Fear Conner PhD Thesis Report (v99).pdf

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MECHANISTIC ROLE OF THERMAL EFFECTS ON LITHIUM PLATING

thesis
posted on 29.07.2022, 23:56 authored by Conner FearConner Fear

 In the pursuit to enable the rapid charging of lithium-ion batteries, lithium plating at the anode  poses one of the most significant challenges. Additionally, the heat generation that accompanies  high rate battery operation in conjunction with non-uniform cooling and localized heating at tabs  is known to result in thermal inhomogeneity. Such thermal anomalies in the absence of proper  thermal management can instigate accelerated degradation in the cell. This work seeks to elucidate  the link between thermal gradients and lithium plating in lithium-ion batteries using a combined  experimental and simulation-based approach. First, we experimentally characterize the lithium  plating phenomenon on graphite anodes under a wide variety of charging rates and temperatures  to gain mechanistic insights into the processes at play. An in operando detection method for the  onset of dendritic lithium plating is developed. Lithium plating regimes are identified as either  nucleate or dendritic, which exhibit vast differences in reversibility. An operando method to  quantify lithium stripping based on the rest phase voltage plateau is presented. Next, a model is  employed to provide fundamental insights to the thermo-electrochemical interactions during  charging in scenarios involving an externally imposed in-plane and inter-electrode thermal  gradient. The relative importance of in-plane vs. inter-electrode thermal gradients to charging  performance and cell degradation is necessary to inform future cell design and cooling systems for  large-format cells, which are crucial for meeting the energy requirements of applications like  electric vehicles. While in-plane thermal gradients strongly influence active material utilization,  the lithium plating severity was found to be very similar to an isothermal case at the same mean  temperature. By contrast, inter-electrode thermal gradients cause a shifting on the solid phase  potential at each electrode during charging, related to the increase or decrease in overpotential due  to local temperature variation. An experiment is then performed on a commercial multi-layer  pouch cell, in which it was found that applied thermal gradients provide a slight reduction in  lithium plating severity and degradation rate when compared to an isothermal cell at the same  mean temperature. The presence of a thermal gradient causes heterogeneous lithium plating  deposition within the cell, with colder regions experiencing higher quantities of plating and larger  thermal gradients leading to more severe heterogeneity.   

Funding

N00014-17-1-2942

History

Degree Type

Doctor of Philosophy

Department

Mechanical Engineering

Campus location

West Lafayette

Advisor/Supervisor/Committee Chair

Partha Mukherjee

Additional Committee Member 2

Vilas Pol

Additional Committee Member 3

Liang Pan

Additional Committee Member 4

Corey Love