Peer-Reviewed Journal Details
Mandatory Fields
McStay, N;Molphy, Z;Coughlan, A;Cafolla, A;McKee, V;Gathergood, N;Kellett, A
2017
January
Nucleic Acids Research
C-3-symmetric opioid scaffolds are pH-responsive DNA condensation agents
Published
4 ()
Optional Fields
MULTIVALENT CATIONS PLATINUM COMPLEXES TRIVALENT CATIONS CRYSTAL-STRUCTURE LIGHT-SCATTERING GROOVE BINDING RECOGNITION MORPHINE SELECTIVITY TRANSITION
45
527
540
Herein we report the synthesis of tripodal C-3-symmetric opioid scaffolds as high-affinity condensation agents of duplex DNA. Condensation was achieved on both supercoiled and canonical B-DNA structures and identified by agarose electrophoresis, viscosity, turbidity and atomic force microscopy (AFM) measurements. Structurally, the requirement of a tris-opioid scaffold for condensation is demonstrated as both di-(C-2-symmetric) and mono-substituted (C-1-symmetric) mesitylenelinked opioid derivatives poorly coordinate dsDNA. Condensation, observed by toroidal and globule AFM aggregation, arises from surface-binding ionic interactions between protonated, cationic, tertiary amine groups on the opioid skeleton and the phosphate nucleic acid backbone. Indeed, by converting the 6-hydroxyl group of C-3-morphine (MC3) to methoxy substituents in C-3-heterocodeine (HC3) and C-3-oripavine (OC3) molecules, dsDNA compaction is retained thus negating the possibility of phosphate--hydroxyl surface-binding. Tripodal opioid condensation was identified as pH dependent and strongly influenced by ionic strength with further evidence of cationic amine-phosphate backbone coordination arising from thermal melting analysis and circular dichroism spectroscopy, with compaction also witnessed on synthetic dsDNA co-polymers poly[d(A-T)(2)] and poly[ d(G-C)(2)]. On-chip microfluidic analysis of DNA condensed by C-3-agents provided concentration-dependent protection (inhibition) to site-selective excision by type II restriction enzymes: BamHI, HindIII, SalI and EcoRI, but not to the endonuclease DNase I.
OXFORD
0305-1048
10.1093/nar/gkw1097
Grant Details