Preparation and Electrochemical Characterization of Y-Doped Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> Solid Electrolytes for Lithium-Metal Batteries

Lithium-conducting NASICON materials have emerged as a promising alternative to organic liquid electrolytes for high-energy-density Li-metal batteries, owing to their superior ionic conductivity and excellent air stability. However, their practical application is hindered by poor sintering character...

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Main Authors: Zhongran Yao, Fen Qi, Qiang Sun, Lin Ye, Xiaowei Yang, Guojie Chao, Pei Tang, Kongjun Zhu
Format: Article
Language:English
Published: MDPI AG 2024-12-01
Series:Crystals
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Online Access:https://www.mdpi.com/2073-4352/15/1/31
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author Zhongran Yao
Fen Qi
Qiang Sun
Lin Ye
Xiaowei Yang
Guojie Chao
Pei Tang
Kongjun Zhu
author_facet Zhongran Yao
Fen Qi
Qiang Sun
Lin Ye
Xiaowei Yang
Guojie Chao
Pei Tang
Kongjun Zhu
author_sort Zhongran Yao
collection DOAJ
description Lithium-conducting NASICON materials have emerged as a promising alternative to organic liquid electrolytes for high-energy-density Li-metal batteries, owing to their superior ionic conductivity and excellent air stability. However, their practical application is hindered by poor sintering characteristics and high grain boundary resistance. In this investigation, Li<sub>1.3</sub>Al<sub>0.3−x</sub>Y<sub>x</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> (LAYTP-<i>x</i>, <i>x</i> = 0.00, 0.01, 0.03, 0.05, and 0.07) were successfully synthesized via conventional solid-state reaction to explore the impact of Y<sup>3+</sup> on both ionic conductivity and chemical stability. The structural, morphological, and transport properties of the samples were comprehensively characterized in order to identify the optimal doping concentration. All samples exhibited a NASICON structure with a uniform distribution of Y elements within the electrolyte. Due to its highest relative density (95.8%), the LAYTP-0.03 electrolyte demonstrated the highest total conductivity of 2.03 × 10<sup>−4</sup> S cm<sup>−1</sup> with a relatively low activation energy of 0.33 eV, making it suitable for solid-state batteries. When paired with the NCM811 cathode, the Li/LAYTP-0.03/NCM811 cell exhibited outstanding electrochemical performance: a high capacity of 155 mAh/g was achieved at 0.2C after 50 cycles with a Coulombic efficiency of approximately 100%, indicating highly reversible lithium plating/stripping facilitated by the LAYTP-0.03 electrolyte. These results suggest that the LAYTP-0.03 ceramic electrolyte could be a promising alternative for developing safe solid-state Li-metal batteries.
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spelling doaj-art-eed48cdfdf604bc49d5f98286c6215c22025-01-24T13:28:04ZengMDPI AGCrystals2073-43522024-12-011513110.3390/cryst15010031Preparation and Electrochemical Characterization of Y-Doped Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> Solid Electrolytes for Lithium-Metal BatteriesZhongran Yao0Fen Qi1Qiang Sun2Lin Ye3Xiaowei Yang4Guojie Chao5Pei Tang6Kongjun Zhu7School of Automobile and Traffic Engineering, Wuxi Institute of Technology, Wuxi 214121, ChinaKai Yuan School of Innovation and Entrepreneurship, Wuxi Institute of Technology, Wuxi 214121, ChinaSchool of Automobile and Traffic Engineering, Wuxi Institute of Technology, Wuxi 214121, ChinaSchool of Automobile and Traffic Engineering, Wuxi Institute of Technology, Wuxi 214121, ChinaSchool of Automobile and Traffic Engineering, Wuxi Institute of Technology, Wuxi 214121, ChinaSchool of Automobile and Traffic Engineering, Wuxi Institute of Technology, Wuxi 214121, ChinaSchool of Automotive Engineering, Yancheng Institute of Technology, Yancheng 224051, ChinaState Key Laboratory of Mechanics and Control for Aerospace Structures, College of Aerospace Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, ChinaLithium-conducting NASICON materials have emerged as a promising alternative to organic liquid electrolytes for high-energy-density Li-metal batteries, owing to their superior ionic conductivity and excellent air stability. However, their practical application is hindered by poor sintering characteristics and high grain boundary resistance. In this investigation, Li<sub>1.3</sub>Al<sub>0.3−x</sub>Y<sub>x</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> (LAYTP-<i>x</i>, <i>x</i> = 0.00, 0.01, 0.03, 0.05, and 0.07) were successfully synthesized via conventional solid-state reaction to explore the impact of Y<sup>3+</sup> on both ionic conductivity and chemical stability. The structural, morphological, and transport properties of the samples were comprehensively characterized in order to identify the optimal doping concentration. All samples exhibited a NASICON structure with a uniform distribution of Y elements within the electrolyte. Due to its highest relative density (95.8%), the LAYTP-0.03 electrolyte demonstrated the highest total conductivity of 2.03 × 10<sup>−4</sup> S cm<sup>−1</sup> with a relatively low activation energy of 0.33 eV, making it suitable for solid-state batteries. When paired with the NCM811 cathode, the Li/LAYTP-0.03/NCM811 cell exhibited outstanding electrochemical performance: a high capacity of 155 mAh/g was achieved at 0.2C after 50 cycles with a Coulombic efficiency of approximately 100%, indicating highly reversible lithium plating/stripping facilitated by the LAYTP-0.03 electrolyte. These results suggest that the LAYTP-0.03 ceramic electrolyte could be a promising alternative for developing safe solid-state Li-metal batteries.https://www.mdpi.com/2073-4352/15/1/31NASICON materialsLi-metal batteriesionic conductivitysolid-state batterieselectrochemical performance
spellingShingle Zhongran Yao
Fen Qi
Qiang Sun
Lin Ye
Xiaowei Yang
Guojie Chao
Pei Tang
Kongjun Zhu
Preparation and Electrochemical Characterization of Y-Doped Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> Solid Electrolytes for Lithium-Metal Batteries
Crystals
NASICON materials
Li-metal batteries
ionic conductivity
solid-state batteries
electrochemical performance
title Preparation and Electrochemical Characterization of Y-Doped Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> Solid Electrolytes for Lithium-Metal Batteries
title_full Preparation and Electrochemical Characterization of Y-Doped Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> Solid Electrolytes for Lithium-Metal Batteries
title_fullStr Preparation and Electrochemical Characterization of Y-Doped Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> Solid Electrolytes for Lithium-Metal Batteries
title_full_unstemmed Preparation and Electrochemical Characterization of Y-Doped Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> Solid Electrolytes for Lithium-Metal Batteries
title_short Preparation and Electrochemical Characterization of Y-Doped Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> Solid Electrolytes for Lithium-Metal Batteries
title_sort preparation and electrochemical characterization of y doped li sub 1 3 sub al sub 0 3 sub ti sub 1 7 sub po sub 4 sub sub 3 sub solid electrolytes for lithium metal batteries
topic NASICON materials
Li-metal batteries
ionic conductivity
solid-state batteries
electrochemical performance
url https://www.mdpi.com/2073-4352/15/1/31
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