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锕-228 发生器的制备。

Preparation of an Actinium-228 Generator.

机构信息

Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States of America.

出版信息

Inorg Chem. 2020 Mar 2;59(5):3200-3206. doi: 10.1021/acs.inorgchem.9b03563. Epub 2020 Feb 16.

Abstract

Advances in targeted α-therapies have increased the interest in actinium (Ac), whose chemistry is poorly defined due to scarcity and radiological hazards. Challenges associated with characterizing Ac chemistry are magnified by its 5f6d electronic configuration, which precludes the use of many spectroscopic methods amenable to small amounts of material and low concentrations (like EPR, UV-vis, fluorescence). In terms of nuclear spectroscopy, many actinium isotopes (Ac and Ac) are equally "unfriendly" because the actinium α-, β-, and γ-emissions are difficult to resolve from the actinium daughters. To address these issues, we developed a method for isolating an actinium isotope (Ac) whose nuclear properties are well-suited for γ-spectroscopy. This four-step procedure isolates Ra from naturally occurring Th. The relatively long-lived Ra ( = 5.75(3) years) radioisotope subsequently decays to Ac. Because the Ac decay rate [ = 6.15(2) h] is fast, Ac rapidly regenerates after being harvested from the Ra parent. The resulting Ac generator provides frequent and long-term access (of many years) to the spectroscopically "friendly" Ac radionuclide. We have demonstrated that the Ac product can be routinely "milked" from this generator on a daily basis, in chemically pure form, with high specific activity and in excellent yield (∼95%). Hence, in the same way that developing synthesis routes to new starting materials has advanced coordination chemistry for many metals by broadening access, this Ac generator has the potential to broaden actinium access for the inorganic community, facilitating the characterization of actinium chemical behavior.

摘要

靶向 α 疗法的进展增加了人们对锕(Ac)的兴趣,由于锕的稀缺性和放射性危害,其化学性质还没有得到很好的定义。由于其 5f6d 电子构型,锕化学的特点是难以用许多适用于少量材料和低浓度的光谱方法来描述(如 EPR、UV-vis、荧光),因此,表征锕化学所面临的挑战更加艰巨。就核光谱学而言,许多锕同位素(Ac 和 Ac)同样“不友好”,因为锕的 α、β 和 γ 发射很难与锕的子体区分开来。为了解决这些问题,我们开发了一种分离锕同位素(Ac)的方法,该同位素的核性质非常适合γ光谱学。这个四步程序从天然存在的钍中分离出镭。相对长寿命的镭( = 5.75(3) 年)放射性同位素随后衰变为锕。由于 Ac 的衰变率 [ = 6.15(2) h] 很快,因此 Ac 可以在从 Ra 母体中收获后迅速再生。由此产生的 Ac 发生器可以提供频繁且长期(多年)获得光谱学上“友好”的 Ac 放射性核素的机会。我们已经证明,Ac 产物可以每天以化学纯形式、高比活度和极好的产率(约 95%)从该发生器中常规地“提取”出来。因此,就像开发新起始材料的合成途径通过拓宽通道来推进许多金属的配位化学一样,这种 Ac 发生器有可能拓宽无机界对锕的获取途径,从而促进对锕化学行为的表征。

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