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

236 Citations (Scopus)

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
Publication statusPublished - 23 Mar 2016
Externally publishedYes

Fingerprint

Transition metals
Sulfur
Tuning
Polysulfides
Oxides
Cathodes
Electrochemical cells
Energy storage
Cyclic voltammetry
Lithium sulfur batteries
sulfur monoxide
Spectroscopy
Oxidation-Reduction
polysulfide
Costs

Keywords

  • 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

Tuning Transition Metal Oxide-Sulfur Interactions for Long Life Lithium Sulfur Batteries : The "goldilocks" Principle. / Liang, Xiao; Kwok, Chun Yuen; Lodi-Marzano, Fernanda; Pang, Quan; Cuisinier, Marine; Huang, He; Hart, Connor J.; Houtarde, Diane; Kaup, Kavish; Sommer, Heino; Brezesinski, Torsten; Janek, Jürgen; Nazar, Linda F.

In: Advanced Energy Materials, Vol. 6, No. 6, 1501636, 23.03.2016.

Research output: Contribution to journalArticle

Liang, X, Kwok, CY, Lodi-Marzano, F, Pang, Q, Cuisinier, M, Huang, H, Hart, CJ, Houtarde, D, Kaup, K, Sommer, H, Brezesinski, T, Janek, J & Nazar, LF 2016, 'Tuning Transition Metal Oxide-Sulfur Interactions for Long Life Lithium Sulfur Batteries: The "goldilocks" Principle', Advanced Energy Materials, vol. 6, no. 6, 1501636. https://doi.org/10.1002/aenm.201501636
Liang, Xiao ; Kwok, Chun Yuen ; Lodi-Marzano, Fernanda ; Pang, Quan ; Cuisinier, Marine ; Huang, He ; Hart, Connor J. ; Houtarde, Diane ; Kaup, Kavish ; Sommer, Heino ; Brezesinski, Torsten ; Janek, Jürgen ; Nazar, Linda F. / Tuning Transition Metal Oxide-Sulfur Interactions for Long Life Lithium Sulfur Batteries : The "goldilocks" Principle. In: Advanced Energy Materials. 2016 ; Vol. 6, No. 6.
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