Abstract
Electrostatically coassembled micelles constitute a versatile class of functional soft materials with broad application potential as, for example, encapsulation agents for nanomedicine and nanoreactors for gels and inorganic particles. The nanostructures that form upon the mixing of selected oppositely charged (block co)polymers and other ionic species greatly depend on the chemical structure and physicochemical properties of the micellar building blocks, such as charge density, block length (ratio), and hydrophobicity. Nearly three decades of research since the introduction of this new class of polymer micelles shed significant light on the structure and properties of the steady-state association colloids. Dynamics and out-of-equilibrium processes, such as (dis)assembly pathways, exchange kinetics of the micellar constituents, and reaction-assembly networks, have steadily gained more attention. We foresee that the broadened scope will contribute toward the design and preparation of otherwise unattainable structures with emergent functionalities and properties. This Viewpoint focuses on current efforts to study such dynamic and out-of-equilibrium processes with greater spatiotemporal detail. We highlight different approaches and discuss how they reveal and rationalize similarities and differences in the behavior of mixed micelles prepared under various conditions and from different polymeric building blocks.
Highlights
Coassembled micelles constitute a versatile class of functional soft materials with broad application potential as, for example, encapsulation agents for nanomedicine and nanoreactors for gels and inorganic particles
The electrostatic coassembly of copolymers with oppositely charged species received widespread attention in the last decades as a versatile approach to create a new class of polymer micelles with interesting properties
Conflicting results claim different mechanisms dominate the relaxation from transient structures to micelles
Summary
The electrostatic coassembly of (diblock) copolymers with oppositely charged species received widespread attention in the last decades as a versatile approach to create a new class of polymer micelles with interesting properties. We anticipate a growing interest in macroscopic materials prepared from C3Ms and coacervates, such as hydrogels, thin films, adhesives, and saloplastics Their steady-state properties are well-studied including their dependence on choice of one or two block copolymers, polymer length (ratios) and chemical nature of the components. The formation of kinetically trapped states has long been seen as a bottleneck, but is embraced as an effective means to create various nanostructures with unprecedented complexity from identical building blocks Another important development is the shift in focus from equilibrium to out-ofequilibrium conditions. The (dis)assembly kinetics and exchange dynamics of these mixed micelles are being studied in-depth using time-resolved scattering tools and fluorescence spectroscopy These studies disclose transient (nano)structures, which may be annealed or vitrified in the future to broaden the scope of attainable architectures.
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