Porphyrin/Ionic-Liquid Co-assembly Polymorphism Controlled by Liquid-Liquid Phase Separation.

Area of Science:

• Supramolecular Chemistry
• Materials Science
• Chemical Engineering

Background:

• Controlling multicomponent co-assembly is crucial for materials fabrication, pharmaceutical polymorphism, and supramolecular polymerization.
• Challenges persist in understanding and directing these complex self-assembly processes.

Purpose of the Study:

• To investigate the initial steps in multicomponent co-assembly.
• To identify a strategy for controlling co-assembly structures and properties.

Main Methods:

• Utilized a model system of water-soluble porphyrin and ionic liquids.
• Observed liquid-liquid phase separation (LLPS) and subsequent co-assembly nucleation.
• Analyzed the role of LLPS-formed droplets as nucleation precursors.

Main Results:

• Discovered that LLPS into distinct liquid phases is the initial step before co-assembly nucleation.
• Demonstrated that LLPS droplets act as nucleation sites, determining co-assembly outcomes.
• Achieved co-assembly polymorphism and tunable supramolecular phase transitions by regulating interactions at the LLPS stage.

Conclusions:

• LLPS plays a pivotal role in the evolution of multicomponent co-assemblies.
• LLPS offers an effective strategy for controlling co-assembly polymorphism and supramolecular phase transitions.