Reactive nanofibers – Design of stimuli-responsive supramolecular bottlebrushes

Recent advances in the field of supramolecular chemistry have enabled scientists to design highly ordered nanostructures on the one-dimensional scale. With nature's complex, hierarchically organized structures serving as a major source of inspiration for research, self-assembly processes that rely on supramolecular interactions have become a key method for generating functional nanostructures in water. This results in fascinating shapes, such as micrometer-long fibers that are densely covered with polymer chains, or, as we call them, supramolecular polymer bottlebrushes. In this context, special emphasis is put onto architectures that exhibit responsiveness to external stimuli like temperature, light and pH-change of the environment, as these adaptive functionalities widen the scope of application of the structures towards targeted drug delivery, tissue engineering and biosensing. In prior studies, we have established various benzene-based supramolecular building blocks as reliable workhorses for achieving fibrous one-dimensional nanostructures which show exceptional stability in water. In the present work, stability can now be reversed through the introduction of cleavable ester-functionalities and pH-responsive amino acid moieties. We hereby aim to showcase the potential of supramolecular nanostructures to selectively disassemble in water through pH-changes and enzymatic degradation, highlighting its biocompatibility and tunability for tailored applications.