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.

中文翻译：

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锂电沉积和剥离的动力学

电沉积和剥离是金属的基本电化学过程，由于锂金属电极的存在，在可再充电锂离子电池中已变得越来越重要。与锂金属电沉积和剥离相关的电极动力学对​​于确定快速放电和充电时的性能至关重要，这对于电动垂直起降（eVTOL）飞机和电动汽车（EV）至关重要。在这项工作中，我们展示了使用Marcus-Hush-Chidsey（MHC）动力学来准确地根据Boyle等人的工作预测Tafel曲线数据。[ACS Energy Lett。5（3），701（2020）]。我们讨论了从Marcus-Hush模型和MHC模型对四种溶剂中的锂金属电极进行重组能预测的差异。MHC动力学模型在Cantera中实施并开源。在具有锂阳极和LiFePO ₄阴极配对的伪2D电池模型中使用反应动力学模型，我们显示了考虑MHC动力学的重要性，并将其与Butler-Volmer和Marcus-Hush动力学模型进行了比较。我们发现在三种不同速率定律下，与eVTOL和EV有关的快速充放电条件下，与反应动力学相关的极限电流存在明显偏差。