The temporal control of enzymatic activity by external stimuli is a hallmark of life, whereby most often chemical reactions are only transiently switched on as long as the stimulus is present. In order to mimic such control over biocatalysis with artificial nanosystems, we have developed bioinspired block copolymer vesicles that become transiently permeable for enzyme substrates in response to visible light or mechanical forces. To this end, amphiphilic block copolymers were functionalized in their hydrophobic block with Donor-Acceptor Stenhouse Adducts (DASAs) or with nucleobases. The resulting biocatalytic nanoreactors can be switched on by light or by turbulent mixing. They switch back to their inactive state as soon as the external stimulus is withdrawn. Thus, these nanoreactors allow precise temporal control over biocatalysis, which opens up new applications in drug delivery and in molecular systems engineering. Moreover, this work shows that stimuli-responsive polymers can not only be used to tune the activity of enzymes when covalently conjugated to biomolecules, but also when the proteins are non-covalently encapsulated in polymeric nanostructures.

Controlling biocatalysis by transiently switchable polymersome nanoreactors

2019 Spring National Meeting

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.