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Updated: Mar 11, 2026
Author Spotlight: Magnetometric Characterization of Intermediates in the Solid-State Electrochemistry of Redox-Active Metal-Organic Frameworks
Published on: June 9, 2023
Unlocking Synergistic Ligand-Metal Interplay in Dual Redox-Active Metal-Organic Framework for High-Efficiency and
Partha Pratim Mondal1,2, Suprobhat Singha Roy1,3, Rudra Chand1,2
1Academy of Scientific and Innovative Research (AcSIR), Ghaziabad 201002, India.
None:
The development of bifunctional electrocatalysts that efficiently operate for both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in a single electrolyte under high current density remains a critical challenge toward applied overall water splitting. Herein, we designed a robust and microporous Co(II)-based nonpenetrating metal-organic framework (MOF) via juxtaposition of redox-active naphthalenediimide linker and π-electron rich C2-symmetric dicarboxylate ligand that features in situ-generated [Co2(COO)4] chain and exhibits high thermo-chemical stability. The efficient charge-mediating architecture upon interface engineering with conductive nickel foam (NF) delivers remarkable bifunctional water splitting activity in an alkaline medium (1 M KOH), achieving an industrially relevant current density of 100 mA·cm-2 with low overpotentials of 313 mV (OER) and 263 mV (HER). Importantly, rapid reaction kinetics, minimal charge-transfer resistance, and >95% Faradaic efficiency outperform the majority of contemporary as well as benchmark materials. The catalyst demonstrated excellent electrochemical durability in both water oxidation and reduction reactions for over 40 h and retains its structural and morphological attributes after prolonged chronoamperometric operation, demonstrating high-performance water splitting. Performance comparison with an isostructural Cd-MOF analogue confirms the essential contribution of ligand-metal synergism in the Co-MOF for much enhanced redox articulation and electrocatalysis. When deployed as both electrodes, the bifunctional MOF/NF system efficiently catalyzes overall water splitting with only 1.678 V cell voltage at 10 mA·cm-2, marking it among the leading MOF-based electrocatalysts. The findings highlight the pivotal role of ligand-metal cooperativity and hierarchical interface engineering in boosting the electrochemical efficacy of MOF catalysts and provide a promising strategy in designing next-generation bifunctional electrocatalysts for sustainable energy applications.
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