Inorg Chem 2024 Oct 21;6342:19835-19846. doi: 10.1021/acs.inorgchem.4c03195.

Bimetallic NiCo@C with a Hollow Sea Urchin Structure Enables Li-S Batteries to Hasten the Reaction Kinetics and Effectively Inhibit the Shuttling of Polysulfides.

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The "shuttle effect" and several issues related to it are seen as "obstacles" to the study and development of lithium-sulfur batteries (LSBs). This work aims at finding how to fully expose bimetallic sites and quicken the battery reaction kinetics. Here, a bimetallic NiCo-MOF and its derivative NiCo@C with a hollow sea urchin structure are produced. The obtained NiCo@C possesses a micromesoporous structure and fully disclosed bimetallic active sites because of its distinctive structure. The experimental findings demonstrate that fully exposed bimetallic active sites take on chemical adsorbents and collaborate with micromesopores as physical constraints to effectively suppress the "shuttle effect". Furthermore, the hollow sea urchin structure of NiCo@C enables a highly conductive grid, which provides channels to facilitate the movement of solvated Li+. Thanks to these advantages, the NiCo@C-based sulfur cathode offers a high initial discharge specific capacity of 924.41 mAh g-1 at 0.1 C and sustains 390.35 mAh g-1 discharge specific capacity after 100 cycles. The quick transfer of solvated lithium ions (DLi+ = 1.81 × 10-8 cm2 s-1) enables the battery to still contribute a discharge specific capacity of 367.54 mAh g-1 at 1 C. This work provides a new understanding for the structural design of positive electrodes in LSBs.

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