Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>-co-LiNbO<sub>3</sub> Surface Modification Improves the Interface Stability between Cathode and Sulfide Solid-State Electrolyte in All-Solid-State Batteries

With the rapid development of energy storage and electric vehicles, thiophosphate-based all-solid-state batteries (ASSBs) are considered the most promising power source. In order to commercialize ASSBs, the interfacial problem between high-voltage cathode active materials and thiophosphate-based sol...

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Main Authors: Shishuo Liang, Dong Yang, Jianhua Hu, Shusen Kang, Xue Zhang, Yanchen Fan
Format: Article
Language:English
Published: MDPI AG 2023-02-01
Series:Membranes
Subjects:
Online Access:https://www.mdpi.com/2077-0375/13/2/216
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author Shishuo Liang
Dong Yang
Jianhua Hu
Shusen Kang
Xue Zhang
Yanchen Fan
author_facet Shishuo Liang
Dong Yang
Jianhua Hu
Shusen Kang
Xue Zhang
Yanchen Fan
author_sort Shishuo Liang
collection DOAJ
description With the rapid development of energy storage and electric vehicles, thiophosphate-based all-solid-state batteries (ASSBs) are considered the most promising power source. In order to commercialize ASSBs, the interfacial problem between high-voltage cathode active materials and thiophosphate-based solid-state electrolytes needs to be solved in a simple, effective way. Surface coatings are considered the most promising approach to solving the interfacial problem because surface coatings could prevent direct physical contact between cathode active materials and thiophosphate-based solid-state electrolytes. In this work, Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) and LiNbO<sub>3</sub> (LNO) coatings for LiCoO<sub>2</sub> (LCO) were fabricated by in-situ interfacial growth of two high-Li<sup>+</sup> conductive oxide electrolytes on the LCO surface and tested for thiophosphate-based ASSBs. The coatings were obtained from a two-step traditional sol–gel coatings process, the inner coatings were LNO, and the surface coatings were LLZO. Electrochemical evaluations confirmed that the two-layer coatings are beneficial for ASSBs. ASSBs containing LLZO-co-LNO coatings LiCoO<sub>2</sub> (LLZO&LNO@LCO) significantly improved long-term cycling performance and discharge capacity compared with those assembled from uncoated LCO. LLZO&LNO@LCO||Li<sub>6</sub>PS<sub>5</sub>Cl (LPSC)||Li-In delivered discharge capacities of 138.8 mAh/g, 101.8 mAh/g, 60.2 mAh/g, and 40.2 mAh/g at 0.05 C, 0.1 C, 0.2 C, and 0.5 C under room temperature, respectively, and better capacity retentions of 98% after 300 cycles at 0.05 C. The results highlighted promising low-cost and scalable cathode material coatings for ASSBs.
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spelling doaj.art-9470f3fc531e41828f16f05f978899ea2023-11-16T22:02:55ZengMDPI AGMembranes2077-03752023-02-0113221610.3390/membranes13020216Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>-co-LiNbO<sub>3</sub> Surface Modification Improves the Interface Stability between Cathode and Sulfide Solid-State Electrolyte in All-Solid-State BatteriesShishuo Liang0Dong Yang1Jianhua Hu2Shusen Kang3Xue Zhang4Yanchen Fan5State Key Laboratory of Molecular Engineering of Polymer, Department of Macromolecular Science, Fudan University, Shanghai 200438, ChinaState Key Laboratory of Molecular Engineering of Polymer, Department of Macromolecular Science, Fudan University, Shanghai 200438, ChinaState Key Laboratory of Molecular Engineering of Polymer, Department of Macromolecular Science, Fudan University, Shanghai 200438, ChinaSunwoda Electric Vehicle Battery Company, Shenzhen 518107, ChinaCollege of Resources and Environment, Jilin Agricultural University, Changchun 130118, ChinaPetro China Shenzhen Renewable Energy Research Institute Co., Ltd., Shenzhen 518000, ChinaWith the rapid development of energy storage and electric vehicles, thiophosphate-based all-solid-state batteries (ASSBs) are considered the most promising power source. In order to commercialize ASSBs, the interfacial problem between high-voltage cathode active materials and thiophosphate-based solid-state electrolytes needs to be solved in a simple, effective way. Surface coatings are considered the most promising approach to solving the interfacial problem because surface coatings could prevent direct physical contact between cathode active materials and thiophosphate-based solid-state electrolytes. In this work, Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) and LiNbO<sub>3</sub> (LNO) coatings for LiCoO<sub>2</sub> (LCO) were fabricated by in-situ interfacial growth of two high-Li<sup>+</sup> conductive oxide electrolytes on the LCO surface and tested for thiophosphate-based ASSBs. The coatings were obtained from a two-step traditional sol–gel coatings process, the inner coatings were LNO, and the surface coatings were LLZO. Electrochemical evaluations confirmed that the two-layer coatings are beneficial for ASSBs. ASSBs containing LLZO-co-LNO coatings LiCoO<sub>2</sub> (LLZO&LNO@LCO) significantly improved long-term cycling performance and discharge capacity compared with those assembled from uncoated LCO. LLZO&LNO@LCO||Li<sub>6</sub>PS<sub>5</sub>Cl (LPSC)||Li-In delivered discharge capacities of 138.8 mAh/g, 101.8 mAh/g, 60.2 mAh/g, and 40.2 mAh/g at 0.05 C, 0.1 C, 0.2 C, and 0.5 C under room temperature, respectively, and better capacity retentions of 98% after 300 cycles at 0.05 C. The results highlighted promising low-cost and scalable cathode material coatings for ASSBs.https://www.mdpi.com/2077-0375/13/2/216solid-state batteriesLiCoO<sub>2</sub>sulfide solid-state electrolyteLiNbO<sub>3</sub>-coatingLLZO-coating
spellingShingle Shishuo Liang
Dong Yang
Jianhua Hu
Shusen Kang
Xue Zhang
Yanchen Fan
Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>-co-LiNbO<sub>3</sub> Surface Modification Improves the Interface Stability between Cathode and Sulfide Solid-State Electrolyte in All-Solid-State Batteries
Membranes
solid-state batteries
LiCoO<sub>2</sub>
sulfide solid-state electrolyte
LiNbO<sub>3</sub>-coating
LLZO-coating
title Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>-co-LiNbO<sub>3</sub> Surface Modification Improves the Interface Stability between Cathode and Sulfide Solid-State Electrolyte in All-Solid-State Batteries
title_full Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>-co-LiNbO<sub>3</sub> Surface Modification Improves the Interface Stability between Cathode and Sulfide Solid-State Electrolyte in All-Solid-State Batteries
title_fullStr Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>-co-LiNbO<sub>3</sub> Surface Modification Improves the Interface Stability between Cathode and Sulfide Solid-State Electrolyte in All-Solid-State Batteries
title_full_unstemmed Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>-co-LiNbO<sub>3</sub> Surface Modification Improves the Interface Stability between Cathode and Sulfide Solid-State Electrolyte in All-Solid-State Batteries
title_short Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>-co-LiNbO<sub>3</sub> Surface Modification Improves the Interface Stability between Cathode and Sulfide Solid-State Electrolyte in All-Solid-State Batteries
title_sort li sub 7 sub la sub 3 sub zr sub 2 sub o sub 12 sub co linbo sub 3 sub surface modification improves the interface stability between cathode and sulfide solid state electrolyte in all solid state batteries
topic solid-state batteries
LiCoO<sub>2</sub>
sulfide solid-state electrolyte
LiNbO<sub>3</sub>-coating
LLZO-coating
url https://www.mdpi.com/2077-0375/13/2/216
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