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Download fileAllosteric Control of Oxidative Catalysis by a DNA Rotaxane Nanostructure
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posted on 2017-10-23, 00:00 authored by Mathias Centola, Julián Valero, Michael FamulokDNA
is a versatile construction material for the bottom-up assembly
of structures and functional devices in the nanoscale. Additionally,
there are specific sequences called DNAzymes that can fold into tertiary
structures that display catalytic activity. Here we report the design
of an interlocked DNA nanostructure that is able to fine-tune the
oxidative catalytic activity of a split DNAzyme in a highly controllable
manner. As scaffold, we employed a double-stranded DNA rotaxane for
its ability to undergo programmable and predictable conformational
changes. Precise regulation of the DNAzyme’s oxidative catalysis
can be achieved by external stimuli (i.e., addition of release oligos)
that modify the spatial arrangement within the system, without interfering
with the catalytic core, similar to structural rearrangements that
occur in allosterically controlled enzymes. We show that multiple
switching steps between the active and inactive conformations can
be performed consistent with efficient regulation and robust control
of the DNA nanostructure.