Tuning Transition Metal Oxide-Sulfur Interactions for Long Life Lithium Sulfur Batteries: The "goldilocks" Principle

Xiao Liang, Chun Yuen Kwok, Fernanda Lodi-Marzano, Quan Pang, Marine Cuisinier, He Huang, Connor J. Hart, Diane Houtarde, Kavish Kaup, Heino Sommer, Torsten Brezesinski, Jürgen Janek, Linda F. Nazar

Research output: Contribution to journalArticlepeer-review

718 Scopus citations

Abstract

The lithium-sulfur battery is a compelling energy storage system because its high theoretical energy density exceeds Li-ion batteries at much lower cost, but applications are thwarted by capacity decay caused by the polysulfide shuttle. Here, proof of concept and the critical metrics of a strategy to entrap polysulfides within the sulfur cathode by their reaction to form a surface-bound active redox mediator are demonstrated. It is shown through a combination of surface spectroscopy and cyclic voltammetry studies that only materials with redox potentials in a targeted window react with polysulfides to form active surface-bound polythionate species. These species are directly correlated to superior Li-S cell performance by electrochemical studies of high surface area oxide cathodes with redox potentials below, above, and within this window. Optimized Li-S cells yield a very low fade rate of 0.048% per cycle. The insight gained into the fundamental surface mechanism and its correlation to the stability of the electrochemical cell provides a bridge between mechanistic understanding and battery performance essential for the design of high performance Li-S cells.

Original languageEnglish
Article number1501636
JournalAdvanced Energy Materials
Volume6
Issue number6
DOIs
StatePublished - Mar 23 2016
Externally publishedYes

Funding

This research was supported by the BASF International Scientific Network for Electrochemistry and Batteries. L.F.N. also thanks NSERC for generous support via a Canada Research Chair. L.F.N. thanks Ralf Steudel (TU Berlin) for helpful discussions. The spelling of author name Quan Pang was updated on April 4, 2016.

Keywords

  • Li-S batteries
  • polythionate
  • redox potential
  • sulfur hosts
  • transition metal oxides

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