Dual Role of Mo<sub>6</sub>S<sub>8</sub> in Polysulfide Conversion and Shuttle for Mg–S Batteries

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  • Liping Wang
    Helmholtz Institute Ulm (HIU) Electrochemical Energy Storage Helmholtzstrasse 11 Ulm D‐89081 Germany
  • Piotr Jankowski
    Department of Energy Conversion and Storage Technical University of Denmark Kongens Lyngby 2800 Denmark
  • Christian Njel
    Institute for Applied Materials‐Energy Storage Systems (IAM‐ESS) and Karlsruhe Nano Micro Facility (KNMF) Karlsruhe Institute of Technology (KIT) Hermann‐von‐Helmholtz‐Platz 1 Eggenstein‐Leopoldshafen D‐76344 Germany
  • Werner Bauer
    Institute for Applied Materials‐Energy Storage Systems (IAM‐ESS) and Karlsruhe Nano Micro Facility (KNMF) Karlsruhe Institute of Technology (KIT) Hermann‐von‐Helmholtz‐Platz 1 Eggenstein‐Leopoldshafen D‐76344 Germany
  • Zhenyou Li
    Helmholtz Institute Ulm (HIU) Electrochemical Energy Storage Helmholtzstrasse 11 Ulm D‐89081 Germany
  • Zhen Meng
    Helmholtz Institute Ulm (HIU) Electrochemical Energy Storage Helmholtzstrasse 11 Ulm D‐89081 Germany
  • Bosubabu Dasari
    Helmholtz Institute Ulm (HIU) Electrochemical Energy Storage Helmholtzstrasse 11 Ulm D‐89081 Germany
  • Tejs Vegge
    Department of Energy Conversion and Storage Technical University of Denmark Kongens Lyngby 2800 Denmark
  • Juan Maria García Lastra
    Department of Energy Conversion and Storage Technical University of Denmark Kongens Lyngby 2800 Denmark
  • Zhirong Zhao‐Karger
    Helmholtz Institute Ulm (HIU) Electrochemical Energy Storage Helmholtzstrasse 11 Ulm D‐89081 Germany
  • Maximilian Fichtner
    Helmholtz Institute Ulm (HIU) Electrochemical Energy Storage Helmholtzstrasse 11 Ulm D‐89081 Germany

Description

<jats:title>Abstract</jats:title><jats:p>Magnesium–Sulfur batteries are one of most appealing options among the post‐lithium battery systems due to its potentially high energy density, safe and sustainable electrode materials. The major practical challenges are originated from the soluble magnesium polysulfide intermediates and their shuttling between the electrodes, which cause high overpotentials, low sulfur utilization, and poor Coulombic efficiency. Herein, a functional Mo<jats:sub>6</jats:sub>S<jats:sub>8</jats:sub> modified separator is designed to effectively address these issues. Both the experimental results and density functional theory calculations show that the electrochemically active Mo<jats:sub>6</jats:sub>S<jats:sub>8</jats:sub> layer has a superior adsorption capability of polysulfides and simultaneously acts as a mediator to accelerate the polysulfide conversion kinetics. Remarkably, the magnesium–sulfur cell assembled with the functional separator delivers a high specific energy density (942.9 mA h g<jats:sup>−1</jats:sup> in the 1st cycle) and can be cycled at 0.2 C for 200 cycles with a Coulombic efficiency of 96%. This work demonstrates a new design concept toward high‐performance metal–sulfur batteries.</jats:p>

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