We derive and implement a method to describe the thermodynamics of electrode materials based on a substitutional lattice model. To assess the utility and generality of the method, we compare model results with experimental data for a variety of electrode materials: lithiated graphite and layered nickel-manganese-cobalt oxide (Chevrolet Bolt Electric Vehicle negative and positive electrode materials, respectively), manganese oxide (in the positive electrodes of the Gen 1 and Gen 2 Chevrolet Volt Extended Range Electric Vehicle and the positive electrode of many high-power-density batteries), and iron phosphate (Gen 1 Chevrolet Spark Electric Vehicle positive electrode material and of immediate interest for 12 and 48 V applications). An early version of the model has been applied to lithiated silicon (Li-Si). As was found in the Li-Si study, the model enables one to quantitatively represent experimental data from these different electrode materials with a small number of parameters, and, in this sense, the approach is both general and efficient. An open question is the utility of controlled-potential vs. controlled-current experiments for the elucidation of the system thermodynamics. We provide commentary on this question, and we highlight other open questions throughout this work.

中文翻译：

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替代材料的热力学模型：在锂化石墨，尖晶石锰氧化物，磷酸铁和层状镍锰钴氧化物中的应用

我们推导并实现了一种基于置换晶格模型描述电极材料热力学的方法。为了评估该方法的实用性和通用性，我们将模型结果与多种电极材料的实验数据进行了比较：锂化石墨和层状镍锰钴氧化物（分别为雪佛兰螺栓电动汽车的负极和正极材料），氧化锰（在Gen 1和Gen 2 Chevrolet Volt增程电动车的正极以及许多高功率密度电池的正极中）和磷酸铁（Gen 1 Chevrolet Spark电动车的正极材料，对12和48 V应用）。该模型的早期版本已应用于锂化硅（Li-Si）。正如锂硅研究中发现的那样，该模型使人们能够以少量参数定量表示来自这些不同电极材料的实验数据，从这个意义上讲，该方法既通用又有效。一个悬而未决的问题是控制电势与控制电流实验在阐明系统热力学方面的实用性。我们提供有关此问题的评论，并在整个工作中重点介绍其他未解决的问题。