Signal responsive transient coacervation in complex coacervate core micelles

Triggered coacervate phase (de)stabilisation in complex coacervate core micelles (C3Ms) has traditionally been limited to changes in pH and salt concentration, limiting options in responsive C3M material design. To expand this toolbox, we have developed C3Ms, that, at constant physiological pH, assemble and disassemble by coupling to a chemical reaction network (CRN) driven by the conversion of electron deficient allyl acetates and thiol or amine nucleophiles. This CRN produces transient quaternization of tertiary amine-functionalised block copolymers, which can then form the complex coacervate phase. We demonstrate triggered C3M assembly using two different allyl acetates, resulting in dramatically different assembly rates from hours to days. These are applied in various combinations with selected nucleophiles, demonstrating sequential signal induced C3M formation and deformation, as well as transient non-equilibrium (de)formation. We expect that timed and signal-responsive control over coacervate phase formation at physiological pH will find application in nucleic acid delivery, nano reactors and protocell research.

Signal responsive transient coacervation in complex coacervate core micelles

Triggered coacervate phase (de)stabilisation in complex coacervate core micelles (C3Ms) has traditionally been limited to changes in pH and salt concentration, limiting options in responsive C3M material design. To expand this toolbox, we have developed C3Ms, that, at constant physiological pH, assemble and disassemble by coupling to a chemical reaction network (CRN) driven by the conversion of electron deficient allyl acetates and thiol or amine nucleophiles. This CRN produces transient quaternization of tertiary amine-functionalised block copolymers, which can then form the complex coacervate phase. We demonstrate triggered C3M assembly using two different allyl acetates, resulting in dramatically different assembly rates from hours to days. These are applied in various combinations with selected nucleophiles, demonstrating sequential signal induced C3M formation and deformation, as well as transient non-equilibrium (de)formation. We expect that timed and signal-responsive control over coacervate phase formation at physiological pH will find application in nucleic acid delivery, nano reactors and protocell research.

Multicompartment dendrimicelles with binary, ternary and quaternary core composition

Förster Resonance Energy Transfer in combination with fluorescence quenching are exploited to reveal the binary, ternary and quaternary core compositions of dendrimer-based complex coacervate core micelles.

On Complex Coacervate Core Micelles: Structure-Function Perspectives

The co-assembly of ionic-neutral block copolymers with oppositely charged species produces nanometric colloidal complexes, known, among other names, as complex coacervates core micelles (C3Ms). C3Ms are of widespread interest in nanomedicine for controlled delivery and release, whilst research activity into other application areas, such as gelation, catalysis, nanoparticle synthesis, and sensing, is increasing. In this review, we discuss recent studies on the functional roles that C3Ms can fulfil in these and other fields, focusing on emerging structure–function relations and remaining knowledge gaps.