当前位置: X-MOL 学术Proc. Natl. Acad. Sci. U.S.A. › 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.)
The role of the water contact layer on hydration and transport at solid/liquid interfaces
Proceedings of the National Academy of Sciences of the United States of America ( IF 9.4 ) Pub Date : 2024-09-11 , DOI: 10.1073/pnas.2407877121
J Gäding 1, 2 , V Della Balda 3 , J Lan 4, 5 , J Konrad 1 , M Iannuzzi 3 , R H Meißner 1, 2 , G Tocci 3
Affiliation  

Understanding the structure in the nanoscopic region of water that is in direct contact with solid surfaces, so-called contact layer, is key to quantifying macroscopic properties that are of interest to e.g. catalysis, ice nucleation, nanofluidics, gas adsorption, and sensing. We explore the structure of the water contact layer on various technologically relevant solid surfaces, namely graphene, MoS 2 , Au(111), Au(100), Pt(111), and Pt(100), which have been previously hampered by time and length scale limitations of ab initio approaches or force field inaccuracies, by means of molecular dynamics simulations based on ab initio machine learning potentials built using an active learning scheme. Our results reveal that the in-plane intermolecular correlations of the water contact layer vary greatly among different systems: Whereas the contact layer on graphene and on Au(111) is predominantly homogeneous and isotropic, it is inhomogeneous and anisotropic on MoS 2 , on Au(100), and on the Pt surfaces, where it additionally forms two distinct sublayers. We apply hydrodynamics and the theory of the hydrophobic effect, to relate the energy corrugation and the characteristic length-scales of the contact layer with wetting, slippage, the hydration of small hydrophobic solutes and diffusio-osmotic transport. Thus, this work provides a microscopic picture of the water contact layer and links it to macroscopic properties of liquid/solid interfaces that are measured experimentally and that are relevant to wetting, hydrophobic solvation, nanofluidics, and osmotic transport.

中文翻译:


水接触层对固/液界面水合和传输的作用



了解与固体表面直接接触的水的纳米级区域(即所谓的接触层)的结构是量化宏观特性的关键,这些宏观特性对催化、冰成核、纳米流体、气体吸附和传感等感兴趣。我们探索了各种技术相关的固体表面上的水接触层的结构,即石墨烯、MoS 2 、Au(111)、Au(100)、Pt(111) 和 Pt(100),这些表面先前已受到时间的阻碍通过基于使用主动学习方案构建的从头算机器学习潜力的分子动力学模拟,解决从头算方法的长度尺度限制或力场不准确性。我们的结果表明,不同体系中水接触层的面内分子间相关性差异很大:石墨烯和 Au(111) 上的接触层主要是均匀和各向同性的,而 MoS 2 、Au 上的接触层是不均匀和各向异性的(100),并且在 Pt 表面上,它还形成两个不同的子层。我们应用流体动力学和疏水效应理论,将接触层的能量波纹和特征长度尺度与润湿、滑移、小疏水性溶质的水合和扩散渗透传输联系起来。因此,这项工作提供了水接触层的微观图像,并将其与通过实验测量的液/固界面的宏观特性联系起来,这些特性与润湿、疏水溶剂化、纳米流体和渗透传输相关。
更新日期:2024-09-11
down
wechat
bug