Using molecular dynamics to quantify the electrical double layer and examine the potential for its direct observation in the in-situ TEM
Using molecular dynamics to quantify the electrical double layer and examine the potential for its direct observation in the in-situ TEM
复制标题
使用分子动力学量化双电层并检查在原位 TEM 中直接观察的潜力
DOI：
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发表时间：
2015
影响因子：
--
通讯作者：
N. Browning
中科院分区：
文献类型：
--
作者：
D. Welch;B. L. Mehdi;Hannah Hatchell;R. Faller;James E. Evans;N. Browning
了解电池中电极-电解液界面发生的基本过程将对下一代储能技术的发展起到关键作用。电极-电解液界面最基本的方面之一是电双层(EDL)。鉴于扫描电子显微镜(STEM)的高空间分辨率原位电化学流体池的发展，我们现在有可能直接观察EDL的形成和动力学。在本文中，我们使用经典模型和原子分子动力学(MD)模拟来预测EDL中的电解液结构。经典模型预测的浓度分布与分子动力学模型相差很大。因此，为了准确地预测电极-电解液界面的STEM图像，必须使用MD。对于高对比度电解液(高原子序数CsCL电解液)，结合MD和图像模拟，可以确定，为了获得平滑的界面，EDL内的浓度分布在实验上应该是可见的。当考虑到正常的实验参数，如粗糙的界面和低Z电解液(如锂离子电池中使用的那些)时，观察EDL似乎更困难。
Understanding the fundamental processes taking place at the electrode-electrolyte interface in batteries will play a key role in the development of next generation energy storage technologies. One of the most fundamental aspects of the electrode-electrolyte interface is the electrical double layer (EDL). Given the recent development of high spatial resolution in-situ electrochemical fluid cells for scanning transmission electron microscopy (STEM), there now exists the possibility that we can directly observe the formation and dynamics of the EDL. In this paper we predict electrolyte structure within the EDL using classical models and atomistic Molecular Dynamics (MD) simulations. Classical models are found to greatly differ from MD in predicted concentration profiles. It is thus suggested that MD must be used in order to accurately predict STEM images of the electrode-electrolyte interface. Using MD and image simulation together for a high contrast electrolyte (the high atomic number CsCl electrolyte), it is determined that, for a smooth interface, concentration profiles within the EDL should be visible experimentally. When normal experimental parameters such as rough interfaces and low-Z electrolytes (like those used in Li-ion batteries) are considered, observation of the EDL appears to be more difficult.
DOI：
10.1021/jp9108865
发表时间：
2010-05-13
期刊：
The journal of physical chemistry. B
影响因子：
--
作者：
Howard JJ;Perkyns JS;Pettitt BM
通讯作者：
Pettitt BM
模拟原位液体显微镜的真实成像条件。
影响因子：
2.2
作者：
Welch,DavidA;Faller,Roland;Evans,JamesE;Browning,NigelD
通讯作者：
Browning,NigelD
影响因子：
17.1
作者：
White, Edward R.;Singer, Scott B.;Augustyn, Veronica;Hubbard, William A.;Mecklenburg, Matthew;Dunn, Bruce;Regan, Brian C.
通讯作者：
Regan, Brian C.