Block Copolymer Micellization of DNA Origami Promotes Solubility in Organic Solvents

The DNA origami technique allows the precise synthesis
of complex,
biocompatible nanomaterials containing small molecules, biomolecules,
and inorganic nanoparticles. The negatively charged phosphates in
the backbone make DNA highly water-soluble and require salts to shield
its electrostatic repulsion. DNA origamis are therefore not soluble
in most organic solvents. While this is not problematic for applications
in biochemistry, biophysics, or nanomedicine, other potential applications,
processes, and substrates are incompatible with saline solutions,
which include the synthesis of many nanomaterials, and reactions in
templated synthesis, the operation of nanoelectronic devices, or semiconductor
fabrication. To overcome this limitation, we coated DNA origami with
amphiphilic poly(ethylene glycol) polylysine block copolymers and
transferred them into various organic solvents including chloroform,
dichloromethane, acetone, or 1-propanol. Our approach maintains the
shape of the nanostructures and protects functional elements bound
to the structure, such as fluorophores, gold nanoparticles, or proteins.
The DNA origami polyplex micellization (DOPM) strategy hence enables
solubilization or a phase transfer of complex structures into various
organic solvents, which significantly expands the use of DNA origami
for a range of potential applications and technical processes.