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Stability of Electrode-Electrolyte Interfaces During Charging in Lithium Batteries


Natsiavas, Panagiotis Philippos (2016) Stability of Electrode-Electrolyte Interfaces During Charging in Lithium Batteries. Dissertation (Ph.D.), California Institute of Technology. doi:10.7907/Z93R0QR8.


In this thesis we study the growth of a Li electrode-electrolyte interface in the presence of an elastic prestress. In particular, we focus our interest on Li-air batteries with a solid electrolyte, LIPON, which is a new type of secondary or rechargeable battery. Theoretical studies and experimental evidence show that during the process of charging the battery the replated lithium adds unevenly to the electrode surface. This phenomenon eventually leads to dendrite formation as the battery is charged and discharged numerous times. In order to suppress or alleviate this deleterious effect of dendrite growth, we put forth a study based on a linear stability analysis. Taking into account all the mechanisms of mass transport and interfacial kinetics, we model the evolution of the interface. We find that, in the absence of stress, the stability of a planar interface depends on interfacial diffusion properties and interfacial energy. Specifically, if Herring-Mullins capillarity-driven interfacial diffusion is accounted for, interfaces are unstable against all perturbations of wavenumber larger than a critical value. We find that the effect of an elastic prestress is always to stabilize planar interfacial growth by increasing the critical wavenumber for instability. A parametric study results in quantifying the extent of the prestress stabilization in a manner that can potentially be used in the design of Li-air batteries. Moreover, employing the theory of finite differences we numerically solve the equation that describes the evolution of the surface profile and present visualization results of the surface evolution by time. Lastly, numerical simulations performed in a commercial finite element software validate the theoretical formulation of the interfacial elastic energy change with respect to the planar interface.

Item Type:Thesis (Dissertation (Ph.D.))
Subject Keywords:stability analysis; lithium batteries; dendrites; interface
Degree Grantor:California Institute of Technology
Division:Engineering and Applied Science
Major Option:Mechanical Engineering
Thesis Availability:Public (worldwide access)
Research Advisor(s):
  • Ortiz, Michael
Thesis Committee:
  • Ravichandran, Guruswami (chair)
  • Kochmann, Dennis M.
  • Weinberg, Kerstin
  • Ortiz, Michael
Defense Date:21 October 2015
Record Number:CaltechTHESIS:11222015-173649284
Persistent URL:
Default Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:9282
Deposited By: Panagiotis Natsiavas
Deposited On:24 Nov 2015 19:11
Last Modified:04 Oct 2019 00:11

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