A pyrophosphate-responsive gadolinium(III) MRI contrast agent

A.J. Surman, C.S. Bonnet, M.P. Lowe, G.D. Kenny, J.D. Bell, E. Tõth, R. Vilar

Research output: Contribution to journalArticlepeer-review

32 Citations (Scopus)


This study shows that the relaxivity and optical properties of functionalised lanthanide-DTPA-bis-amide complexes (lanthanide=Gd(3+) and Eu(3+) , DTPA=diethylene triamine pentaacetic acid) can be successfully modulated by addition of specific anions, without direct Ln(3+) /anion coordination. Zinc(II)-dipicolylamine moieties, which are known to bind strongly to phosphates, were introduced in the amide "arms" of these ligands, and the interaction of the resulting Gd-Zn(2) complexes with a range of anions was screened by using indicator displacement assays (IDAs). Considerable selectivity for polyphosphorylated species (such as pyrophosphate and adenosine-5'-triphosphate (ATP)) over a range of other anions (including monophosphorylated anions) was apparent. In addition, we show that pyrophosphate modulates the relaxivity of the gadolinium(III) complex, this modulation being sufficiently large to be observed in imaging experiments. To establish the binding mode of the pyrophosphate and gain insight into the origin of the relaxometric modulation, a series of studies including UV/Vis and emission spectroscopy, luminescence lifetime measurements in H(2) O and D(2) O, (17) O and (31) P NMR spectroscopy and nuclear magnetic resonance dispersion (NMRD) studies were carried out.
Original languageEnglish
Pages (from-to)223-230
Number of pages8
JournalChemistry (Weinheim an der Bergstrasse, Germany)
Issue number1
Early online date7 Dec 2010
Publication statusPublished - 3 Jan 2011


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