期刊
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
卷 -, 期 18, 页码 2435-2443出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/ejic.201700176
关键词
Copper; Macrocyclic ligands; N ligands; Imaging agents; Potentiometry
资金
- FEDER funds through COMPETE2020 - Programa Operacional Competitividade e Interna-cionalizacao (POCI) [LISBOA-01-0145-FEDER-007660]
- FCT (Fundacao para a Ciencia e a Tecnologia) [SFRH/BPD/73361/2010]
- Fundação para a Ciência e a Tecnologia [SFRH/BPD/73361/2010] Funding Source: FCT
Three 1,4,7-triazacyclononane-based (tacn-based) ligands containing picolyl and picolinate pendant arms (no3py, no2pa1py, and no3pa) were synthesized, and their copper(II) complexation properties were studied to evaluate their potentials as chelators for copper radioisotopes. The thermodynamic stability constants of the complexes were determined by potentiometric titrations. These studies evidenced the formation of mononuclear species for no3py and mono- and dinuclear species for no2pa1py and no3pa. The pCu values decreased as the number of carboxypicolyl arms increased. The [Cu(no3py)](2+) complex presented a very high stability constant (logK(CuL) = 27.4) and a very high selectivity towards Zn2+ ions (logK(ZnL) = 17.25). Vis/NIR (NIR = near-infrared) absorption and electron paramagnetic resonance (EPR) spectroscopy indicated that the three complexes present distorted octahedral geometries with two paramagnetic species, which were identified as the () and () isomers [and their corresponding enantiomeric forms () and ()] by DFT calculations. The electrochemical properties were investigated by cyclic voltammetry, which revealed quasireversible behavior for the [Cu(no3py)](2+) complex but irreversible Cu2+/Cu+ systems for [Cu(no2pa1py)] and [Cu(no3pa)](-).
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