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An amphiphilic-DNA platform for the design of crystalline frameworks with programmable structure and functionality

Accepted version
Peer-reviewed

Type

Article

Change log

Authors

Brady, Ryan 
Brooks, Nicholas 
Fodara, Vito 
Di Michele, Lorenzo  ORCID logo  https://orcid.org/0000-0002-1458-9747

Abstract

The reliable preparation of functional, ordered, nanostructured frameworks would be a game changer for many emerging technologies, from energy storage to nanomedicine. Underpinned by the excellent molecular recognition of nucleic acids, along with their facile synthesis and breadth of available functionalizations, DNA Nanotechnology is widely acknowledged as a prime route for the rational design of nanostructured materials. Yet, the preparation of crystalline DNA frameworks with programmable structure and functionality remains a challenge. Here we demonstrate the potential of simple amphiphilic DNA motifs, dubbed C-stars, as a versatile platform for the design of programmable DNA crystals. In contrast to all-DNA materials, in which structure depends on the precise molecular details of individual build-ing blocks, the self-assembly of C-stars is controlled uniquely by their topology and symmetry. Exploiting this robust self-assembly principle we design a range of topologically identical, but structurally and chemically distinct C-stars that following a one-pot reaction self- assemble into highly porous, functional, crystalline frameworks. Simple design variations allow us to fine-tune the lattice parameter and thus control the partitioning of macromolecules within the frameworks, embed responsive motifs that can induce isothermal disassembly, and include chemical moieties to capture target proteins specifically and reversibly.

Description

Keywords

DNA, Green Fluorescent Proteins, Nanostructures, Nanotechnology, Nucleic Acid Conformation, Osmolar Concentration, Particle Size, Surface-Active Agents

Journal Title

Journal of the American Chemical Society

Conference Name

Journal ISSN

1520-5126
1520-5126

Volume Title

Publisher

American Chemical Society (ACS)
Sponsorship
Leverhulme Trust (ECF-2015-494)
Isaac Newton Trust (MIN 1508(S))
Royal Society (UF160152)
Royal Society (RGF/R1/180043)
EPSRC (via Imperial College London) (CHIS_P39012)
EPSRC (1494571)
Engineering and Physical Sciences Research Council (EP/L015978/1)
Engineering and Physical Sciences Research Council (EP/J017566/1)
LDM, PC and NJB acknowledge support from the EPSRC Programme Grant CAPITALS number EP/J017566/1. LDM acknowledges support from the Leverhulme Trust and the Isaac Newton Trust through an Early Career Fellow- 9 ship (ECF-2015-494) and from the Royal Society through a University Research Fellowship (UF160152). RAB acknowledges support from the EPSRC CDT in Nanoscience and Nanotechnology (NanoDTC), grant number EP/L015978/1.
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