Interaction of Transuranium Elements with Biologically Important Ligands: Structural and Spectroscopic Evidence for Nucleotide Coordination to Plutonium

Andreev, G. B.; Budantseva, N. A.; Sokolova, M. N.; Тананаев, И. Г.; Myasoedov, Β. F.

doi:10.1021/ic802053s

Cited by 13 publications

(13 citation statements)

References 17 publications

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“…Although, the coordination of the 5'-phosphate group and the 2'-and 3'-hydroxyl groups of the ribose to the U(VI) is similar to that suggested earlier by Feldman, the number and the structures of the formed complexes are different [8]. With transuranium elements, very recently, a first crystallographic structure of a Pu-nucleotide complex has been published in the literature with the deoxycytidinemonophosphate-Pu(IV) complex [9].…”

Section: Introductionsupporting

confidence: 60%

Actinide Complexation with Biomimetic Phosphorylated Molecules

et al. 2012

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International audienceMost data available on the interaction of actinides with biological systems are based on physiological or biokinetic measurements, with scarce information on the structure of the actinide coordination site. This proceeding article describes an approach for structural elucidation of actinide biological complexes. Indeed most of c.a. actinide circulation pathways are unknown, as they accumulate mostly in bones, kidney and liver. In case of accidental release of radionuclide in the environment, internal contamination under either acute or chronic conditions has the potential to induce both radiological and chemical toxicity through significant interaction with the metabolome or proteome followed by possible functional modifications. For instance, the metalloproteins present primary, secondary and tertiary structures, and also different post-translational modifications, all playing a crucial role in interacting with their partners, which can be altered by actinide bonding. When tightly bound, metal ions are critical to the function, structure, and stability of the proteins, by disabling specific interactions through significant local or global conformational modifications. In order to overcome the intricacy of actinide chemistry combined with that of metalloproteins, a simplified study toward better understanding the interaction of actinides and biological systems using simple biomolecules such as amino acids has therefore been considered. Focus is made on the cation coordination site itself, given that conformational effects are not taken into account in this approach. In a first step, we have selected simple phosphorylated building blocks that may be considered as chemical representatives of some ubiquitous target metalloproteins or some important phosphorylated peptides or proteins

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Section: Introductionsupporting

confidence: 60%

Actinide Complexation with Biomimetic Phosphorylated Molecules

et al. 2012

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“…1À to Th 4+ , U 4+ , Np 4+ , Pu 3+ , Am 3+ , Nd 3+ , Sm 3+ , Gd 3+ , and Eu 3+ . 20,[42][43][44][45][46][47][48] This structural data was consistent with the EXAFS model included here. It is unclear to us why metal-ligand bonds would be shorter for neutral H 2 O vs. anionic O 2 CMe 1À ligands.…”

Section: Solution-phase Speciationsupporting

confidence: 87%

Advancing understanding of actinide(iii) (Ac, Am, Cm) aqueous complexation chemistry

et al. 2021

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“…The presence of O and P atoms in the first and second coordination shells of M = Th(IV), Pu(IV) was determined via EXAFS spectroscopy and confirmed by ab initio MD calculations. EXAFS best fit distances and ab initio MD distances agree within 0.1 Å. Distances in both PEI-MP-Pu and PEI-MP-Th complexes are very similar to the intermolecular distances found in other Pu-phosphonate complexes 61,62.…”

supporting

confidence: 66%

“…An example is given by Andreev et al, who described the structure of a plutunium nucleotide complex (deoxycytidinemonophosphate, H 2 dCMP). 62 In this structure, there are two independent Pu atoms with similar environments: three O atoms of the monodentate phosphates belonging to three HdCMP − anions, two bidentate nitrate anions, and two water molecules. The three O phosphate atoms are located at an average of 2.21 Å.…”

Section: ■ Experimental Sectionmentioning

confidence: 99%

“…In the real polymer, this N atom would be closer and the coordination would be larger than 7. The EXAFS adjustment Pu-nucleotide complex (deoxycytidinemonophosphate acid, H2dCMP) 62. In this structure, there are 2 independent Pu atoms with similar environments: three O atoms of the monodentate phosphates belonging to three HdCMPanions, two bidentate nitrate anions, and two water molecules.…”

mentioning

confidence: 99%

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Carboxylate- and Phosphonate-Modified Polyethylenimine: Toward the Design of Actinide Decorporation Agents

et al. 2019

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Plutonium (Pu) is an anthropogenic element involved in the nuclear industry cycle. Located at the bottom of the periodic table within the actinide family, it is a chemical toxic but also a radiological toxic, regardless of isotopy. After nearly 80 years of plutonium industrialization, it has become clear that inhalation and wounds represent the two main ways a person may become contaminated after an accident. In order to reduce the deleterious health effects of Pu, it is crucial to limit chronic exposure by removing it or preventing its incorporation into the body. Diethylene triamine penta acetic acid (DTPA) has emerged as the gold standard for plutonium decorporation, although it suffers from very short retention time in serum. Other molecules like the hydroxypyridonate family with high chemical affinity have also been considered. We have been considering alternative polymeric chelates and, in particular, polyethyleneimine (PEI) analogues of DTPA (carbonate or phosphonate version), which may present a real breakthrough in plutonium decorporation not only because of their higher loading capacity, but also because of their indirect vectorization properties correlated with a specific biodistribution into the lungs, bone, kidney or liver. In the first part of this forum article, new data on the structural characterization of the complexation of Pu(IV) with polyethyleneimine methylphosphonate (PEI-MP) were obtained using the combination of EXAFS spectroscopy (Extended X-Ray Absorption Fine Structure) and ab initio Molecular Dynamics calculations (AIMD). The use of thorium (Th) as a Pu chemical

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Interaction of Transuranium Elements with Biologically Important Ligands: Structural and Spectroscopic Evidence for Nucleotide Coordination to Plutonium

Cited by 13 publications

References 17 publications

Actinide Complexation with Biomimetic Phosphorylated Molecules

Actinide Complexation with Biomimetic Phosphorylated Molecules

Advancing understanding of actinide(iii) (Ac, Am, Cm) aqueous complexation chemistry

Carboxylate- and Phosphonate-Modified Polyethylenimine: Toward the Design of Actinide Decorporation Agents

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