Research & Teaching Faculty

Metal ion size profoundly affects H3glyox chelate chemistry

TitleMetal ion size profoundly affects H3glyox chelate chemistry
Publication TypeJournal Article
Year of Publication2021
AuthorsChoudhary, N, Barrett, KE, Kubeil, M, Radchenko, V, Engle, JW, Stephan, H, Jaraquemada-Peláez, Mde Guadalu, Orvig, C
JournalRSC Adv.
Volume11
Pagination15663-15674
Date Published04/2021
Abstract

The bisoxine hexadentate chelating ligand{,} H3glyox was investigated for its affinity for Mn2+{,} Cu2+ and Lu3+ ions; all three metal ions are relevant with applications in nuclear medicine and medicinal inorganic chemistry. The aqueous coordination chemistry and thermodynamic stability of all three metal complexes were thoroughly investigated by detailed DFT structure calculations and stability constant determination{,} by employing UV in-batch spectrophotometric titrations{,} giving pM values (pM = −log[Mn+]free when [Mn+] = 1 μM{,} [L] = 10 μM at pH 7.4 and 25 °C) – pCu (25.2) > pLu (18.1) > pMn (12.0). DFT calculated structures revealed different geometries and coordination preferences of the three metal ions; notable was an inner sphere water molecule in the Mn2+ complex. H3glyox labels [52gMn]Mn2+{,} [64Cu]Cu2+ and [177Lu]Lu3+ at ambient conditions with apparent molar activities of 40 MBq μmol−1{,} 500 MBq μmol−1 and 25 GBq μmol−1{,} respectively. Collectively{,} these initial investigations provide insight into the effects of metal ion size and charge on the chelation with the hexadentate H3glyox and indicate that further investigations of the Mn2+–H3glyox complex in 52g/55Mn-based bimodal imaging might be worthwhile.

URLhttp://dx.doi.org/10.1039/D1RA01793D
DOI10.1039/D1RA01793D
Refereed DesignationRefereed