Ferrocene-containing DNA assemblies

Ma, Yifeng ORCID: 0000-0001-8152-7573 (2024). Ferrocene-containing DNA assemblies. University of Birmingham. Ph.D.

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Abstract

In recent decades, significant achievements have been made in the development of modified nucleic acids and nucleic acid analogues. As far as metal-containing systems are concerned, ferrocene has emerged as a popular choice due to its stability, ease of functionalisation, and well-understood electrochemistry. It can also be readily incorporated into oligomeric strands using standard automated synthesis.

In this thesis, the scope of ferrocene-containing nucleic acids has been expanded in two main ways. Firstly, the design, assembly, and electrochemical characterisation of ferrocene-containing DNA tetrahedra are reported. These nanostructures, which contain ferrocene units located at up to four of their vertices, have been shown to form stable self-assembled monolayers (SAMs) on gold surfaces and exhibit reversible electrochemistry.

Secondly, a series of hybrid oligomer strands containing DNA and ferrocene nucleic acid (FcNA) units have been synthesised. The synthetic chemistry of the FcNA monomeric components has been optimised so that units with either two thymine or two cytosine units can be made in sufficient quantities for oligomerisation. Further evidence is provided using high field NMR spectroscopy for cross-duplex H-bonding between FcNA and DNA nucleobases within complementary duplexes. Furthermore, the FcNA unit has been shown to be compatible for templating the insertion of polymerase-mediated nucleotide triphosphates into growing DNA strands, providing the first example of a functional biological use for FcNA-containing oligonucleotides.

Type of Work:

Thesis (Doctorates > Ph.D.)

Award Type:

Doctorates > Ph.D.

Supervisor(s):