Charge-dominated phase separation synthesis method of Janus particles with well-defined separated lobes and...

Synthesizing Janus particles (JPs) with well-defined separated lobes and customizable surface chemistries has broad scientific and engineering application prospects but has proven extremely challenging. Here, we report a novel phase-separation-based fabrication method leveraging charge-dominated seeded emulsion polymerization, which enables the synthesis of JPs with multi-scale lobe architectures (ranging from isotropic asymmetric shapes to chemically anisotropic forms such as ellipses, dumbbells, and triblock structures) and customizable surface chemistries (including functional groups like carboxyl, sulfate, and sulfonate). Our method is based on the principles of multicomponent systems' heterogeneous nucleation and growth, where the interfacial energy is meticulously controlled by fine-tuning the surface charges/chemical properties of polystyrene (PS) seeds and methacryloxypropyl trimethoxysilane (MPS) emulsions, while the growth kinetics of polymethacryloxypropyl trimethoxysilane (PMPS) lobes are guided through a synergistic combination of radical polymerization and hydrolysis-condensation reactions. Charge-dominated repulsive forces at the interface play a crucial role in driving the phase separation, enabling the synthesis of well-defined JPs and making this strategy broadly applicable to a variety of negatively charged PS seeds or MPS emulsions for customizable two-lobe surface chemistries. Furthermore, the PMPS hemisphere can be selectively modified, enabling applications in Pickering emulsions. This work offers a scalable method for the controllable fabrication of JPs with programmable architectures and surface chemistries.