Insights into the role of interphasial morphology on the electrochemical performance of lithium electrodes

Carmen M. López, John T. Vaughey, Dennis W. Dees

Research output: Contribution to journalArticle

24 Citations (Scopus)

Abstract

With a theoretical specific capacity of 3862 mAhg and other desirable properties such as high voltage, light weight, and high energy density, metallic lithium remains one of the materials of greatest promise for advanced battery applications. However, the complicated reactivity of this electrode with most practical battery electrolytes leads to substantial morphological and chemical changes that affect the safety and efficiency of the system, and have prevented its further implementation on rechargeable batteries. In this work we demonstrate how to establish a direct and systematic relationship between such morphological changes in the lithium electrode and the cycle performance of the battery. We demonstrate that the main morphological changes are associated with the decomposition of the redox-formed SEI layer, which follows different electrochemical pathways leading to different morphologies depending on the cycling rate of the cell. At high cycling rates (i ≥ 0.16 mAcm-2), a three-layer morphology (dendritic layer, porous layer, residual lithium layer) is observed. At low cycling rates (i < 0.16 mAcm-2), polymerization of electrolytes solvents and gas evolution leading to macroscopic bubble clusters is observed. Furthermore, we demonstrate the advantages of using these systematic morphology-property relationships to fit and interpret complicated electrochemical impedance spectroscopy (EIS) data.

Original languageEnglish
JournalJournal of the Electrochemical Society
Volume159
Issue number6
DOIs
Publication statusPublished - 2012
Externally publishedYes

Fingerprint

Lithium
lithium
electric batteries
Electrolytes
Electrodes
electrodes
cycles
Secondary batteries
Electrochemical impedance spectroscopy
electrolytes
gas evolution
Gases
Polymerization
Decomposition
Electric potential
high voltages
safety
bubbles
polymerization
reactivity

ASJC Scopus subject areas

  • Electrochemistry
  • Electronic, Optical and Magnetic Materials
  • Materials Chemistry
  • Surfaces, Coatings and Films
  • Renewable Energy, Sustainability and the Environment
  • Condensed Matter Physics

Cite this

Insights into the role of interphasial morphology on the electrochemical performance of lithium electrodes. / López, Carmen M.; Vaughey, John T.; Dees, Dennis W.

In: Journal of the Electrochemical Society, Vol. 159, No. 6, 2012.

Research output: Contribution to journalArticle

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