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  4. Surface stress during electro-oxidation of carbon monoxide and bulk stress evolution during electrochemical intercalation of lithium
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Surface stress during electro-oxidation of carbon monoxide and bulk stress evolution during electrochemical intercalation of lithium

Full metadata

Title
Surface stress during electro-oxidation of carbon monoxide and bulk stress evolution during electrochemical intercalation of lithium
Description

This work investigates in-situ stress evolution of interfacial and bulk processes in electrochemical systems, and is divided into two projects. The first project examines the electrocapillarity of clean and CO-covered electrodes. It also investigates surface stress evolution during electro-oxidation of CO at Pt{111}, Ru/Pt{111} and Ru{0001} electrodes. The second project explores the evolution of bulk stress that occurs during intercalation (extraction) of lithium (Li) and formation of a solid electrolyte interphase during electrochemical reduction (oxidation) of Li at graphitic electrodes. Electrocapillarity measurements have shown that hydrogen and hydroxide adsorption are compressive on Pt{111}, Ru/Pt{111}, and Ru{0001}. The adsorption-induced surface stresses correlate strongly with adsorption charge. Electrocatalytic oxidation of CO on Pt{111} and Ru/Pt{111} gives a tensile surface stress. A numerical method was developed to separate both current and stress into background and active components. Applying this model to the CO oxidation signal on Ru{0001} gives a tensile surface stress and elucidates the rate limiting steps on all three electrodes. The enhanced catalysis of Ru/Pt{111} is confirmed to be bi-functional in nature: Ru provides adsorbed hydroxide to Pt allowing for rapid CO oxidation. The majority of Li-ion batteries have anodes consisting of graphite particles with polyvinylidene fluoride (PVDF) as binder. Intercalation of Li into graphite occurs in stages and produces anisotropic strains. As batteries have a fixed size and shape these strains are converted into mechanical stresses. Conventionally staging phenomena has been observed with X-ray diffraction and collaborated electrochemically with the potential. Work herein shows that staging is also clearly observed in stress. The Li staging potentials as measured by differential chronopotentiometry and stress are nearly identical. Relative peak heights of Li staging, as measured by these two techniques, are similar during reduction, but differ during oxidation due to non-linear stress relaxation phenomena. This stress relaxation appears to be due to homogenization of Li within graphite particles rather than viscous flow of the binder. The first Li reduction wave occurs simultaneously with formation of a passivating layer known as the solid electrolyte interphase (SEI). Preliminary experiments have shown the stress of SEI formation to be tensile (~+1.5 MPa).

Date Created
2011
Contributors
  • Mickelson, Lawrence (Author)
  • Friesen, Cody (Thesis advisor)
  • Sieradzki, Karl (Committee member)
  • Buttry, Daniel (Committee member)
  • Venables, John (Committee member)
  • Arizona State University (Publisher)
Topical Subject
  • Materials Science
  • Chemistry
  • electrochemistry
  • Fuel Cells
  • Lithium-ion
  • Solid Electrolyte Interphase
  • Surface Stress
  • Lithium ion batteries
  • Electrolytes--Conductivity--Mathematical models.
  • Electrolytes
Genre
Doctoral Dissertation
Academic theses
Extent
xvi, 207 p. : ill. (some col.).a
Language
eng
Copyright Statement
In Copyright
Reuse Permissions
All Rights Reserved
Primary Member of
ASU Electronic Theses and Dissertations
Peer-reviewed
No
Open Access
No
Handle
https://hdl.handle.net/2286/R.I.9139
Statement of Responsibility
by Lawrence Mickelson
Description Source
Retrieved on Oct. 2, 2012
Level of coding
full
System Created
  • 2011-08-12 04:32:10
System Modified
  • 2021-08-26 09:04:40
  •     
  • 2 years ago
Additional Formats
  • OAI Dublin Core
  • MODS XML

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