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Managing safety and supply-chain risks associated with lithium-ion batteries (LIBs) is an urgent task for sustainable development. Aqueous proton batteries are attractive alternatives to LIBs because using water and protons addresses these two risks. However, most host materials undergo large volume changes upon H+ intercalation, which induces intraparticle cracking to accelerates parasitic reactions. Herein, we report that Mo3Nb2O14 bronze exhibits　reversible H+ intercalation (200 mAh g−1) with a Coulombic efficiency of 99.7% owing to near-zero volume change and solid-solution-type phase transition. Combination of experimental and theoretical analyses clarifies that rotation and shrinkage of open tunnels, which consist of flexible corner-sharing Mo/NbOn polyhedra, relieve local structural distortions upon H+ intercalation to suppress intraparticle cracking. The prototype full cell of an aqueous proton battery with a Mo3Nb2O14 anode operates stably over 1000 charge/discharge cycles. This study reveals the importance of implementing distortion-relieving voids in host materials to reduce volume change upon charge/discharge.

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• In Copyright
  

  This is the peer reviewed version of the following article: K. Kawai, S.-H. Jang, Y. Igarashi, K. Yazawa, K. Gotoh, J. Kikkawa, A. Yamada, Y. Tateyama, M. Okubo, Angew. Chem. Int. Ed. 2025, 64, e202410971, which has been published in final form at https://doi.org/10.1002/anie.202410971. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.

Keyword: aqueous battery, proton, bronze oxides, molecular crowding electrolyte

Date published: 2025-01-15

Publisher: Wiley

Journal:

• Angewandte Chemie International Edition (ISSN: 14337851) vol. 64 issue. 3

Funding:

• Kazuchika Okura Memorial Foundation
• Core Research for Evolutional Science and Technology JPMJCR21O6
• Ministry of Education, Culture, Sports, Science and Technology JPMXP1121467561
• Ministry of Education, Culture, Sports, Science and Technology JPMXP1020200301
• Ministry of Education, Culture, Sports, Science and Technology JPMXP1020230325
• Ministry of Education, Culture, Sports, Science and Technology JP24H02204

Manuscript type: Author's version (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.5294

First published URL: https://doi.org/10.1002/anie.202410971

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Updated at: 2025-08-28 08:30:41 +0900

Published on MDR: 2025-08-28 08:18:04 +0900