Nano-coacervates from in-situ Polymerization of Dipolar-driven Mesomorphic State surviving in harsh environments

we have utilized in-situ template polymerization of the dipole-driven mesomorphic aggregates to create topologically interlocked nano-coacervates. Templated coacervation leads to inter-entangled double network, that is, the guest reinforces the template host of dipole-driven mesomorphic assemblies and being married permanently with the host. Without any chemical crosslinkers, the stable state of nano-coacervates can persist in both high salt concentrations and low salt concentrations due to their topologically interlocked structures. Topologically interlocked nano-coacervates being tougher than traditional coacervates, since the template polymerization can not only generate a force to uncomplex the traditional coacervates, but can also polymerize the dipolar NaAc monomers into PAc chains to newly form topologically interlocked nano-coacervates. Simulation results demonstrate that the critical condition to create topologically interlocked nano-coacervate with loops is the molar charge ratio r >1. Compared to the bulk polymerization without dipolar template effect, the template polymerization by utilizing dipolar interactions can not only significantly improve the chemical conversion but also polymerize long PAc chains with chain size similar to the PLL template chain size. When Cs >1.08M, the dipole-dipole interactions would be fully screened and the template effect in the polymerization would be absent.

Such topologically interlocked nano-coacervates may reveal the mechanism of how the first living system was born and survived in the primordial sea with extremely high salt concentrations. Moreover, our strategy to utilize template polymerization of dipolar-driven mesomorphic assemblies to remove the RNA-polypeptides complexed coacervates exhibits conceptual similarities to the inverse process of biomolecular condensation, and may enlighten the therapeutic intervention and treatment in protein aggregation diseases.