American Chemical Society
ja9b10491_si_001.pdf (3.8 MB)

Precision Anisotropic Brush Polymers by Sequence Controlled Chemistry

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journal contribution
posted on 2019-12-26, 16:34 authored by Chaojian Chen, Katrin Wunderlich, Debashish Mukherji, Kaloian Koynov, Astrid Johanna Heck, Marco Raabe, Matthias Barz, George Fytas, Kurt Kremer, David Yuen Wah Ng, Tanja Weil
The programming of nanomaterials at molecular length-scales to control architecture and function represents a pinnacle in soft materials synthesis. Although elusive in synthetic materials, Nature has evolutionarily refined macromolecular synthesis with perfect atomic resolution across three-dimensional space that serves specific functions. We show that biomolecules, specifically proteins, provide an intrinsic macromolecular backbone for the construction of anisotropic brush polymers with monodisperse lengths via grafting-from strategy. Using human serum albumin as a model, its sequence was exploited to chemically transform a single cysteine, such that the expression of said functionality is asymmetrically placed along the backbone of the eventual brush polymer. This positional monofunctionalization strategy was connected with biotin–streptavidin interactions to demonstrate the capabilities for site-specific self-assembly to create higher ordered architectures. Supported by systematic experimental and computational studies, we envisioned that this macromolecular platform provides unique avenues and perspectives in macromolecular design for both nanoscience and biomedicine.