Multi-scale simulation of the adsorption of lithium ion on graphite surface: From quantum Monte Carlo to molecular density functional theory.
Multi-scale simulation of the adsorption of lithium ion on graphite surface: From quantum Monte Carlo to molecular density functional theory.
复制标题
锂离子在石墨表面吸附的多尺度模拟：从量子蒙特卡罗到分子密度泛函理论
DOI：
10.1063/5.0082944
复制
发表时间：
2021
期刊：
影响因子：
--
通讯作者：
C. Pierleoni
中科院分区：
文献类型：
--
作者：
M. Ruggeri;Kyle G. Reeves;Tzu;Guillaume Jeanmairet;M. Salanne;C. Pierleoni
在碳电极表面形成的双层结构由电极和电解质物种之间的相互作用决定。然而，碳是出了名的难以精确模拟，即使是用成熟的方法，如电子密度泛函理论和分子动力学。在这里，我们专注于锂离子与石墨表面接触的重要情况，我们进行了一系列参考量子蒙特卡罗计算，使我们能够基准各种电子密度泛函理论泛函。然后，我们拟合了一个精确的碳-锂对势，该势用于分子密度泛函理论计算，以确定在水存在下离子在表面上吸附的自由能。在水溶液中的吸附配置文件显着不同的气相结果，这强调了溶剂的作用的双电层的性能。
The structure of the double-layer formed at the surface of carbon electrodes is governed by the interactions between the electrode and the electrolyte species. However, carbon is notoriously difficult to simulate accurately, even with well-established methods such as electronic density functional theory and molecular dynamics. Here, we focus on the important case of a lithium ion in contact with the surface of graphite, and we perform a series of reference quantum Monte Carlo calculations that allow us to benchmark various electronic density functional theory functionals. We then fit an accurate carbon-lithium pair potential, which is used in molecular density functional theory calculations to determine the free energy of the adsorption of the ion on the surface in the presence of water. The adsorption profile in aqueous solution differs markedly from the gas phase results, which emphasize the role of the solvent on the properties of the double-layer.
影响因子：
4.4
作者：
Brandenburg, Jan Gerit;Zen, Andrea;Michaelides, Angelos
通讯作者：
Michaelides, Angelos
影响因子：
3.4
作者：
Lehtola, Susi;Steigemann, Conrad;Marques, Miguel A. L.
通讯作者：
Marques, Miguel A. L.