Using an Aluminum-Nitride Layer
title_short Improvement of the Interface between the Lithium Anode and a Garnet-Type Solid Electrolyte of Lithium Batteries Using an Aluminum-Nitride Layer
title_sort improvement of the interface between the lithium anode and a garnet type solid electrolyte of lithium batteries using an aluminum nitride layer
topic LLZTO
solid-state electrolytes
lithium/electrolyte interface
anode interface
lithium-ion battery
url https://www.mdpi.com/2079-4991/12/12/2023
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