Ionic liquids intercalation in titanium carbide MXenes: A first-principles investigation,Journal of Computational Chemistry

当前位置： X-MOL 学术 › J. Comput. Chem. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Ionic liquids intercalation in titanium carbide MXenes: A first-principles investigation
Journal of Computational Chemistry ( IF 3.4 ) Pub Date : 2024-06-07 , DOI: 10.1002/jcc.27444
Shaoze Zhang _{1,

2} , De-En Jiang ₃ , Nan Zhou _{1,

2} , Jiaxing Tang _{1,

2} , Keyu Zhang _{1,

2} , Yin Li _{1,

2} , Junxian Hu _{1,

2} , Changjun Peng ₄ , Honglai Liu ₄ , Bin Yang _{1,

2} , Yaochun Yao _{1,

2}

Affiliation

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) Ti₃C₂T_x 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.

中文翻译：

碳化钛 MXene 中离子液体插层：第一性原理研究

在此，我们提出了具有色散校正（DFT-D）计算的密度泛函理论，该理论重点关注离子液体（IL）电解质插入二维（2D）Ti ₃ C ₂ T _x MXenes中。这些离子液体包括阳离子 1-乙基-3-甲基咪唑鎓 (Emim ⁺ )，并伴有三种不同的阴离子：双(三氟甲基磺酰基)亚胺 (TFSA ⁻ )、(氟磺酰基)亚胺 (FSA ⁻ ) 和氟磺酰基(三氟甲磺酰基)亚胺 (FTFSA ^{− )} ）。通过改变表面终止元件，我们探索了中性、负性和正性孔隙系统中离子液体嵌入的复杂几何形状。通过 Hirshfeld、Hirshfeld-I、DDEC6（静电和化学密度导出）、Bader 和 VDD（voronoi 变形密度）电荷等五种总体分析模型实现电荷转移的准确估计。在这项工作中，我们推荐 DDEC6 和 Hirshfeld-I 电荷模型，因为它们提供适中的值并表现出合理的趋势。该研究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 MXene 内离子液体插层现象中的作用。这种作用的大小取决于两个因素：阳离子的具体排列以及参与该过程的阴离子种类的性质。

更新日期：2024-06-07

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南