A pseudo-2-dimensional model of the nonlinear impedance response of a nickel-iron battery

J. M. E. Abarro, J. A. Paraggua
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Abstract

Pseudo-2-dimensional (P2D) models are computationally efficient tools for accurately predicting the battery’s performance. These models have been widely used to simulate lithium-ion batteries, but their application can be extended to other battery chemistries. Nickel-iron batteries are one type of storage that is regaining attention due to their durability and large theoretical specific capacity. However, their tendency to form an irreversible passivation layer and hydrogen gas leads to lower overall specific capacity and charging efficiency. Physics-based models of impedance spectra can help understand and interpret mass transport, thermodynamic, and reaction processes in a system. Batteries, being nonlinear systems in nature, can be better evaluated through nonlinear electrochemical impedance spectroscopy (NLEIS), an extension of the traditional electrochemical impedance spectroscopy (EIS), to break the degeneracy of a linear model. Base case parameters were used to generate the impedance spectra by applying moderate-amplitude current modulations. This work compared the first harmonic linear response and the second harmonic nonlinear response simulated through a P2D model. Unlike EIS, the nonlinear response shows sensitivity to charge transfer symmetry. At the negative electrode, the nonlinear response demonstrates strong dependence on the kinetic properties, suggesting that the overall battery performance is mainly influenced by the processes at the negative electrode-electrolyte interface.
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镍铁电池非线性阻抗响应的伪二维模型
伪二维(P2D)模型是准确预测电池性能的高效计算工具。这些模型已被广泛用于模拟锂离子电池,但其应用范围也可扩展到其他电池化学成分。镍铁电池因其耐用性和较大的理论比容量而重新受到关注。然而,它们容易形成不可逆的钝化层和氢气,导致整体比容量和充电效率降低。基于物理的阻抗谱模型有助于理解和解释系统中的质量传输、热力学和反应过程。电池本质上是非线性系统,通过非线性电化学阻抗谱(NLEIS)(传统电化学阻抗谱(EIS)的扩展)可以更好地评估电池,从而打破线性模型的退化。通过应用中等振幅的电流调制,使用基本情况参数生成阻抗谱。这项研究比较了第一次谐波线性响应和通过 P2D 模型模拟的第二次谐波非线性响应。与 EIS 不同,非线性响应显示出对电荷转移对称性的敏感性。在负极,非线性响应对动力学特性有很强的依赖性,这表明电池的整体性能主要受负极-电解质界面过程的影响。
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