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 journalArticle

272 Citations (Scopus)


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
Issue number6
Publication statusPublished - 23 Mar 2016
Externally publishedYes



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

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

Cite this

Liang, X., Kwok, C. Y., Lodi-Marzano, F., Pang, Q., Cuisinier, M., Huang, H., Hart, C. J., Houtarde, D., Kaup, K., Sommer, H., Brezesinski, T., Janek, J., & Nazar, L. F. (2016). Tuning Transition Metal Oxide-Sulfur Interactions for Long Life Lithium Sulfur Batteries: The "goldilocks" Principle. Advanced Energy Materials, 6(6), [1501636]. https://doi.org/10.1002/aenm.201501636