Abstract
Nucleobase-containing polymers are an emerging class of building blocks for the self-assembly of nanoobjects with promising applications in nanomedicine and biology. Here we present a macromolecular engineering approach to design nucleobase-containing polypeptide polymers incorporating thymine that further self-assemble in nanomaterials. Diblock and triblock copolypeptide polymers were prepared using sequential ring-opening polymerization of γ-Benzyl-l-glutamate N-carboxyanhydride (BLG-NCA) and γ-Propargyl-l-glutamate N-carboxyanhydride (PLG-NCA), followed by an efficient copper(I)-catalyzed azide alkyne cycloaddition (CuAAc) functionalization with thymidine monophosphate. Resulting amphiphilic copolymers were able to spontaneously form nanoobjects in aqueous solutions avoiding a pre-solubilization step with an organic solvent. Upon self-assembly, light scattering measurements and transmission electron microscopy (TEM) revealed the impact of the architecture (diblock versus triblock) on the morphology of the resulted nanoassemblies. Interestingly, the nucleobase-containing nanoobjects displayed free thymine units in the shell that were found available for further DNA-binding.
Highlights
Amphiphilic block copolymers are known to self-assemble in aqueous solutions into a wide range of nanostructures including worm-like or spherical micelles and vesicles [1,2,3]
We showed that nucleobase-containing polypeptides paved the way to unprecedented amphiphilic copolymers fully based on amino acid and nucleotide building blocks
These results suggested a contradictory reciprocity between two phenomena—the alignment of the PBLG macrodipoles and the negative charges repulsion of the ionic polypeptides
Summary
Amphiphilic block copolymers are known to self-assemble in aqueous solutions into a wide range of nanostructures including worm-like or spherical micelles and vesicles [1,2,3] In this field, polypeptide-based copolymers show considerable promise as building blocks to design bioinspired nanomaterials interfacing living systems [4,5]. Amphiphilic polypeptides with α-helical “rod” hydrophobic block have been extensively used to prepare vesicles [13,14] In this direction, poly(γ-benzyl-l-glutamate) (PBLG) has a strong. We showed that nucleobase-containing polypeptides paved the way to unprecedented amphiphilic copolymers fully based on amino acid and nucleotide building blocks. Their simple self-assembly in aqueous solution resulted in nanomaterials whose hydrophilic shells promoted efficient
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