Molecular Probes Reveal Chemical Selectivity of the Solid–Electrolyte Interphase,The Journal of Physical Chemistry C |
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Molecular Probes Reveal Chemical Selectivity of the Solid–Electrolyte Interphase,The Journal of Physical Chemistry C
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The solid–electrolyte interphase (SEI) is well-known to provide critical protection between the strongly reducing negative electrode and the organic electrolytes of nonaqueous batteries. Batteries with a poorly passivating SEI will suffer from rapid capacity fade and short lifetimes. Despite its importance and extensive study of its structure and composition, the mechanism of SEI passivation remains poorly understood. In this work, we demonstrate using electrochemical collector-generator measurements that the SEI is chemically selective in its passivation and propose a model based on catalytic active sites to explain its performance. Electrochemically interrogating the SEI with functionalized ferrocene mediators shows that the through-film mediator reduction is much more sensitive to mediator functional group than size, indicating preferential partitioning into the organic SEI layer. Additional experiments with controlled electrode crosstalk show that incorporation of dissolved transition metals increases both the density and the activity of active sites within the SEI. We conclude that the inner, inorganic layer is responsible for preventing charge transfer through the SEI while the outer, organic layer is minimally important. Our model reconciles contradictory observations from the literature and identifies the most important components of a functional battery interface.
中文翻译：
众所周知，固态电解质间相（SEI）在强还原性负极和非水电池的有机电解质之间提供关键保护。SEI钝化差的电池将遭受快速的容量衰减和短寿命的困扰。尽管其重要性和对其结构和组成的广泛研究，但对SEI钝化的机理仍知之甚少。在这项工作中，我们证明了使用电化学收集器-发电机的测量方法可以证明SEI在钝化过程中具有化学选择性，并提出了一个基于催化活性位的模型来解释其性能。用功能化的二茂铁介体对SEI进行电化学查询显示，通过膜介体还原对介体官能团的敏感性比其大小要大得多，表示优先划分为有机SEI层。具有受控的电极串扰的其他实验表明，溶解的过渡金属的结合既增加了SEI内的密度，又增加了活性位点的活性。我们得出结论，内部无机层负责防止电荷通过SEI传输，而外部有机层则至关重要。我们的模型调和了文献中相互矛盾的意见，并确定了功能电池接口的最重要组成部分。无机层负责防止电荷通过SEI传输，而有机层的外部则至关重要。我们的模型调和了文献中相互矛盾的观察结果，并确定了功能电池接口的最重要组成部分。无机层负责防止电荷通过SEI传输，而有机层的外部则至关重要。我们的模型调和了文献中相互矛盾的意见，并确定了功能电池接口的最重要组成部分。 |
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