Atomic High-Spin Cobalt Unlocks Reversible Multi-Electron Transfer Chemistry for Superb Aqueous Zn-Mn Batteries.

Authors

Yajun Zhao, Qi Li, Yanan Lv, Shuoxiao Zhang, Kai Jiang, Meng Xu, Mudasir Muhammad, Yueyang Wang, Yang Ren, Yi Zhao, Xiaoming Sun

Published in

Nano-micro letters. Volume 19. Issue 1. Aug 10, 2026. Epub Aug 10, 2026.

Abstract

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 (t_2g⁴e_g²) 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.

PMID:
42572103
Bibliographic data and abstract were imported from PubMed on 10 Aug 2026.

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