Inhibiting irreversible Zn²⁺/H⁺ co-insertion chemistry in aqueous zinc-MoOₓ batteries for enhanced capacity stability

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dc.contributor.authorZheng, C.
dc.contributor.authorGuan, X.
dc.contributor.authorHuang, Z.
dc.contributor.authorMao, S.
dc.contributor.authorHan, X.
dc.contributor.authorDuan, X.
dc.contributor.authorLi, H.
dc.contributor.authorMa, T.
dc.date.issued2025
dc.description.abstractRechargeable aqueous Zn-MoOₓ batteries are promising energy storage devices with high theoretical specific capacity and low cost. However, MoO₃ cathodes suffer drastic capacity decay during the initial discharging/charging process in conventional electrolytes, resulting in a short cycle life and challenging the development of Zn-MoOₓ batteries. Here we comprehensively investigate the dissolution mechanism of MoO₃ cathodes and innovatively introduce a polymer to inhibit the irreversible processes. Our findings reveal that this capacity decay originates from the irreversible Zn²⁺/H⁺ co-intercalation/extraction process in aqueous electrolytes. Even worse, during Zn²⁺ intercalation, the formed ZnₓMoO₃−x intermediate phase with lower valence states (Mo⁵⁺/Mo⁴⁺) experiences severe dissolution in aqueous environments. To address these challenges, we developed a first instance of coating a polyaniline (PANI) shell around the MoO₃ nanorod effectively inhibiting these irreversible processes and protecting structural integrity during long-term cycling. Detailed structural analysis and theoretical calculations indicate that =N– groups in PANI@MoO₃−x simultaneously weaken H+ adsorption and enhance Zn²⁺ adsorption, which endowed the PANI@MoO₃−x– cathode with reversible Zn²⁺/H⁺ intercalation/extraction. Consequently, the obtained PANI@MoO₃−x cathode delivers an excellent discharge capacity of 316.86 mA hg¯¹ at 0.1 A g¯¹ and prolonged cycling stability of 75.49% capacity retention after 1000 cycles at 5 A g¯¹. This work addresses the critical issues associated with MoO₃ cathodes and significantly advances the understanding of competitive multi-ion energy storage mechanisms in aqueous Zn-MoO₃ batteries.
dc.description.statementofresponsibilityChen Zheng, Xinwei Guan, Zihang Huang, Shuai Mao, Xu Han, Xiaoguang Duan, Hui Li, Tianyi Ma
dc.identifier.citationJournal of Energy Chemistry, 2025; 102:98-106
dc.identifier.doi10.1016/j.jechem.2024.10.034
dc.identifier.issn2095-4956
dc.identifier.issn2095-4956
dc.identifier.orcidDuan, X. [0000-0001-9635-5807]
dc.identifier.urihttps://hdl.handle.net/2440/144986
dc.language.isoen
dc.publisherElsevier
dc.relation.granthttp://purl.org/au-research/grants/arc/FT210100298
dc.relation.granthttp://purl.org/au-research/grants/arc/DP220100603
dc.relation.granthttp://purl.org/au-research/grants/arc/LP210200504
dc.relation.granthttp://purl.org/au-research/grants/arc/LP220100088
dc.relation.granthttp://purl.org/au-research/grants/arc/LP230200897
dc.relation.granthttp://purl.org/au-research/grants/arc/IH240100009
dc.rights© 2024 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
dc.source.urihttp://dx.doi.org/10.1016/j.jechem.2024.10.034
dc.subjectco-insertion chemistry; surface modification engineering; molybdenum oxide; cycling stability; aqueous zinc battery
dc.titleInhibiting irreversible Zn²⁺/H⁺ co-insertion chemistry in aqueous zinc-MoOₓ batteries for enhanced capacity stability
dc.typeJournal article
pubs.publication-statusPublished

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