Unconventional Charge Transport in MgCr2O4 and Implications for Battery Intercalation Hosts

化学 阴极 阳极 电池(电) 离子 储能 化学物理 离子运输机 锂(药物) 电化学 热传导 纳米技术 热力学 材料科学 电极 物理 物理化学 医学 功率(物理) 有机化学 内分泌学
作者
I. Johnson,Aashutosh Mistry,Liang Yin,Megan Murphy,Mark Wolfman,Timothy T. Fister,Saul H. Lapidus,Jordi Cabana,Venkat Srinivasan,Brian J. Ingram
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:144 (31): 14121-14131 被引量:16
标识
DOI:10.1021/jacs.2c03491
摘要

Ion transport in solid-state cathode materials prescribes a fundamental limit to the rates batteries can operate; therefore, an accurate understanding of ion transport is a critical missing piece to enable new battery technologies, such as magnesium batteries. Based on our conventional understanding of lithium-ion materials, MgCr2O4 is a promising magnesium-ion cathode material given its high capacity, high voltage against an Mg anode, and acceptable computed diffusion barriers. Electrochemical examinations of MgCr2O4, however, reveal significant energetic limitations. Motivated by these disparate observations; herein, we examine long-range ion transport by electrically polarizing dense pellets of MgCr2O4. Our conventional understanding of ion transport in battery cathode materials, e.g., Nernst-Einstein conduction, cannot explain the measured response since it neglects frictional interactions between mobile species and their nonideal free energies. We propose an extended theory that incorporates these interactions and reduces to the Nernst-Einstein conduction under dilute conditions. This theory describes the measured response, and we report the first study of long-range ion transport behavior in MgCr2O4. We conclusively show that the Mg chemical diffusivity is comparable to lithium-ion electrode materials, whereas the total conductivity is rate-limiting. Given these differences, energy storage in MgCr2O4 is limited by particle-scale voltage drops, unlike lithium-ion particles that are limited by concentration gradients. Future materials design efforts should consider the interspecies interactions described in this extended theory, particularly with respect to multivalent-ion systems and their resultant effects on continuum transport properties.
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