Mediator-Assisted Catalysis of Polysulfide Conversion for High-Loading Lithium-Sulfur Batteries Operating Under the Lean Electrolyte Condition

The kinetics of S <-> Li2S conversion in lithium-sulfur (Li-S) batteries can be improved with electrocatalysts to increase the application performance. The effectiveness of electrocatalysis reduces under the lean electrolyte condition due to the preponderance of solid reaction products (sulfur and Li2S) in a small amount of electrolyte; and the difficulty of catalyzing solid sulfur and Li2S. In this report, we describe the development of a mediated catalytic pathway in which a solid cathode catalyst is used alongside a soluble mediator to enable a cooperative catalysis that increases the sulfur utilization from 44% to 61% for high-loading (5.6 mg cm(-2)) lean-electrolyte (5.0 mu L mg(-1)) Li-S batteries. The improved sulfur utilization is due primarily to the mediator working as a scavenger to capture and reutilize the otherwise inactive sulfur species (S/Li2S) in the cathode. Mediated catalysis is therefore a new strategy to noticeably improve polysulfide catalysis and sulfur utilization beyond what is possible with conventional use of catalysts.

Automated summary

This report discusses the development of a mediated catalytic pathway which utilizes a mediator to capture and reuse inactive sulfur species in the cathode to increase sulfur utilization in lithium-sulfur batteries. This mediated catalysis is a new strategy to significantly improve polysulfide catalysis and sulfur utilization beyond conventional catalyst use.