This study presents the development of a composite electrode material for lithium-sulphur (Li-S) batteries, combining MOF-74 with carbon black and sulphur. The MOF-74 structures, incorporating Ni(II), Mg(II), and Fe(II) metal ions, were synthesized via a solvothermal method and used to encapsulate sulphur. The microporous nature of MOF-74 facilitates the physical confinement and storage of sulphur, potentially enhancing the performance of Li-S batteries. The investigation focuses on how different central metal ions in MOF-74 influence the performance of sulphur-based electrodes. Among the metal ions studied, Fe(II) and Mg(II) were selected for their low toxicity, cost-effectiveness, and availability, while Ni(II) was included for its high catalytic properties. The materials were thoroughly characterized using infrared spectroscopy, thermogravimetric analysis, scanning electron microscopy, powder X-ray diffraction, elemental analysis and X-ray photoelectron spectroscopy. The thermal stability and textural properties of the materials were assessed, showing that MOF-74(Mg) exhibited the highest stability, followed by MOF-74(Ni) and MOF-74(Fe). Nitrogen adsorption/desorption measurements indicated that the specific surface area and pore volume varied with activation temperature, impacting the material's performance. Among the tested materials, MOF-74(Ni) exhibited the strongest interaction with sulfur, as confirmed by XPS analysis. Electrochemical tests revealed that the S/MOF-74(Ni) electrode demonstrated superior stability and capacity retention with a minimal capacity fading rate of 0.001% per cycle over 200 cycles, achieving a reversible capacity of 465 mAh g-1 and a capacity retention of 99.75%. In contrast, the S/MOF-74(Fe) electrode showed significantly reduced performance. A structure-performance correlation was established to assess sulfur interaction, electrode stability, and degradation behavior. Overall, the results highlight that MOF-74(Ni) offers the most promising performance due to its effective sulphur immobilization and superior electrochemical properties compared to MOF-74(Mg) and MOF-74(Fe).

CNRS MADIREL Aix Marseille University 133 97 Marseille France

Department of Chemical Sciences Bernal Institute University of Limerick Limerick V94 T9PX Ireland

Department of Electrical and Electronic Technology Faculty of Electrical Engineering and Communication Brno University of Technology Technická 10 616 00 Brno Czech Republic

Department of Inorganic Chemistry Faculty of Sciences Pavol Jozef Šafárik University in Košice Moyzesova 11 040 01 Kosice Slovak Republic

Department of Physical Chemistry Faculty of Sciences Pavol Jozef Šafárik University in Košice Moyzesova 11 040 01 Kosice Slovak Republic

Department of Solid State Physics Faculty of Sciences Pavol Jozef Šafárik University in Košice Park Angelinum 9 040 01 Kosice Slovak Republic

Faculty of Chemistry Jagiellonian University Gronostajowa 2 30 387 Kraków Poland

Institute of Experimental Physics Slovak Academy of Sciences Watsonova 47 040 01 Kosice Slovak Republic

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