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Atomic High-Spin Cobalt Unlocks Reversible Multi-Electron Transfer Chemistry for Superb Aqueous Zn-Mn Batteries
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DOI：10.1007/s40820-026-02328-z.png)
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Abstract
En 中文
To settle inherent irreversible phase transition and motivate re-dissolution of deposited “dead” MnO2 without acid and redox mediator addition, we introduced atomic-dispersed Co atoms with high-spin state into layered MnO2, denoted as Co–MnO2, via an in situ topological phase transformation strategy, thereby unlocking reversible multi-electron transfer chemistry for superb Zn–Mn batteries. Specifically, atomic-distributed Co atoms within Co–MnO2 effectively modulate [MnO6] octahedral symmetry and reduce Co–O bond covalency along with enhanced lattice oxygen activity. Based on this, high-spin Co (t2g4eg2) greatly mitigates the Jahn–Teller distortion as well as promotes electrolytic MnO2 deposited onto the cathode surface completely converted from adsorbed Mn2+ for inhibited “Mn dendrites”, achieving reversible MnO2/Mn3+ and electrolytic MnO2/Mn2+ reactions with highly thermodynamical favorability. Benefiting from the “two-step, three-electron” mechanism triggered by high-spin Co, Zn//Co–MnO2 battery delivers an outstanding capacity of 658 mAh g–1 and ultra-long lifespan over 15,000 cycles. This work reveals the critical role of transition-metal spin state modulation for energy-dense and durable Zn-MnO2 batteries with reversible multi-electron storage mechanisms.
Keywords:
Aqueous Zn battery
Atomic high-spin Co
Reversible MnO2 deposition/dissolution
Multi-electron transfer chemistry
High performance
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36.3
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2.6K
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3.6W
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