Abstract
Recent experimental works suggested that the confinement into a cylindrical nanopore induced the microphase separation of a binary liquid, despite the miscible character of its bulk counterpart. A core–shell organization was evidenced such that one of the liquids was strongly anchored to the solid surface whereas the other was confined at the center of the pore. At the same time, a study based on atomistic simulations suggested a strong heterogeneity and the absence of a separation. In this work, by refining the solid–liquid interactions to qualitatively reproduce the experimental adsorption isotherms of both single liquids, the microphase separation and the core–shell structure are captured. By tuning the surface chemistry of the nanopore to mimic hydrophilic and hydrophobic confinement, we show that it is possible to control the structural characteristics of the core–shell structure.The molecular origin of the microphase separation is then ascribed to the strong hydrogen bonds and a commensurate arrangement between the confining material and both liquids.
Highlights
IntroductionFor three decades confinement effects at the nanoscale on the physics of fluids have been been intensively studied.[1,2,3,4,5,6,7,8,9,10,11,12,13,14,15] Many new properties have been discovered such as the giant diffusion of liquids,[16,17,18] the apparition of new phases and new transitions,[19,20,21,22] giant dielectric properties,[11,12,23,24,25] the increase of optical properties,[26] and the possible mixing of non-miscible mixtures.[27]
Harrach et al.[33] have studied the phase behavior of a mixture of isobutyric acid and water confined in mesoporous SBA-15 silica material and have shown that the iBA-rich phase is close to the pore wall and the water-rich phase is in the center of the pores
Whereas these works only suggest a partial separation of two hydrogen bonds forming liquids or two apolar liquids near the solid surface, Morineau and co-workers[15] have recently provided a direct experimental structural evidence of the microphase separation of macroscopically miscible liquids consisting of hydrogen bonds forming liquid and an apolar one
Summary
For three decades confinement effects at the nanoscale on the physics of fluids have been been intensively studied.[1,2,3,4,5,6,7,8,9,10,11,12,13,14,15] Many new properties have been discovered such as the giant diffusion of liquids,[16,17,18] the apparition of new phases and new transitions,[19,20,21,22] giant dielectric properties,[11,12,23,24,25] the increase of optical properties,[26] and the possible mixing of non-miscible mixtures.[27]. Whereas these works only suggest a partial separation of two hydrogen bonds forming liquids or two apolar liquids near the solid surface, Morineau and co-workers[15] have recently provided a direct experimental structural evidence of the microphase separation of macroscopically miscible liquids consisting of hydrogen bonds forming liquid and an apolar one
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