Ultra-Efficient Americium/Lanthanide Separation through Oxidation State Control,Journal of the American Chemical Society

当前位置： X-MOL 学术 › J. Am. Chem. Soc. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Ultra-Efficient Americium/Lanthanide Separation through Oxidation State Control
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-03-30 , DOI: 10.1021/jacs.2c00594
Zhipeng Wang ₁ , Jun-Bo Lu ₂ , Xue Dong ₁ , Qiang Yan ₁ , Xiaogui Feng ₁ , Han-Shi Hu ₃ , Shuao Wang ₄ , Jing Chen ₁ , Jun Li _{2,

3} , Chao Xu ₁

Affiliation

Lanthanide/actinide separation is a worldwide challenge for atomic energy and nuclear waste treatment. Separation of americium (Am), a critical actinide element in the nuclear fuel cycle, from lanthanides (Ln) is highly desirable for minimizing the long-term radiotoxicity of nuclear waste, yet it is extremely challenging given the chemical similarity between trivalent Am(III) and Ln(III). Selective oxidation of Am(III) to a higher oxidation state (OS) could facilitate this separation, but so far, it is far from satisfactory for practical application as a result of the unstable nature of Am in a high OS. Herein, we find a novel strategy to generate stable pentavalent Am (Am(V)) through coordination of Am(III) with a diglycolamide ligand and oxidation with Bi(V) species in the presence of an organic solvent. This strategy leads to efficient stabilization of Am(V) and an extraordinarily high separation factor (>10⁴) of Am from Ln through one single contact in solvent extraction, thereby opening a new avenue to study the high-OS chemistry of Am and fulfill the crucial task of Ln/Am separation in the nuclear fuel cycle. The synergistic coordination and oxidation process is found to occur in the organic solvent, and the mechanism has been well elucidated by quantum-theoretical modeling.

中文翻译：

通过氧化态控制实现超高效镅/镧系元素分离

镧系元素/锕系元素分离是原子能和核废料处理的世界性挑战。将镅 (Am)（核燃料循环中的关键锕系元素）与镧系元素 (Ln) 分离对于最大限度地降低核废料的长期放射性毒性是非常可取的，但鉴于三价 Am(III) 之间的化学相似性，这是极具挑战性的) 和 Ln(III)。将 Am(III) 选择性氧化为更高的氧化态 (OS) 可以促进这种分离，但到目前为止，由于 Am 在高 OS 中的不稳定性质，它的实际应用还远远不能令人满意。在此，我们找到了一种新的策略，通过 Am(III) 与二甘醇酰胺配体的配位以及在有机溶剂存在下与 Bi(V) 物质的氧化来生成稳定的五价 Am (Am(V))。⁴）通过溶剂萃取中的一次接触将Am从Ln中分离出来，从而为研究Am的高OS化学和完成核燃料循环中Ln/Am分离的关键任务开辟了一条新途径。发现协同配位和氧化过程发生在有机溶剂中，其机理已通过量子理论模型得到很好的阐明。

更新日期：2022-03-30

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南