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A Tandem Electrocatalysis of Sulfur Reduction by Bimetal 2D MOFs

机译:Bimetal 2D MOF的硫磺减少串联电催化

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摘要

The diversity and coupling of sulfur redox intermediates and its associated solid-liquid-solid multiphase conversion mechanism pose great challenges in designing a proper electrocatalysts for Li-S batteries. In this report, it is proposed that an ideal catalyst should possess two catalytic centers which catalyze liquid-liquid conversion and liquid-solid conversion in tandem within one structure, with the use of 2D MOF nanosheets with different metal centers for validation. It is uncovered that the Ni-MOF is more effective in catalyzing the reduction of long-chain polysulfides, while Co-MOF benefits the Li2S deposition kinetics. Moreover, synergistic sulfur electrocatalytic activity for the integrated bimetal CoNi-MOF is witnessed. It greatly decreases the reaction activation energies, accelerates the faradaic current density for both of the reaction regions, and effectively inhibits the shuttle effect. This is attributed to charge redistribution between Ni and Co via bridge O in the MOF structure. The S@CoNi-MOF composite endows high reversible capacity (1450 mAh g(-1) at 0.1 C), enhanced cycling stability (500 cycles at 1 C with a low-capacity decay rate of 0.036% per cycle), and improved rate capability.
机译:硫磺氧化还原中间体的多样性和偶联及其相关的固体 - 固体多相转化机理在设计Li-S电池的适当电池时造成巨大挑战。在本报告中,提出了理想的催化剂应具有两个催化中心,其在一种结构中串联催化液 - 液转化和液体固体转化率,使用2D MOF纳米片与不同的金属中心进行验证。揭示Ni-MOF在催化长链多硫化物的还原时更有效,而CO-MOF有益于LI2S沉积动力学。此外,目睹了集成双金属锥体的协同硫催化活性。它大大降低了反应激活能量,加速了两种反应区的游览电流密度,有效地抑制了梭效果。这归因于MOF结构中的NI和CO之间的电荷再分配。 S @ Coni-Mof复合材料赋予高可逆容量(0.1℃的1450mAh(-1)),增强循环稳定性(1℃下的500个循环,低容量衰减率为0.036%,每循环0.036%)和提高速率能力。

著录项

  • 来源
    《Advanced energy materials》 |2021年第47期|2102819.1-2102819.11|共11页
  • 作者单位

    Hunan Univ Coll Chem & Chem Engn Adv Catalyt Engn Res Ctr Minist Educ State Key Lab Chem Biosensing & Chemometr Changsha 410082 Peoples R China;

    Hunan Univ Coll Chem & Chem Engn Adv Catalyt Engn Res Ctr Minist Educ State Key Lab Chem Biosensing & Chemometr Changsha 410082 Peoples R China;

    Hunan Univ Coll Chem & Chem Engn Adv Catalyt Engn Res Ctr Minist Educ State Key Lab Chem Biosensing & Chemometr Changsha 410082 Peoples R China;

    Hunan Univ Coll Chem & Chem Engn Adv Catalyt Engn Res Ctr Minist Educ State Key Lab Chem Biosensing & Chemometr Changsha 410082 Peoples R China;

    Chinese Acad Sci Inst High Energy Phys Beijing 100049 Peoples R China;

    Hunan Univ Coll Chem & Chem Engn Adv Catalyt Engn Res Ctr Minist Educ State Key Lab Chem Biosensing & Chemometr Changsha 410082 Peoples R China;

    Hunan Univ Coll Chem & Chem Engn Adv Catalyt Engn Res Ctr Minist Educ State Key Lab Chem Biosensing & Chemometr Changsha 410082 Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    bimetal 2D MOF; polysulfides; synergic catalysis; tandem catalysis;

    机译:双金属2d mof;多硫化物;协同催化;串联催化;

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