Lattice-level defect engineering of dense Mn2O3 hosts unlocks fast H+/Zn2+ storage and long-life aqueous zinc-ion batteries Yu, Ao Chang, Xingqi Lu, Xuan He, Ren Yang, Linlin Chai, Jiali Bi, Xiaoyu Chacón-Borrero, Jesús Mejia-Centeno, Karol V. Llorca, Jordi Villalobos-Portillo, Eduardo Liu, Qirong Shang, Jian Cabot, Andreu Manganese-based aqueous zinc-ion batteries (AZIBs) have emerged as promising candidates for large-scale energy storage owing to their low cost, intrinsic safety, and the abundance of constituent elements. However, their practical deployment is still restricted by severe capacity fading caused by Jahn–Teller-induced structural instability and sluggish Zn2+ transport in the cathode. Although surface coating, heteroatom doping, and structural regulation have been widely explored to improve Mn-based cathodes, these approaches may suffer from increased interfacial resistance, compositional complexity, or limited control over the intrinsic electronic structure. In this context, oxygen-vacancy engineering offers a more direct route to modulate local coordination environments and accelerate Zn2+/H+ storage kinetics. Herein, lattice-level defect engineering of a dense Mn2O3 host is achieved through a metal–organic framework-derived synthesis followed by mild secondary annealing. The introduced oxygen vacancies regulate the local electronic structure and coordination environment, thereby facilitating Zn2+ diffusion, accelerating charge-transfer kinetics, and improving electrochemical reversibility. Combined experimental and theoretical investigations further show that oxygen-vacancy engineering enhances electronic conductivity, reduces the Zn2+ migration barrier, and enables a reversible dual-ion storage mechanism involving both H+ and Zn2+. Benefiting from these effects, the Zn‖Vo-Mn2O3 battery delivers a high specific capacity of 359 mAh g−1 at 0.3 A g−1, maintains 210 mAh g−1 at 6 A g−1, and retains 74.3% of its capacity after 10 000 cycles at 12 A g−1 after only 150 s of initial preconditioning. This work highlights oxygen-vacancy engineering as an effective route to enhancing the kinetic and structural stability of Mn-based cathodes for advanced AZIBs. Royal Society of Chemistry 2026 info:eu-repo/semantics/article doc-type:Article Article http://purl.org/coar/resource_type/c_2df8fbb1 https://research-explorer.ista.ac.at/record/22965 Yu A, Chang X, Lu X, et al. Lattice-level defect engineering of dense Mn2O3 hosts unlocks fast H+/Zn2+ storage and long-life aqueous zinc-ion batteries. <i>Journal of Materials Chemistry A</i>. 2026. doi:<a href="https://doi.org/10.1039/d6ta05844b">10.1039/d6ta05844b</a> eng info:eu-repo/semantics/altIdentifier/doi/10.1039/d6ta05844b info:eu-repo/semantics/altIdentifier/issn/2050-7488 info:eu-repo/semantics/altIdentifier/e-issn/2050-7496 info:eu-repo/semantics/closedAccess