Accelerated Kinetics of Desolvation and Redox Transformation Enabled by MOF Sieving for High-Loading Mg-S Battery

文献类型： 外文期刊

第一作者： Guan, Qinghua

作者： Guan, Qinghua;Cheng, Shuang;Lin, Hongzhen;Guan, Qinghua;Cheng, Shuang;Lin, Hongzhen;Wang, Jian;Wang, Jian;Wang, Jian;Zhuang, Quan;Xu, Wenlong;Zhang, Jing;Liu, Meinan;Zhang, Yongzheng

作者机构：

关键词： interfacial desolvation; magnesium-sulfur battery; molecular catalysis; pore sieving; sulfur conversion kinetics

期刊名称：ADVANCED FUNCTIONAL MATERIALS （ 影响因子：19.0； 五年影响因子：19.4 ）

ISSN： 1616-301X

年卷期： 2025 年

页码：

收录情况： SCI

摘要： Magnesium-sulfur (Mg-S) batteries have attracted growing interest as a promising candidate of post-lithium-ion battery systems due to their high energy density, natural abundance of Mg and S, and superior safety. However, they are severely inhibited by the sluggish electrochemical kinetics of interfacial Mg2+ desolvation and successive sulfur redox species conversions, leading to dissatisfactory "shuttling effect". Herein, a strategy of combining porous sieve desolvation and molecular electrocatalysis is proposed to dissociate Mg2+-solvents structure, stimulate free Mg2+ diffusion, and further improve the kinetics of sulfur redox conversion. As a protocol, the metal-organic frameworks (MOF) of representative MIL-101(Cr) with pore structure is capable of sieving larger Mg(solvents)(x)(2+) cluster to release free Mg2+ to react with sulfur species, and also the Lewis acid site of central Cr(III) can effectively adsorb and transform polysulfides, as thoroughly revealed by experimental and in situ/ex situ characterizations. Consequently, the as-fabricated Mg-S batteries employed with MIL-101(Cr)-decorated separator can deliver the capacity of 974 mA h g(-1) after 250 cycles, and exhibit a high-rate performance of 694 mA h g(-1) at 2 C. Impressively, the high-mass-loading cell of 6.4 mg cm(-2) stabilizes for more than 60 cycles, demonstrating the polar MOF with pore sieving effect for practical application of Mg-S batteries.

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