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Plutonium Biokinetics in Human Body A. Luciani - Kit-Bibliothek - FZK

Plutonium Biokinetics in Human Body A. Luciani - Kit-Bibliothek - FZK

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Recent technologic developments <strong>in</strong> <strong>Plutonium</strong> isotopes production made available<br />

amounts of 237 Pu with <strong>in</strong>creas<strong>in</strong>g levels of isotopes purity. Metabolism of <strong>Plutonium</strong> was<br />

<strong>in</strong>vestigated follow<strong>in</strong>g <strong>in</strong>travenous <strong>in</strong>jection of 237 Pu as Pu(IV) citrate <strong>in</strong> two healthy male<br />

volunteers [98, 99]. Excreta and blood samples were collected at <strong>in</strong>tervals dur<strong>in</strong>g the first 21<br />

days and measurements of their <strong>Plutonium</strong> content were carried out. The patterns of hepatic<br />

and skeletal uptake too were monitored up to 153 days after <strong>in</strong>jection with an external<br />

sc<strong>in</strong>tillation counter located close to liver, sacrum, knees and skull. Yet, these measurements<br />

provided only a limited <strong>in</strong>formation on organs uptake because of the difficulties <strong>in</strong><br />

discrim<strong>in</strong>at<strong>in</strong>g the contributions from activity <strong>in</strong> adjacent tissues and blood.<br />

Follow<strong>in</strong>g the same experimental methodology, ten further volunteers were<br />

<strong>in</strong>travenously <strong>in</strong>jected with 237 Pu(IV) [100]. Larger amounts of <strong>Plutonium</strong> were adm<strong>in</strong>istered<br />

<strong>in</strong> order to detect it <strong>in</strong> bioassays for a longer time after <strong>in</strong>jection. Moreover six women were<br />

<strong>in</strong>cluded <strong>in</strong> the studied groups of volunteers and sex-related differences <strong>in</strong> <strong>Plutonium</strong><br />

metabolism, particularly <strong>in</strong> the excreta, were <strong>in</strong>vestigated and considerations were extended<br />

also to other act<strong>in</strong>ides [101]. Samples of ur<strong>in</strong>e, feces and blood were collected and measured<br />

at <strong>in</strong>tervals for the first 21 days after <strong>in</strong>jection. Further samples were collected and analyzed at<br />

around 40 and 90 days post <strong>in</strong>jection. Measurements of hepatic uptake and gonads deposition<br />

were also carried out [102, 103].<br />

2.1.2 EMPIRICAL CURVES<br />

The orig<strong>in</strong>al data set from Langham’s subjects has been used and re-evaluated<br />

numerous times over the years by various researchers. This confirms the importance and<br />

orig<strong>in</strong>ality of these first experiments that were for different decades the only source of direct<br />

knowledge about <strong>Plutonium</strong> biok<strong>in</strong>etics. One of the first modifications of Langham’s ur<strong>in</strong>ary<br />

excretion curve was proposed by Beach and Dolph<strong>in</strong> [104] to dist<strong>in</strong>guish two phases <strong>in</strong> the<br />

<strong>Plutonium</strong> excretion: an <strong>in</strong>itial rapid excretion of the <strong>in</strong>jected <strong>Plutonium</strong> <strong>in</strong> the citrate form<br />

and the lower excretion rate of metabolized plutonium. This approach yielded a non<strong>in</strong>tegrable<br />

equation for which a graphical solution was provided.<br />

As a result of the developments <strong>in</strong> computer programm<strong>in</strong>g slight discrepancies were<br />

observed between Langham’s function and the functions calculated by m<strong>in</strong>imization rout<strong>in</strong>e<br />

with computer. On this basis the follow<strong>in</strong>g function for the percentage daily ur<strong>in</strong>ary excretion<br />

was calculated by Robertson and Cohn [105] with the Brookhaven Merl<strong>in</strong> computer:<br />

eu(t) = 0.193t −0.721<br />

36<br />

equation 2.1.4<br />

Yet the most important and <strong>in</strong>terest<strong>in</strong>g re-evaluation of Langham’s subjects data set<br />

was carried out at the beg<strong>in</strong>n<strong>in</strong>g of seventies by Durb<strong>in</strong> [106]. A meticulous re-exam<strong>in</strong>ation<br />

of the orig<strong>in</strong>al data was carried out particularly consider<strong>in</strong>g the physiological and health status<br />

of the <strong>in</strong>vestigated subjects and <strong>in</strong>tegrat<strong>in</strong>g the available data with occupational exposure and<br />

laboratory animals’ data. The need of a <strong>Plutonium</strong> ur<strong>in</strong>ary excretion curve representative of<br />

an adult human be<strong>in</strong>g <strong>in</strong> good health was po<strong>in</strong>ted out. Therefore only the data from those<br />

subjects without abnormal kidney function or abnormal plasma <strong>Plutonium</strong> b<strong>in</strong>d<strong>in</strong>g due to<br />

anaemic status were considered, because irregular <strong>Plutonium</strong> ur<strong>in</strong>ary excretion rates were<br />

observed for subjects characterized by such pathologies. Moreover differences <strong>in</strong> biok<strong>in</strong>etics<br />

of Pu(IV) and Pu(VI) were po<strong>in</strong>ted out, particularly for the early ur<strong>in</strong>ary excretion. As the<br />

Pu(IV) oxidation state was deemed likely to be the chemical form of <strong>Plutonium</strong> commonly

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