A highly efficient polysulfide mediator for lithium–sulfur batteries

By Xiao Liang, Connor J. Hart, Q. Pang, A. Garsuch, T. Weiss, L. Nazar. Nature Communications, 2015

1,825 citations recorded by the source corpus.

The lithium–sulfur battery is receiving intense interest because its theoretical energy density exceeds that of lithium-ion batteries at much lower cost, but practical applications are still hindered by capacity decay caused by the polysulfide shuttle. Here we report a strategy to entrap polysulfides in the cathode that relies on a chemical process, whereby a host—manganese dioxide nanosheets serve as the prototype—reacts with initially formed lithium polysulfides to form surface-bound intermediates. These function as a redox shuttle to catenate and bind ‘higher’ polysulfides, and convert them on reduction to insoluble lithium sulfide via disproportionation. The sulfur/manganese dioxide nanosheet composite with 75 wt% sulfur exhibits a reversible capacity of 1,300 mA h g−1 at moderate rates and a fade rate over 2,000 cycles of 0.036%/cycle, among the best reported to date. We furthermore show that this mechanism extends to graphene oxide and suggest it can be employed more widely. The polysulfide shuttle is a major problem leading to capacity decay in lithium–sulfur batteries. Here, the authors show that in-situ-generated thiosulfate species on a manganese oxide nanosheet act as a polysulfide mediator, which effectively prevents polysulfide dissolution, leading to enhanced cyclability.

Subfields: Automotive Engineering, Electrical and Electronic Engineering

View Paper: https://www.semanticscholar.org/paper/8175b5433bace9a32f982220f3def2cbe2e7fad5

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