A highly efficient polysulfide mediator for lithium–sulfur batteries
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Abstract
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.
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The record
- Venue
- Nature Communications
- Topic
- Advanced Battery Materials and Technologies
- Field
- Engineering
- Canadian institutions
- University of Waterloo
- Funders
- Natural Sciences and Engineering Research Council of Canada
- Keywords
- PolysulfideNanosheetSulfurLithium (medication)DissolutionChemistryInorganic chemistryDisproportionationOxideRedoxManganeseMaterials scienceThiosulfateChemical engineeringNanotechnologyElectrodeOrganic chemistryCatalysisElectrolyte
- Has abstract in OpenAlex
- yes