纳米结构
深共晶溶剂
共晶体系
化学工程
材料科学
吸附
纳米技术
溶剂
化学
化学物理
结晶学
物理化学
有机化学
微观结构
工程类
作者
Aaron Elbourne,Quinn A. Besford,Nastaran Meftahi,Russell J. Crawford,Torben Daeneke,Tamar L. Greaves,Christopher McConville,Gary Bryant,Saffron J. Bryant,Andrew J. Christofferson
摘要
Deep eutectic solvents (DESs) are tuneable solvents with attractive properties for numerous applications. Their structure–property relationships are still under investigation, especially at the solid–liquid interface. Moreover, the influence of water on interfacial nanostructure must be understood for process optimization. Here, we employ a combination of atomic force microscopy and molecular dynamics simulations to determine the lateral and surface-normal nanostructure of the DES choline chloride:glycerol at the mica interface with different concentrations of water. For the neat DES system, the lateral nanostructure is driven by polar interactions. The surface adsorbed layer forms a distinct rhomboidal symmetry, with a repeat spacing of ~0.9 nm, comprising all DES species. The adsorbed nanostructure remains largely unchanged in 75 mol-% DES compared with pure DES, but at 50 mol-%, the structure is broken and there is a compromise between the native DES and pure water structure. By 25 mol-% DES, the water species dominates the adsorbed liquid layer, leaving very few DES species aggregates at the interface. In contrast, the near-surface surface-normal nanostructure, over a depth of ~3 nm from the surface, remains relatively unchanged down to 25 mol-% DES where the liquid arrangement changed. These results demonstrate not only the significant influence that water has on liquid nanostructure, but also show that there is an asymmetric effect whereby water disrupts the nanostructure to a greater degree closer to the surface. This work provides insight into the complex interactions between DES and water and may enhance their optimization for surface-based applications.
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