Investigation of actinides(III)-DOTA complexes by electrospray ionization mass spectrometry

Audras, Matthieu; Berthon, Laurence; Martin, Nicolas P.; Zorz, Nicole; Moisy, Philippe

doi:10.1007/s10967-014-3672-2

Cited by 12 publications

(21 citation statements)

References 76 publications

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“…248 Cm, t½ = 340,000 yr) that can be produced and purified on the multi-gram scale, (ii) in aqueous solution it is exclusively found in the +III oxidation state and, (iii) trivalent Cm(III) can readily be sensitised by organic ligands in aqueous media. 40,[42][43][44][45][46][47][48][49][50][51] The three metal ions probed in this study, Eu(III), Tb(III), and Cm(III), are very similar in size, as indicated by their respective ionic radii (Fig. 1, r = 0.03 Å), and, from a coordination chemistry perspective, can almost exclusively be differentiated by the nature of their valence electrons.…”

Section: Introductionmentioning

confidence: 79%

“…[41][42][43] Here, we investigate a series of kinetically inert complexes of Eu(III), Tb(III), and Cm(III) to decipher subtle coordination differences between the 4f and 5f elements, using a macrocyclic ligand appended with an antenna chromophore (L, Figure 1). In the actinide series, Cm is a paradigm for direct comparisons with Tb(III) and Eu(III) since (i) it has long-lived isotopes (e.g.…”

Section: Introductionmentioning

confidence: 99%

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Investigating subtle 4f vs. 5f coordination differences using kinetically inert Eu(iii), Tb(iii), and Cm(iii) complexes of a coumarin-appended 1,4,7,10-tetraazacyclododecane-1,4,7-triacetate (DO3A) ligand

et al. 2018

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TitleInvestigating subtle 4f vs. 5f coordination differences using kinetically inert Eu(iii), Tb(iii), and Cm(iii) complexes of a coumarin-appended 1,4,7,10-tetraazacyclododecane-1,4,7-triacetate (DO3A) ligand In order to reveal subtle differences between the solution chemistries of trivalent 4f and 5f elements, the physicochemical and photophysical properties of europium(III), terbium(III) and curium(III) complexes formed with a 7-methoxy-coumarin appended 1,4,7,10-tetraazadodecane-1,4,7-triacid (DO3A) ligand were studied. All three complexes were found to be kinetically inert and exhibit stability constants similar to their 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA) equivalents. The Cm(III) and Eu(III) complexes feature strong sensitised emission, while the triplet energy of the coumarin prohibits efficient sensitisation of the Tb(III) analogue. The data presented here indicate significant differences in perturbation of the sensitising chromophore photophysics between the 4f and 5f elements. In contrast, the size of the metal center appears to not be a determining factor for the physicochemical properties of these kinetically inert Eu(III), Tb(III,) and Cm(III) complexes.

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Section: Introductionmentioning

confidence: 79%

Section: Introductionmentioning

confidence: 99%

Investigating subtle 4f vs. 5f coordination differences using kinetically inert Eu(iii), Tb(iii), and Cm(iii) complexes of a coumarin-appended 1,4,7,10-tetraazacyclododecane-1,4,7-triacetate (DO3A) ligand

et al. 2018

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“…In ESI-MS, variation of the skimmer voltage (in-source CID) can be used to study the change in the distribution of the ion intensity as a result of in-source fragmentation of the precursor ion [32]. Shown by Lyapchenko, the skimmer voltage corresponding to the maximum ion abundance is characteristic of a given ion and may be closely related to intrinsic properties of the ion [56].…”

Section: Influence Of Skimmer Voltage On Species Stabilitymentioning

confidence: 99%

“…One advantage of this technique that lends it to be quite useful in actinide studies is its low detection level, as only small amounts of sample are required for analysis [30][31][32][33]. Actinide species have been studied by ESI-MS since the early 1990's where the use of electrospray mass spectrometry was utilized for the analysis of various elements, including UO 2 2?…”

Section: Introductionmentioning

confidence: 99%

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Redox behavior of gas phase Pu(IV)-monodentate ligand complexes: an investigation by electrospray ionization mass spectrometry

Drader¹,

Martin²,

Boubals³

et al. 2016

J Radioanal Nucl Chem

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This study reports the gas phase complexation behavior of Pu(IV) with N,N-dialkylamide ligands and tributylphosphate by electrospray ionization mass spectrometry. In-source collision induced dissociation (CID) and ion trap collision induced dissociation were used to investigate the kinetic stability of Pu species in the gas phase. With both class of ligands, N,N-dialkylamide and trialkylphosphate, oxidation of Pu from the tetravalent state to the hexavalent state was observed at both high skimmer voltages and during ion trap CID. The results suggest that oxidation is due to the presence of a nitrate group in the coordination sphere of the metal and is independent of the ligand.

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Development of a large peptoid–DOTA combinatorial library

Singh¹,

Lopes

Udugamasooriya

2016

Biopolymers

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Conventional one-bead one-compound (OBOC) library synthesis is typically used to identify molecules with therapeutic value. The design and synthesis of OBOC libraries that contain molecules with imaging or even potentially therapeutic and diagnostic capacities (e.g. theranostic agents) has been overlooked. The development of a therapeutically active molecule with a built-in imaging component for a certain target is a daunting task, and structure-based rational design might not be the best approach. We hypothesize to develop a combinatorial library with potentially therapeutic and imaging components fused together in each molecule. Such molecules in the library can be used to screen, identify, and validate as direct theranostic candidates against targets of interest. As the first step in achieving that aim, we developed an on-bead library of 153,600 Peptoid-DOTA compounds in which the peptoids are the target-recognizing and potentially therapeutic components and the DOTA is the imaging component. We attached the DOTA scaffold to TentaGel beads using one of the four arms of DOTA, and we built a diversified 6-mer peptoid library on the remaining three arms. We evaluated both the synthesis and the mass spectrometric sequencing capacities of the test compounds and of the final library. The compounds displayed unique ionization patterns including direct breakages of the DOTA scaffold into two units, allowing clear decoding of the sequences. Our approach provides a facile synthesis method for the complete on-bead development of large peptidomimetic-DOTA libraries for screening against biological targets for the identification of potential theranostic agents in the future.

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Investigation of actinides(III)-DOTA complexes by electrospray ionization mass spectrometry

Cited by 12 publications

References 76 publications

Investigating subtle 4f vs. 5f coordination differences using kinetically inert Eu(iii), Tb(iii), and Cm(iii) complexes of a coumarin-appended 1,4,7,10-tetraazacyclododecane-1,4,7-triacetate (DO3A) ligand

Investigating subtle 4f vs. 5f coordination differences using kinetically inert Eu(iii), Tb(iii), and Cm(iii) complexes of a coumarin-appended 1,4,7,10-tetraazacyclododecane-1,4,7-triacetate (DO3A) ligand

Redox behavior of gas phase Pu(IV)-monodentate ligand complexes: an investigation by electrospray ionization mass spectrometry

Development of a large peptoid–DOTA combinatorial library

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