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<p><?tk 4?>Metal–organic frameworks (MOFs) have recently emerged as promising cathode materials for aqueous zinc-ion batteries (AZIBs) due to their tunable porosity and abundant redox-active sites. However, achieving high capacity together with fast Zn²⁺ transport and long-term structural stability remains a critical challenge. Herein, hierarchical porous ZnMOF-74 microspheres were synthesized through a controlled solution-mediated coordination strategy and systematically investigated as cathodes for aqueous zinc-ion batteries. Structural characterization reveals a highly crystalline MOF-74 framework assembled into interconnected microspherical architectures with a high specific surface area (~ 750&#xa0;m² g⁻¹) and hierarchical micro/mesoporosity, which facilitate electrolyte penetration and ion transport. When coupled with a Zn(OTf)₂ electrolyte, the ZnMOF-74 cathode delivers a high reversible capacity of ~ 332 mAh g⁻¹ and exhibits excellent rate capability with stable cycling over 1000 cycles and nearly 100% coulombic efficiency. Kinetic analysis demonstrates that the charge storage process is governed by a synergistic mechanism involving Zn²⁺ diffusion-controlled insertion and dominant pseudocapacitive contributions. Ex-situ XPS analysis further confirms reversible Zn²⁺ coordination within the MOF framework accompanied by dynamic evolution of Zn–O bonding environments. The enhanced electrochemical performance originates from the synergistic interplay between the hierarchical porous architecture and the favorable solvation chemistry of the Zn(OTf)₂ electrolyte, which collectively accelerate Zn²⁺ transport and stabilize the electrode–electrolyte interface. This work highlights the critical role of electrolyte engineering in unlocking the electrochemical potential of MOF-based cathodes and provides new insights into the design of high-performance materials for next-generation aqueous zinc-ion batteries.</p>

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Electrolyte-Driven Zn²⁺ Storage in Hierarchical ZnMOF-74 Cathodes for High-Performance Aqueous Zinc-Ion Batteries

  • 期刊论文

  • 发表日期：

    2026年6月22日

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  • Moufida Boukriba

摘要

Metal–organic frameworks (MOFs) have recently emerged as promising cathode materials for aqueous zinc-ion batteries (AZIBs) due to their tunable porosity and abundant redox-active sites. However, achieving high capacity together with fast Zn²⁺ transport and long-term structural stability remains a critical challenge. Herein, hierarchical porous ZnMOF-74 microspheres were synthesized through a controlled solution-mediated coordination strategy and systematically investigated as cathodes for aqueous zinc-ion batteries. Structural characterization reveals a highly crystalline MOF-74 framework assembled into interconnected microspherical architectures with a high specific surface area (~ 750 m² g⁻¹) and hierarchical micro/mesoporosity, which facilitate electrolyte penetration and ion transport. When coupled with a Zn(OTf)₂ electrolyte, the ZnMOF-74 cathode delivers a high reversible capacity of ~ 332 mAh g⁻¹ and exhibits excellent rate capability with stable cycling over 1000 cycles and nearly 100% coulombic efficiency. Kinetic analysis demonstrates that the charge storage process is governed by a synergistic mechanism involving Zn²⁺ diffusion-controlled insertion and dominant pseudocapacitive contributions. Ex-situ XPS analysis further confirms reversible Zn²⁺ coordination within the MOF framework accompanied by dynamic evolution of Zn–O bonding environments. The enhanced electrochemical performance originates from the synergistic interplay between the hierarchical porous architecture and the favorable solvation chemistry of the Zn(OTf)₂ electrolyte, which collectively accelerate Zn²⁺ transport and stabilize the electrode–electrolyte interface. This work highlights the critical role of electrolyte engineering in unlocking the electrochemical potential of MOF-based cathodes and provides new insights into the design of high-performance materials for next-generation aqueous zinc-ion batteries.