Arrested Coalescence of Ionic Liquid Droplets: A Facile Strategy for Spatially Organized Multicompartment Assemblies

Multicompartment assemblies attract much attention for their wide applications. However, the fabrication of multicompartment assemblies usually requires elaborately designed building blocks and careful controlling. The emergence of droplet networks has provided a facile way to construct multiple droplet architectures, which can further be converted to multicompartment assemblies. Herein, the bind motif-free building blocks are presented, which consist of the hydrophobic Tf₂N⁻-based ionic liquid (IL) dissolving LiTf₂N salt, that can conjugate via arrested coalescence in confined-space templates to form IL droplet networks. Subsequent ultraviolent polymerization generates robust free-standing multicompartment assemblies. The conjugation of building blocks relies not on the peripheral bind motif but on the interfacial instability-induced arrested coalescence, avoiding tedious surface modification and assembly process. By tuning structures of templates and building blocks, multicompartment assemblies with 0D, 1D, 2D, and 3D structures are prepared in a facile and high-throughput way. Importantly, the bottom-up construction enables modular control over the compositions and spatial positions of individual building blocks. Combining with the excellent solvency of ILs, this system can serve as a general platform towards versatile multicompartment architectures. As demonstrations, by tailoring the chambers the multicompartment assemblies can spatiotemporally sense and report the chemical cues and perform various modes of motion.