H Hemanth, Mewada Rohan, Mallajosyula Sairam S
Discipline of Chemistry, Indian Institute of Technology Gandhinagar Palaj Gujarat India-382355
Discipline of Material Science and Engineering, Indian Institute of Technology Gandhinagar Palaj Gujarat India-382355.
Nanoscale Adv. 2023 Jan 10;5(3):796-804. doi: 10.1039/d2na00733a. eCollection 2023 Jan 31.
We present a systematic investigation capturing the charge and size effects of ions interacting with a graphene surface using polarizable simulations. Our results utilizing the Drude polarizable force field (FF) for ions, water and graphene surfaces, show that the graphene parameters previously developed by us are able to accurately capture the dynamics at the electrolyte-graphene interface. For monovalent ions, with increasing size, the solvation shell plays a crucial role in controlling the ion-graphene interactions. Smaller monovalent ions directly interact with the graphene surface, while larger ions interact with the graphene surface a well-formed solvation shell. For divalent ions, both interaction modes are observed. For the anion Cl, we observe direct interaction between the ions and the graphene surface. The anion-graphene interactions are strongly driven by the polarizability of the graphene surface. These effects are not captured in the absence of polarization by additive FF simulations. The present study underlines the importance of polarizability in capturing the interfacial phenomenon at the solid-solute interface.
我们通过可极化模拟对与石墨烯表面相互作用的离子的电荷和尺寸效应进行了系统研究。我们利用德鲁德可极化力场（FF）来描述离子、水和石墨烯表面，结果表明我们之前开发的石墨烯参数能够准确捕捉电解质-石墨烯界面处的动力学过程。对于单价离子，随着尺寸增大，溶剂化层在控制离子与石墨烯的相互作用中起着关键作用。较小的单价离子直接与石墨烯表面相互作用，而较大的离子则通过形成良好的溶剂化层与石墨烯表面相互作用。对于二价离子，两种相互作用模式均有观察到。对于阴离子Cl，我们观察到离子与石墨烯表面之间的直接相互作用。阴离子与石墨烯的相互作用受到石墨烯表面极化率的强烈驱动。在无极化的加和力场模拟中无法捕捉到这些效应。本研究强调了极化率在捕捉固-溶质界面处界面现象中的重要性。
