Regulating of Liquid–Liquid Phase Separation and Molecular Self-Assembly through Selective Solvation

Abstract

Effectively regulating the liquid–liquid phase separation (LLPS) phenomenon in the process of molecular self-assembly is critical for controlling the qualities of the final products. However, the underlying mechanisms of LLPS that greatly affect the transition from molecules to crystals have not been fully addressed. Here, target solvents with properties of solvation or selective solvation suppression were theoretically screened to regulate the emergence and elimination of LLPS. Quantitative analysis of molecular electrostatic potential surfaces (MESP) was first applied to screen the antisolvent with solvation suppressing effect. Selective solvation suppressing was revealed, and the evolution mechanism of self-assembly in the nucleation pathways with or without LLPS was explored by experiments. It was found that clusters with unique properties of core–shell structure with dispersion transition layer may be the key to the occurrence of LLPS. This further provides new insights for understanding LLPS, which is a typical case for nonclassical nucleation theory.

Self-Assembled Nanotubes Based on Chiral H8-BINOL Modified with 1,2,3-Triazole to Recognize Bi3+ Efficiently by ICT Mechanism

“…As a cross-discipline between supramolecular chemistry and materials chemistry, the structural study of supramolecular self-assembly can help to enhance the understanding of the microstructure of molecular materials [ 4 , 5 , 6 ]. In the process of chemical development, molecular self-assembly nanomaterials have attracted more and more attention due to their wide applications in sensing, separation [ 7 , 8 ], catalysis [ 9 , 10 ], biomedicine [ 11 , 12 , 13 ], pharmacology [ 14 , 15 , 16 ] and other fields.…”

Tracking Prenucleation Molecular Clustering of Salicylamide in Organic Solvents

“…We use the latter term here. Other than PCS, methods such as nanoparticle tracking analysis (NTA) are powerful for direct determination of the size of mesoscale clusters in the prenucleation stage of organic compounds through their solvodynamic diameter just like the PCS. , The internal structures of the prenucleation clusters have also been studied by small-angle X-ray scattering (SAXS) or small-angle neutron scattering (SANS) with increasing solute concentration. On the other hand, transmission electron microscopy (TEM) offers real-time tracking of prenucleation clusters by visualization; methods such as cryo-TEM have proven extremely useful in delineating nucleation pathway. , …”