在这里,我们提出了具有色散校正(DFT-D)计算的密度泛函理论,该计算的重点是将离子液体(IL)电解质嵌入二维(2D)Ti3C2TxMXenes中。这些IL包括阳离子1-乙基-3-甲基咪唑(Emim),伴随着三个不同的阴离子:双(三氟甲基磺酰基)酰亚胺(TFSA-),(氟磺酰基)酰亚胺(FSA-)和氟磺酰基(三氟甲磺酰基)酰亚胺(FTFA-)。通过改变表面终止元件,我们探索了中性白细胞插入的复杂几何形状,负,和正孔隙系统。通过五种群体分析模型实现电荷转移的准确估计,比如Hirshfeld,Hirshfeld-I,DDEC6(密度衍生静电和化学),Bader,和VDD(Voronoi变形密度)电荷。在这项工作中,我们推荐DDEC6和Hirshfeld-I充电型号,因为它们提供适度的价值并表现出合理的趋势。调查,旨在可视化非共价相互作用,阐明了阳离子-MXene和阴离子-MXene相互作用在控制MXenes内离子液体的嵌入现象中的作用。这种作用的大小取决于两个因素:阳离子的特定排列,以及参与该过程的阴离子物种的性质。
Herein, we present a density functional theory with dispersion correction (DFT-D) calculations that focus on the
intercalation of ionic liquids (ILs) electrolytes into the two-dimensional (2D) Ti3C2Tx MXenes. These ILs include the cation 1-ethyl-3-methylimidazolium (Emim+), accompanied by three distinct anions: bis(trifluoromethylsulfonyl)imide (TFSA-), (fluorosulfonyl)imide (FSA-) and fluorosulfonyl(trifluoromethanesulfonyl)imide (FTFSA-). By altering the surface termination elements, we explore the intricate geometries of IL
intercalation in neutral, negative, and positive pore systems. Accurate estimation of charge transfer is achieved through five population analysis models, such as Hirshfeld, Hirshfeld-I, DDEC6 (density derived electrostatic and chemical), Bader, and VDD (voronoi deformation density) charges. In this work, we recommend the DDEC6 and Hirshfeld-I charge models, as they offer moderate values and exhibit reasonable trends. The investigation, aimed at visualizing non-covalent interactions, elucidates the role of cation-MXene and anion-MXene interactions in governing the
intercalation phenomenon of ionic liquids within MXenes. The magnitude of this role depends on two factors: the specific arrangement of the cation, and the nature of the anionic species involved in the process.