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DOE OSTI · 3001462

Five-volt-class high-capacity all-solid-state lithium batteries

Son, Jun Pyo [Yonsei Univ., Seoul (Korea, Republic of)]·Park, Juhyoun [Yonsei Univ., Seoul (Korea, Republic of)]·Kim, Hae-Yong [Dongguk Univ., Seoul (Korea, Republic of)] (ORCID:0009000020984279)·Kim, Jae-Seung [Korea Advanced Institute Science and Technology (KAIST), Daejeon (Korea, Republic of)] (ORCID:0000000330526444)·Song, Yong Bae [Yonsei Univ., Seoul (Korea, Republic of)]·Kim, Changhoon [Yonsei Univ., Seoul (Korea, Republic of)]·Kim, Donghyeok [Yonsei Univ., Seoul (Korea, Republic of)]·Kim, Jong Seok [Yonsei Univ., Seoul (Korea, Republic of)]·Lee, Junwoo [Yonsei Univ., Seoul (Korea, Republic of)]·Ko, Sunho [Dongguk Univ., Seoul (Korea, Republic of)] (ORCID:0009000791616140)·Jung, Soon-Jae [Ulsan National Institute of Science and Technology (UNIST), Ulsan (Korea, Republic of)]·Choi, Seungwoo [Ulsan National Institute of Science and Technology (UNIST), Ulsan (Korea, Republic of)]·Ahn, Docheon [Pohang Accelerator Laboratory (PAL) (Korea, Republic of)] (ORCID:0000000318415418)·Chae, Keun Hwa [Korea Institute of Science and Technology (KIST), Bucheon (Korea, Republic of)] (ORCID:000000033894670X)·Kwon, Gihan [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000279632136)·Wierzbicki, Dominik [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000305587405)·Du, Yonghua [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:000000032655045X)·Lee, Hyun-Wook [Ulsan National Institute of Science and Technology (UNIST), Ulsan (Korea, Republic of)] (ORCID:0000000190741619)·Seo, Dong-Hwa [Korea Advanced Institute Science and Technology (KAIST), Daejeon (Korea, Republic of)] (ORCID:0000000272007186)·Nam, Kyung-Wan [Dongguk Univ., Seoul (Korea, Republic of)] (ORCID:0000000162786369)·Jung, Yoon Seok [Yonsei Univ., Seoul (Korea, Republic of)] (ORCID:0000000303579508)

Abstract

Advances in battery technology have been impeded by the voltage constraints of electrolytes. Here, in this study, we present a high-energy all-solid-state battery design featuring >5 V operation and an ultrahigh areal capacity of 35.3 mAh cm −2 ; these attributes were enabled by a highly conductive and ultrahigh-voltage stable fluoride solid electrolyte, LiCl–4Li 2 TiF 6 (1.7 × 10 −5 S cm −1 at 30 °C). LiCl–4Li 2 TiF 6 shields high-voltage spinel oxide cathodes, achieving 106 mAh g −1 at 2C with 75.2% retention over 500 cycles for LiNi 0.5 Mn 1.5 O 4 , sharply contrasting with the conventional LiNbO 3 counterpart, which decomposes and fails to prevent detrimental interfacial degradation. The efficacy of LiCl–4Li 2 TiF 6 is validated across various systems, including LiCoMnO 4 , LiFe 0.5 Mn 1.5 O 4 and pouch-type LiNi 0.5 Mn 1.5 O 4 ||Li (or Ag–C) all-solid-state batteries, and further demonstrated by operability down to 2.3 V with 258 mAh g −1 and ultrathick 1.8-mm electrodes. This shielding layer with >5 V stability introduces a transformative design paradigm by revisiting the previously forbidden high-voltage cathodes.

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BibTeXRIS

Son, Jun Pyo [Yonsei Univ., Seoul (Korea, Republic of)], Park, Juhyoun [Yonsei Univ., Seoul (Korea, Republic of)], Kim, Hae-Yong [Dongguk Univ., Seoul (Korea, Republic of)] (ORCID:0009000020984279), Kim, Jae-Seung [Korea Advanced Institute Science and Technology (KAIST), Daejeon (Korea, Republic of)] (ORCID:0000000330526444), Song, Yong Bae [Yonsei Univ., Seoul (Korea, Republic of)], Kim, Changhoon [Yonsei Univ., Seoul (Korea, Republic of)], Kim, Donghyeok [Yonsei Univ., Seoul (Korea, Republic of)], Kim, Jong Seok [Yonsei Univ., Seoul (Korea, Republic of)], Lee, Junwoo [Yonsei Univ., Seoul (Korea, Republic of)], Ko, Sunho [Dongguk Univ., Seoul (Korea, Republic of)] (ORCID:0009000791616140), Jung, Soon-Jae [Ulsan National Institute of Science and Technology (UNIST), Ulsan (Korea, Republic of)], Choi, Seungwoo [Ulsan National Institute of Science and Technology (UNIST), Ulsan (Korea, Republic of)], Ahn, Docheon [Pohang Accelerator Laboratory (PAL) (Korea, Republic of)] (ORCID:0000000318415418), Chae, Keun Hwa [Korea Institute of Science and Technology (KIST), Bucheon (Korea, Republic of)] (ORCID:000000033894670X), Kwon, Gihan [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000279632136), Wierzbicki, Dominik [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000305587405), Du, Yonghua [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:000000032655045X), Lee, Hyun-Wook [Ulsan National Institute of Science and Technology (UNIST), Ulsan (Korea, Republic of)] (ORCID:0000000190741619), Seo, Dong-Hwa [Korea Advanced Institute Science and Technology (KAIST), Daejeon (Korea, Republic of)] (ORCID:0000000272007186), Nam, Kyung-Wan [Dongguk Univ., Seoul (Korea, Republic of)] (ORCID:0000000162786369), Jung, Yoon Seok [Yonsei Univ., Seoul (Korea, Republic of)] (ORCID:0000000303579508). 2025-10-03. Five-volt-class high-capacity all-solid-state lithium batteries. https://doi.org/10.1038/s41560-025-01865-y

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