Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 4, Pages 1662-1666Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b09407
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Funding
- Hungarian National Research, Development and Innovation Office [NKFIH K-120224]
- Janos Bolyai Research Scholarship of the Hungarian Academy of Sciences
- Ministry of Human Capacities [UNKP-18-4]
- EU
- European Regional Development Fund [GINOP-2.3.2-15-2016-00008]
- COST action European Network on NMR Relaxometry [CA 15209]
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Smart/intelligent contrast agent candidates for MRI based on Mn(II) ion are rare, as it usually forms labile complexes with polyaminocarboxylate-type ligands. Here, we report the first example of a Mn(II) complex that can be activated by changing the pH of its local environment. The PC2A-EA ligand with an ethylamine pendant arm was found to form a thermodynamically stable (log K-MnL = 19.01, pMn = 9.27) and kinetically inert complex with Mn(II) with respect to trans-chelation with a metal ion such as Cu(II). The [MnH(PCA2-EA)] complex displays a relatively slow water exchange rate ((4.0 +/- 0.2) x 10(7) s(-1)), but the pH-dependent coordination of the ethylamine moiety occurs in the pH range of 6-8 (log K-MnL(H) = 6.88), enabling the complex to exhibit pH-sensitive relaxivity in the biologically relevant pH range.
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