Electrodeposition and stripping are fundamental electrochemical processes for metals and have gained importance in rechargeable Li-ion batteries due to lithium metal electrodes. The electrode kinetics associated with lithium metal electrodeposition and stripping is crucial in determining the performance at fast discharge and charge, which is important for electric vertical takeoff and landing (eVTOL) aircraft and electric vehicles (EV). In this work, we show the use of Marcus–Hush–Chidsey (MHC) kinetics to accurately predict the Tafel curve data from the work of Boyle et al. [ACS Energy Lett. 5(3), 701 (2020)]. We discuss the differences in predictions of reorganization energies from the Marcus–Hush and the MHC models for lithium metal electrodes in four solvents. The MHC kinetic model is implemented and open-sourced within Cantera. Using the reaction kinetic model in a pseudo-2D battery model with a lithium anode paired with a LiFePO4 cathode, we show the importance of accounting for the MHC kinetics and compare it to the use of Butler–Volmer and Marcus–Hush kinetic models. We find significant deviation in the limiting currents associated with reaction kinetics for the three different rate laws for conditions of fast charge and discharge relevant for eVTOL and EV, respectively.
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21 November 2020
Research Article|
November 16 2020
Kinetics of lithium electrodeposition and stripping
Special Collection:
65 Years of Electron Transfer
Daniel Korff
;
Daniel Korff
2
Department of Mechanical Engineering, Colorado School of Mines
, Golden, Colorado 80401, USA
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Steven C. DeCaluwe
;
Steven C. DeCaluwe
2
Department of Mechanical Engineering, Colorado School of Mines
, Golden, Colorado 80401, USA
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Venkatasubramanian Viswanathan
Venkatasubramanian Viswanathan
a)
1
Department of Mechanical Engineering, Carnegie Mellon University
, Pittsburgh, Pennsylvania 15213, USA
a)Author to whom correspondence should be addressed: venkvis@cmu.edu
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a)Author to whom correspondence should be addressed: venkvis@cmu.edu
Note: This paper is part of the JCP Special Topic on 65 Years of Electron Transfer.
J. Chem. Phys. 153, 194701 (2020)
Article history
Received:
August 02 2020
Accepted:
October 26 2020
Citation
Shashank Sripad, Daniel Korff, Steven C. DeCaluwe, Venkatasubramanian Viswanathan; Kinetics of lithium electrodeposition and stripping. J. Chem. Phys. 21 November 2020; 153 (19): 194701. https://doi.org/10.1063/5.0023771
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