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Addressing the properties of “Metallo-DNA” with a Ag(I)-mediated supramolecular duplex

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Abstract

The silver-nucleoside complex [Ag(I)-(N3-cytidine)2], 1, self-assembles to form a supramolecular metal-mediated base-pair array highly analogous to those seen in metallo-DNA. A combination of complementary hydrogen-bonding, hydrophobic and argentophilic interactions drive the formation of a double-helix with a continuous silver core. Electrical measurements on 1 show that despite having Ag?Ag distances within <5% of the metallic radii, the material is electrically insulating. This is due to the electronic structure which features a filled valence band, an empty conduction band dominated by the ligand, and a band gap of 2.5 eV. Hence, as-prepared, such Ag(I)-DNA systems should not be considered molecular nanowires but, at best, proto-wires. The structural features seen in 1 are essentially retained in the corresponding organogel which exhibits thixotropic self-healing that can be attributed to the reversible nature of the intermolecular interactions. Photo-reduced samples of the gel exhibit luminescence confirming that these poly-cytidine sequences appropriately pre-configure silver ions for the formation of quantum-confined metal clusters in line with contemporary views on DNA-templated clusters. Microscopy data reveals the resulting metal cluster/particles are approximately spherical and crystalline with lattice spacing (111) similar to bulk Ag.


Publication metadata

Author(s): Mistry L, El-Zubir O, Dura G, Clegg W, Waddell PG, Pope T, Hofer WA, Wright NG, Horrocks BR, Houlton A

Publication type: Article

Publication status: Published

Journal: Chemical Science

Year: 2019

Volume: 10

Issue: 11

Pages: 3186-3195

Print publication date: 21/03/2019

Online publication date: 08/02/2019

Acceptance date: 08/02/2019

Date deposited: 18/02/2019

ISSN (print): 2041-6520

ISSN (electronic): 2041-6539

Publisher: Royal Society of Chemistry

URL: https://doi.org/10.1039/C8SC05103H

DOI: 10.1039/C8SC05103H


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