Infiltration-driven performance enhancement of poly-crystalline cathodes in all-solid-state batteries

Abstract All-solid-state batteries (ASSBs) with adequately selected cathode materials exhibit a higher energy density and better safety than conventional lithium-ion batteries (LIBs). Ni-rich layered cathodes are benchmark materials for traditional LIBs owing to their high energy density. Recent stu...

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Main Authors: Junghwan Sung, Junyoung Heo, Dong-Hee Kim, Hawon Gu, Yung-Soo Jo, Heetaek Park, Jun-Ho Park, Jeong-Hee Choi, Yoon-Cheol Ha, Doohun Kim, Jun-Woo Park
Format: Article
Language:English
Published: Nature Portfolio 2024-10-01
Series:NPG Asia Materials
Online Access:https://doi.org/10.1038/s41427-024-00555-7
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author Junghwan Sung
Junyoung Heo
Dong-Hee Kim
Hawon Gu
Yung-Soo Jo
Heetaek Park
Jun-Ho Park
Jeong-Hee Choi
Yoon-Cheol Ha
Doohun Kim
Jun-Woo Park
author_facet Junghwan Sung
Junyoung Heo
Dong-Hee Kim
Hawon Gu
Yung-Soo Jo
Heetaek Park
Jun-Ho Park
Jeong-Hee Choi
Yoon-Cheol Ha
Doohun Kim
Jun-Woo Park
author_sort Junghwan Sung
collection DOAJ
description Abstract All-solid-state batteries (ASSBs) with adequately selected cathode materials exhibit a higher energy density and better safety than conventional lithium-ion batteries (LIBs). Ni-rich layered cathodes are benchmark materials for traditional LIBs owing to their high energy density. Recent studies have highlighted the advantages of using crack-free, single-crystalline cathode materials in ASSBs. In this study, a scalable infiltration sheet-type process was used to fabricate composite electrodes with different cathode-material morphologies for ASSBs. Typically, crack-free single-crystalline materials exhibit better retention performance and lower rate capability (i.e., slower kinetics in charge‒discharge processes) than polycrystalline cathode materials. Li6PS5Cl-infiltrated polycrystalline electrodes showed excellent retention performance and rate capability. Galvanostatic intermittent titration technique analysis and transmission electron microscopy of the single-crystalline electrode confirmed severe polarization and the presence of a rock-salt-structure layer in the cathode particles; these results indicated side reactions within the layered structure of the material. In contrast, composite electrodes consisting of polycrystalline cathode materials infiltrated with the solid electrolyte Li6PS5Cl showed excellent electrochemical performance owing to intimate electrode–electrolyte interfacial contact. The result from this study confirmed the critical influence of interface engineering and material morphology on the overall performance and stability of ASSBs and could facilitate the development of high-performance ASSBs in the future.
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publishDate 2024-10-01
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series NPG Asia Materials
spelling doaj-art-c1c9b51d5ef04199b87055f6c2f207452025-01-19T12:28:49ZengNature PortfolioNPG Asia Materials1884-40572024-10-011611910.1038/s41427-024-00555-7Infiltration-driven performance enhancement of poly-crystalline cathodes in all-solid-state batteriesJunghwan Sung0Junyoung Heo1Dong-Hee Kim2Hawon Gu3Yung-Soo Jo4Heetaek Park5Jun-Ho Park6Jeong-Hee Choi7Yoon-Cheol Ha8Doohun Kim9Jun-Woo Park10Battery Research Division, Korea Electrotechnology Research Institute (KERI)Battery Research Division, Korea Electrotechnology Research Institute (KERI)Battery Research Division, Korea Electrotechnology Research Institute (KERI)Battery Research Division, Korea Electrotechnology Research Institute (KERI)Battery Research Division, Korea Electrotechnology Research Institute (KERI)Battery Research Division, Korea Electrotechnology Research Institute (KERI)Battery Research Division, Korea Electrotechnology Research Institute (KERI)Battery Research Division, Korea Electrotechnology Research Institute (KERI)Battery Research Division, Korea Electrotechnology Research Institute (KERI)Battery Research Division, Korea Electrotechnology Research Institute (KERI)Battery Research Division, Korea Electrotechnology Research Institute (KERI)Abstract All-solid-state batteries (ASSBs) with adequately selected cathode materials exhibit a higher energy density and better safety than conventional lithium-ion batteries (LIBs). Ni-rich layered cathodes are benchmark materials for traditional LIBs owing to their high energy density. Recent studies have highlighted the advantages of using crack-free, single-crystalline cathode materials in ASSBs. In this study, a scalable infiltration sheet-type process was used to fabricate composite electrodes with different cathode-material morphologies for ASSBs. Typically, crack-free single-crystalline materials exhibit better retention performance and lower rate capability (i.e., slower kinetics in charge‒discharge processes) than polycrystalline cathode materials. Li6PS5Cl-infiltrated polycrystalline electrodes showed excellent retention performance and rate capability. Galvanostatic intermittent titration technique analysis and transmission electron microscopy of the single-crystalline electrode confirmed severe polarization and the presence of a rock-salt-structure layer in the cathode particles; these results indicated side reactions within the layered structure of the material. In contrast, composite electrodes consisting of polycrystalline cathode materials infiltrated with the solid electrolyte Li6PS5Cl showed excellent electrochemical performance owing to intimate electrode–electrolyte interfacial contact. The result from this study confirmed the critical influence of interface engineering and material morphology on the overall performance and stability of ASSBs and could facilitate the development of high-performance ASSBs in the future.https://doi.org/10.1038/s41427-024-00555-7
spellingShingle Junghwan Sung
Junyoung Heo
Dong-Hee Kim
Hawon Gu
Yung-Soo Jo
Heetaek Park
Jun-Ho Park
Jeong-Hee Choi
Yoon-Cheol Ha
Doohun Kim
Jun-Woo Park
Infiltration-driven performance enhancement of poly-crystalline cathodes in all-solid-state batteries
NPG Asia Materials
title Infiltration-driven performance enhancement of poly-crystalline cathodes in all-solid-state batteries
title_full Infiltration-driven performance enhancement of poly-crystalline cathodes in all-solid-state batteries
title_fullStr Infiltration-driven performance enhancement of poly-crystalline cathodes in all-solid-state batteries
title_full_unstemmed Infiltration-driven performance enhancement of poly-crystalline cathodes in all-solid-state batteries
title_short Infiltration-driven performance enhancement of poly-crystalline cathodes in all-solid-state batteries
title_sort infiltration driven performance enhancement of poly crystalline cathodes in all solid state batteries
url https://doi.org/10.1038/s41427-024-00555-7
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