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Developing bifunctional electrocatalysts with superior oxygen evolution and reduction reaction (OER/ORR) activity and high durability is crucial for rechargeable metal-air batteries. Transition-metal-based layered double hydroxides (LDHs) are promising in the application as cost-effective and high-performance air cathodes. Herein, hierarchical composites of ZIF-derived CoNiFe LDH nanocages in-situ grown on Ag nanowires (CoNiFe LDH@Ag NWs) are synthesized as carbon-free bifunctional oxygen electrocatalysts. The hollow structure of LDH and heterointerface with conductive Ag substrate not only maximizes exposure of active sites, but also ensures effective electron transfer. In addition, the hybridization with Ag induces structural disorder and unsaturated coordination in the LDH shells, thereby enhancing intrinsic catalytic activity. Theoretical calculations reveal that incorporation of Ag species could tune the electronic states and reduce the reaction barriers of OER and ORR. As a result, CoNiFe LDH@Ag NWs exhibit a bifunctional overpotential of 0.63 V. Applied as a carbon-free cathode in zinc-air battery, CoNiFe LDH@Ag NWs yields a high specific capacity of 808 mAh g−1 and long cycling stability up to 300 h. This work provides new insight into the design of LDH hierarchical structure for efficient and durable electrocatalysts.

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  This is the peer reviewed version of the following article: Z. Zhang, R. Zhang, N. Ma, E. Picheau, L. K. Shrestha, W. Zhou, X. Liu, Y. Sugahara, T. Sasaki, R. Ma, Hierarchical Structure Design of ZIF-Derived CoNiFe LDH Nanocages Grown on Ag Nanowires as High-Performance Cathode for Zn-Air Batteries. Small 2025, 21, 2502344, which has been published in final form at https://doi.org/10.1002/smll.202502344. 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: Layered double hydroxide, Ag nanowires, Structure disorder, Bifunctional oxygen electrocatalyst, , Zn-air batteries

Date published: 2025-04-14

Publisher: Wiley

Journal:

• Small (ISSN: 16136810) vol. 21 issue. 23

Funding:

• Japan Society for the Promotion of Science 22H01916
• Japan Society for the Promotion of Science 22K18956

Manuscript type: Author's version (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.5546

First published URL: https://doi.org/10.1002/smll.202502344

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Updated at: 2025-06-24 16:36:32 +0900

Published on MDR: 2026-04-14 08:24:26 +0900