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

Son, Jun Pyo; Park, Juhyoun; Kim, Hae-Yong; Kim, Jae-Seung; Song, Yong Bae; Kim, Changhoon; Kim, Donghyeok; Kim, Jong Seok; Lee, Junwoo; Ko, Sunho; Jung, Soon-Jae; Choi, Seungwoo; Ahn, Docheon; Chae, Keun Hwa; Kwon, Gihan; Wierzbicki, Dominik; Du, Yonghua; Lee, Hyun-Wook; Seo, Dong-Hwa; Nam, Kyung-Wan; Jung, Yoon Seok

doi:10.1038/s41560-025-01865-y

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

Journal Article · Fri Oct 03 00:00:00 UTC 2025 · Nature Energy

DOI: https://doi.org/10.1038/s41560-025-01865-y · OSTI ID:3001462

Son, Jun Pyo ^[1]; Park, Juhyoun ^[1];

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^[3]; Song, Yong Bae ^[1]; Kim, Changhoon ^[1]; Kim, Donghyeok ^[1]; Kim, Jong Seok ^[1]; Lee, Junwoo ^[1];

^[2]; Jung, Soon-Jae ^[4]; Choi, Seungwoo ^[4];

^[5];

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^[2] more »

Yonsei Univ., Seoul (Korea, Republic of)
Dongguk Univ., Seoul (Korea, Republic of)
Korea Advanced Institute Science and Technology (KAIST), Daejeon (Korea, Republic of)
Ulsan National Institute of Science and Technology (UNIST), Ulsan (Korea, Republic of)
Pohang Accelerator Laboratory (PAL) (Korea, Republic of)
Korea Institute of Science and Technology (KIST), Bucheon (Korea, Republic of)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

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–4Li₂TiF₆ (1.7 × 10⁻⁵ S cm⁻¹ at 30 °C). LiCl–4Li₂TiF₆ shields high-voltage spinel oxide cathodes, achieving 106 mAh g⁻¹ at 2C with 75.2% retention over 500 cycles for LiNi_0.5Mn_1.5O₄, sharply contrasting with the conventional LiNbO₃ counterpart, which decomposes and fails to prevent detrimental interfacial degradation. The efficacy of LiCl–4Li₂TiF₆ is validated across various systems, including LiCoMnO₄, LiFe_0.5Mn_1.5O₄ and pouch-type LiNi_0.5Mn_1.5O₄||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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Research Organization:: Brookhaven National Lab; Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: Brookhaven National Lab; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 3001462

Report Number(s):: BNL--229103-2025-JAAM; BNL-229116-2025-JAAM

Journal Information:: Nature Energy, Journal Name: Nature Energy Vol. 10; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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

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