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Experimental and Modeling Studies of Dendrite Initiation during Lithium Electrodeposition

Maraschky, Adam M.
http://orcid.org/0000-0002-9904-098X
http://rave.ohiolink.edu/etdc/view?acc_num=case1590505470067127

Abstract Details

2020, Doctor of Philosophy, Case Western Reserve University, Chemical Engineering.
High-energy density batteries are essential for powering future electric vehicles (EVs) and electric aircraft. These technologies are limited by the capacity of their batteries. Enabling high-specific energy batteries could make longer-range electric vehicles and electric aircraft a reality. The Li-metal anode offers the highest theoretical specific energy among practically available anode materials. However, secondary Li-metal anodes experience capacity loss and safety hazards caused by the growth of dendrites on the anode surface during charging. After four decades of research on Li-metal batteries, rechargeable Li-metal anodes that do not evolve dendrites are still not commercially available. Understanding the physical causes and mechanisms of dendritic Li electrodeposition, in order to develop commercial Li-metal batteries, motivates the present work. It is shown herein that solid-state transport limitations within a dynamic solid electrolyte interphase (SEI) are dominant in controlling the time when Li dendrites first form. Chronopotentiometry and optical imaging provide experimental observations for when dendrites first appear on a Li electrode. Dendrite onset time is shown to increase with increasing temperature and decrease with increasing current density and initial SEI thickness. These phenomena are shown to be due to the onset of diffusion limitations brought on by a thickening SEI. Electrochemical impedance spectroscopy (EIS) provides evidence for SEI growth and enables estimation of the SEI growth rates during Li electrodeposition. These experiments guide the development of an analytical model that explains mechanistically how transport limitations within the SEI control the onset time of dendrite growth during Li electrodeposition. The model also provides predictions of Li dendrite onset times. These predictions agree qualitatively with the observed effects of current density, initial SEI thickness, temperature, and pulsing. Finally, it is shown through numerical modeling that pulsed current (p.c.) plating is not able to mitigate the concentration depletion experienced at the Li electrode in a way that would prevent dendrites during the charging of Li-metal batteries. At an equivalent-plating rate, the increased SEI growth rate and decreased plating efficiency negate the benefits of concentration profile relaxation provided by p.c. plating.
Rohan Akolkar, PhD (Advisor)
Uziel Landau, PhD (Committee Member)
Donald Feke, PhD (Committee Member)
Alp Sehirlioglu, PhD (Committee Member)
107 p.
Chemical Engineering
dendritic growth; electroplating; Li dendrites; mass transport; transport limitation; solid electrolyte interphase; surface film; alkali metal

Recommended Citations

Citations

  • Maraschky, A. M. (2020). Experimental and Modeling Studies of Dendrite Initiation during Lithium Electrodeposition [Doctoral dissertation, Case Western Reserve University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=case1590505470067127

    APA Style (7th edition)

  • Maraschky, Adam. Experimental and Modeling Studies of Dendrite Initiation during Lithium Electrodeposition. 2020. Case Western Reserve University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=case1590505470067127.

    MLA Style (8th edition)

  • Maraschky, Adam. "Experimental and Modeling Studies of Dendrite Initiation during Lithium Electrodeposition." Doctoral dissertation, Case Western Reserve University, 2020. http://rave.ohiolink.edu/etdc/view?acc_num=case1590505470067127

    Chicago Manual of Style (17th edition)

case1590505470067127
455
© 2020, some rights reserved.Creative Commons License Experimental and Modeling Studies of Dendrite Initiation during Lithium Electrodeposition by Adam M. Maraschky is licensed under a Creative Commons Attribution-NonCommercial-ShareAlike 3.0 Unported License. Based on a work at etd.ohiolink.edu.
This open access ETD is published by Case Western Reserve University School of Graduate Studies and OhioLINK.