4.6 Article

Mitigating self-discharge and improving the performance of Mg-S battery in Mg[B(hfip)4]2 electrolyte with a protective interlayer

Journal

JOURNAL OF MATERIALS CHEMISTRY A
Volume 9, Issue 44, Pages 25150-25159

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ta06114c

Keywords

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Funding

  1. Federal Ministry of Education and Research (Bundesministerium fur Bildung und Forschung, BMBF) of Germany within the project MagSiMal [03XP0208]
  2. Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germanys Excellence Strategy [EXC 2154, 390874152]

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The research on magnesium-sulfur (Mg-S) battery has revealed that the spontaneous formation of magnesium polysulfide leads to severe self-discharge, but using graphene-polyaniline coated carbon cloth as a protective interlayer can effectively adsorb the polysulfide and inhibit the self-discharge, thereby improving the performance of the battery.
Magnesium-sulfur (Mg-S) battery is receiving much research attention because of its high theoretical energy density, low-cost and sustainable electrode materials. However, the major issues such as self-discharge, low sulfur utilization in cathode and magnesium anode passivation severely hamper the battery operation. In this study, spontaneous magnesium polysulfide formation is observed in the Mg[B(hfip)(4)](2), Mg(TFSI)(2)-MgCl2 electrolytes, which leads to severe self-discharge of Mg-S cells. Interestingly, unlike in lithium-sulfur battery, these magnesium polysulfides forms as crystalline magnesium polysulfide on the magnesium foil, which could escalate the self-discharge of the cells. The incorporation of graphene-polyaniline coated carbon cloth (GPN-PANI@CC) as a protective interlayer which effectively adsorbs the polysulfide and inhibit the self-discharge of Mg-S cells in the non-corrosive Mg[B(hfip)(4)](2) electrolyte. This interlayer not only improve the polysulfide retention in cathode but also the capacity values in Mg[B(hfip)(4)](2) electrolyte compared to Mg(TFSI)(2)-MgCl2 electrolyte. The cells with interlayer show the initial capacity of 1121 mA h g(-1) and maintained a capacity of 500 mA h g(-1) after 150 cycles with coulombic efficiency of >99%. This cell design strategy provides a promising approach for improving metal-sulfur batteries.

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