Is hydroxypyridonate 3,4,3-LI(1,2-HOPO) a good competitor of fetuin for uranyl metabolism?

Younes, Ali; Creff, Gaëlle; Beccia, Maria Rosa; Moisy, Philippe; Roques, Jérôme; Aupiais, Jean; Hennig, Christoph; Solari, Pier Lorenzo; Auwer, Christophe Den; Vidaud, Claude

doi:10.1039/c8mt00272j

Cited by 12 publications

(20 citation statements)

References 48 publications

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“…Such features are indicative of the axial U−O pairs (hereby denoted U−O ax ) of an "yl" complex 42 and are consistent with the presence of the high energy shoulder in the XANES spectra for each of the U IV -343-chelator complexes (Figure 2). When fits 22 The EXAFS spectrum of U VI -343-HOPO has been collected previously 10 but was recollected here to allow for comparison with U IV -343-HOPO, as well as U VI complexes with the other 343-chelators. The FT of the EXAFS spectra for U VI with all four 343-chelators revealed the characteristic two peaks that are well-known for actinyl moieties (Figure S2, Supporting Information).…”

Section: ■ Introductionmentioning

confidence: 99%

Controlling the Reduction of Chelated Uranyl to Stable Tetravalent Uranium Coordination Complexes in Aqueous Solution

et al. 2020

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The solution-state interactions between octadentate hydroxypyridinone (HOPO) and catecholamide (CAM) chelating ligands and uranium were investigated and characterized by UV− visible spectrophotometry and X-ray absorption spectroscopy (XAS), as well as electrochemically via spectroelectrochemistry (SEC) and cyclic voltammetry (CV) measurements. Depending on the selected chelator, we demonstrate the controlled ability to bind and stabilize U IV , generating with 3,4,3-LI(1,2-HOPO), a tetravalent uranium complex that is practically inert toward oxidation or hydrolysis in acidic, aqueous solution. At physiological pH values, we are also able to bind and stabilize U IV to a lesser extent, as evidenced by the mix of U IV and U VI complexes observed via XAS. CV and SEC measurements confirmed that the U IV complex formed with 3,4,3-LI(1,2-HOPO) is redox inert in acidic media, and U VI ions can be reduced, likely proceeding via a two-electron reduction process.

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Section: ■ Introductionmentioning

confidence: 99%

Controlling the Reduction of Chelated Uranyl to Stable Tetravalent Uranium Coordination Complexes in Aqueous Solution

et al. 2020

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“…Both are significant, because intake of uranium from sources such as contaminated drinking water have been linked to nephrotoxicity and osteotoxicity and pose a health risk as a result . Uranium’s threat to health comes from its chemical rather than its radiological properties, partially because the specific activity of natural uranium, ranging from 25.272 Becquerel (Bq)/mg, is very low. , The human body normally manages metal toxicity by excretion or retention of the metal in a biochemically inactive form. From the bloodstream, metals can be eliminated through ultrafiltration by the kidneys or deposition into target organs, but most accumulate and are fixed in the skeleton, which limits bioavailability.…”

Section: Introductionmentioning

confidence: 99%

“…Fetuin has the highest affinity constant (KD = ∼30 nM) among the 12 major serum proteins for uranyl and can bind three uranyl ions at three different binding sites. Because fetuin participates in bone mineralization and its life cycle ends in the bone, it is also a key protagonist in uranyl contamination . As a result, fetuses are especially susceptible to the contamination.…”

Section: Introductionmentioning

confidence: 99%

“…Because fetuin participates in bone mineralization and its life cycle ends in the bone, it is also a key protagonist in uranyl contamination. 8 As a result, fetuses are especially susceptible to the contamination. Within the kidneys, uranyl complexes must filter through renal glomeruli, and because their structure only allows carbonate and citrate uranyl complexes to pass, the complexes are in direct contact with proximal tubule epithelium and, as such, are toxic for epithelial cells.…”

Section: ■ Introductionmentioning

confidence: 99%

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Uptake and Removal of Uranium by and from Human Teeth

Younes

Ali

Duda

et al. 2021

Chem. Res. Toxicol.

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Uranium-238 ( 238 U), a long-lived radiometal, is widespread in the environment because of both naturally occurring processes and anthropogenic processes. The ingestion or inhalation of large amounts of U is a major threat to humans, and its toxicity is considered mostly chemical rather than radiological. Therefore, a way to remove uranium ingested by humans from uraniumcontaminated water or from the air is critically needed. This study investigated the uranium uptake by hydroxyapatite (HAP), a compound found in human bone and teeth. The uptake of U by teeth is a result of U transport as dissolved uranyl (UO 2 2+) in contaminated water, and U adsorption has been linked to delays in both tooth eruption and development. In this present work, the influence of pH, contact time, initial U concentration, and buffer solution on the uptake and removal of U in synthetic HAP was investigated and modeled. The influence of pH (pH of human saliva, 6.7−7.4) on the uptake of uranyl was negligible. Furthermore, the kinetics were extremely fast; in one second of exposure, 98% of uranyl was uptaken by HAP. The uptake followed pseudosecond-order kinetics and a Freundlich isotherm model. A 0.2 M sodium carbonate solution removed all the uranyl from HAP after 1 h. Another series of in vitro tests were performed with real teeth as targets. We found that, for a 50 mg/L U in PBS solution adjusted to physiological pH, ∼35% of the uranyl was uptaken by the tooth after 1 h, following pseudo-first-order kinetics. Among several washing solutions tested, a commercially available carbonate, as well as a commercially available fluoride solution, enabled removal of all the uranyl taken up by the teeth.

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“…Taking inspiration from the Raymond group's use of the hydroxypyridone motif (HOPO, Fig. 1) due to its high affinity for REs in aqueous conditions [39][40][41][42] and potential biomedical applications [43][44][45][46] , we synthesized the novel proligand tris[(1-hydroxy-2-oxo-1,2-dihydropyridine-3-carboxamido)-ethyl]amine, H 3 tren-1,2,3-HOPO·TFA (H 3 1·TFA). We hypothesized that exchanging the positions of the hydroxyl and carbonyl moieties would maintain the high affinity of HOPOderivates for REs while allowing for bridging interactions that were critical for the separations selectivity of our H 3 TriNOx system [35][36][37][38] .…”

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confidence: 99%

High-throughput screening for discovery of benchtop separations systems for selected rare earth elements

et al. 2020

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Rare earth (RE) elements (scandium, yttrium, and the lanthanides) are critical for their role in sustainable energy technologies. Problems with their supply chain have motivated research to improve separations methods to recycle these elements from end of life technology. Toward this goal, we report the synthesis and characterization of the ligand tris[(1-hydroxy-2-oxo-1, 2-dihydropyridine-3-carboxamido)ethyl]amine, H 3 1·TFA (TFA = trifluoroacetic acid), and complexes 1·RE (RE = La, Nd, Dy). A high-throughput experimentation (HTE) screen was developed to quantitatively determine the precipitation of 1·RE as a function of pH as well as equivalents of H 3 1·TFA. This method rapidly determines optimal conditions for the separation of RE mixtures, while minimizing materials consumption. The HTE-predicted conditions are used to achieve the lab-scale separation of Nd/Dy (SF Nd/Dy = 213 ± 34) and La/Nd (SF La/Nd = 16.2 ± 0.2) mixtures in acidic aqueous media.

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Is hydroxypyridonate 3,4,3-LI(1,2-HOPO) a good competitor of fetuin for uranyl metabolism?

Abstract: Identification of stable HOPO–UO22+–fetuin ternary complexes after a chromatographic separation process.

Cited by 12 publications

References 48 publications

Controlling the Reduction of Chelated Uranyl to Stable Tetravalent Uranium Coordination Complexes in Aqueous Solution

Controlling the Reduction of Chelated Uranyl to Stable Tetravalent Uranium Coordination Complexes in Aqueous Solution

Uptake and Removal of Uranium by and from Human Teeth

High-throughput screening for discovery of benchtop separations systems for selected rare earth elements

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