Helicity- and Molecular-Weight-Driven Self-Sorting and Assembly of Helical Polymers towards Two-Dimensional Smectic Architectures and Selectively Adhesive Gels

Self-sorting plays a crucial role in living systems such as the selective assembly of DNA and specific folding of proteins. However, the self-sorting of artificial helical polymers such as biomacromolecules has rarely been achieved. In this work, single-handed helical poly(phenyl isocyanide)s bearing pyrene (Py) and naphthalene (Np) probes were prepared, which exhibited interesting self-sorting properties driven by both helicity and molecular weight (M-n) in solution, solid state, gel, and on the gel surface as well. The polymers with the same helix sense and similar M-n can self-sort and assemble into well-defined two-dimensional smectic architectures and form stable gels in organic solvents. In contrast, mixed polymers with opposite handedness or different M-n were repulsive to each other and did not aggregate. Moreover, the gels of helical polymers with the same handedness and similar M-n can recognize themselves and adhere together to form a gel.