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Spatially Resolved Potential and Li-Ion Distributions Reveal Performance-Limiting Regions in Solid-State Batteries
ACS Energy Letters ( IF 19.3 ) Pub Date : 2021-10-19 , DOI: 10.1021/acsenergylett.1c01960 Elliot J. Fuller 1 , Evgheni Strelcov 2, 3 , Jamie L. Weaver 2 , Michael W. Swift 4, 5 , Joshua D. Sugar 1 , Andrei Kolmakov 2 , Nikolai Zhitenev 2 , Jabez J. McClelland 2 , Yue Qi 4, 6 , Joseph A. Dura 2 , A. Alec Talin 1
ACS Energy Letters ( IF 19.3 ) Pub Date : 2021-10-19 , DOI: 10.1021/acsenergylett.1c01960 Elliot J. Fuller 1 , Evgheni Strelcov 2, 3 , Jamie L. Weaver 2 , Michael W. Swift 4, 5 , Joshua D. Sugar 1 , Andrei Kolmakov 2 , Nikolai Zhitenev 2 , Jabez J. McClelland 2 , Yue Qi 4, 6 , Joseph A. Dura 2 , A. Alec Talin 1
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The performance of solid-state electrochemical systems is intimately tied to the potential and lithium distributions across electrolyte–electrode junctions that give rise to interface impedance. Here, we combine two operando methods, Kelvin probe force microscopy (KPFM) and neutron depth profiling (NDP), to identify the rate-limiting interface in operating Si-LiPON-LiCoO2 solid-state batteries by mapping the contact potential difference (CPD) and the corresponding Li distributions. The contributions from ions, electrons, and interfaces are deconvolved by correlating the CPD profiles with Li-concentration profiles and by comparisons with first-principles-informed modeling. We find that the largest potential drop and variation in the Li concentration occur at the anode–electrolyte interface, with a smaller drop at the cathode–electrolyte interface and a shallow gradient within the bulk electrolyte. Correlating these results with electrochemical impedance spectroscopy following battery cycling at low and high rates confirms a long-standing conjecture linking large potential drops with a rate-limiting interfacial process.
中文翻译：
空间分辨电位和锂离子分布揭示了固态电池中的性能限制区域
固态电化学系统的性能与引起界面阻抗的电解质 - 电极结的电位和锂分布密切相关。在这里，我们结合了两种操作方法，开尔文探针力显微镜 (KPFM) 和中子深度分析 (NDP)，以确定操作 Si-LiPON-LiCoO 2 中的限速界面通过映射接触电位差 (CPD) 和相应的锂分布来构建固态电池。离子、电子和界面的贡献通过将 CPD 分布与锂浓度分布相关联并通过与第一性原理知情建模进行比较来去卷积。我们发现最大的电位降和锂浓度的变化发生在阳极-电解质界面，阴极-电解质界面的电位降较小，体电解质内的梯度较浅。将这些结果与电池在低速率和高速率下循环后的电化学阻抗谱相关联，证实了将大电位降与限速界面过程联系起来的长期猜想。
更新日期：2021-11-12
中文翻译：
空间分辨电位和锂离子分布揭示了固态电池中的性能限制区域
固态电化学系统的性能与引起界面阻抗的电解质 - 电极结的电位和锂分布密切相关。在这里，我们结合了两种操作方法，开尔文探针力显微镜 (KPFM) 和中子深度分析 (NDP)，以确定操作 Si-LiPON-LiCoO 2 中的限速界面通过映射接触电位差 (CPD) 和相应的锂分布来构建固态电池。离子、电子和界面的贡献通过将 CPD 分布与锂浓度分布相关联并通过与第一性原理知情建模进行比较来去卷积。我们发现最大的电位降和锂浓度的变化发生在阳极-电解质界面，阴极-电解质界面的电位降较小，体电解质内的梯度较浅。将这些结果与电池在低速率和高速率下循环后的电化学阻抗谱相关联，证实了将大电位降与限速界面过程联系起来的长期猜想。
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