Abstract
After entering the blood, plutonium accumulates mainly in the liver and the bones. The mechanisms leading to its accumulation in bone are, however, completely unknown. We already know that another uptake pathway not involving the transferrin-mediated pathways is suspected to intervene in the case of the liver. Fetuin, a protein playing an important role in bone metabolism, is proposed as a potential transporter of Pu from serum to bone. For the first time, the binding constants of these two proteins (transferrin and fetuin) with tetravalent plutonium at physiological pH (pH 7.0) were determined by using capillary electrophoresis (CE) coupled with inductively coupled plasma mass spectrometry (ICP-MS). Their very close values (log10 KPuTf = 26.44 ± 0.28 and log10 KPuFet = 26.20 ± 0.24, respectively) suggest that transferrin and fetuin could compete to chelate plutonium, either in the blood or directly at bone surfaces in the case of Pu deposits. We performed competition reaction studies demonstrating that the relative distribution of Pu-protein complexes is fully explained by thermodynamics. Furthermore, considering the average concentrations of transferrin and fetuin in the blood, our calculation is consistent with the bio-distribution of Pu observed in humans.
Highlights
After entering the blood, plutonium accumulates mainly in the liver and the bones
A coupling between capillary electrophoresis and inductively coupled plasma mass spectrometry (CE-ICP-MS) was performed to monitor metal binding on the proteins
Due to the high radiotoxicity of plutonium, the only analytical tools that allow the chemical behaviour of plutonium species to be investigated are those that involve the coupling of mass spectrometry with separation techniques
Summary
Plutonium accumulates mainly in the liver and the bones. The mechanisms leading to its accumulation in bone are, completely unknown. A coupling between capillary electrophoresis and inductively coupled plasma mass spectrometry (CE-ICP-MS) was performed to monitor metal binding on the proteins. Taking into account their respective concentrations in serum and their binding constants, a distribution of Pu between the two proteins can be calculated.
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