Distribution of plutonium, americium and interfering fission products between nitric acid and a mixed organic phase of TODGA and DMDOHEMA in kerosene, and implications for the design of the "EURO-GANEX" process
Distribution of plutonium, americium and interfering fission products between nitric acid and a mixed organic phase of TODGA and DMDOHEMA in kerosene, and implications for the design of the "EURO-GANEX" process
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DOI：
10.1016/j.hydromet.2014.12.019
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发表时间：
2015-02-01
期刊：
影响因子：
4.7
通讯作者：
Taylor, Robin
中科院分区：
文献类型：
--
作者：
Carrott, Michael;Geist, Andreas;Taylor, Robin
为了从乏核燃料中均匀回收锕系元素，在基于向快中子反应堆过渡的未来核燃料循环中，正在开发一种新的GANEX（分组锕系元素提取）工艺。这潜在地提供了一种用于回收锕系元素的更简单、更抗扩散的湿法冶金方法。所谓的EURO-GANEX方法是基于液-液萃取到有机相中，该有机相包含在无味煤油稀释剂中的0.2mol/L TODGA和0.5mol/L DMODHEMA。在用溶解的快堆乏燃料测试EURO-GANEX工艺之前，需要关于在典型的提取和洗涤条件下可能有问题的裂变产物（Fe、Sr、Zr、Mo、Tc、Ru、Pd）的分布比率的数据。此外，必须确定在存在提取的镧系元素的情况下选择性反洗超铀锕系元素（特别是钚和镅）的合适条件。获得的分配比数据表明，可以确定防止铁和锶穿透的条件，同时保持通过提取-洗涤接触器提取锕系元素，尽管可能会发生一些积累。聚羧酸类配体CDTA能有效地抑制锆、钯的萃取。然而，由于高分配比和CDTA无显著抑制，锝和钼可能在第一接触器中可浸提。钌可以部分提取，但在硝酸中的行为是复杂的。还表明，对于钚浓度范围为1000 μ g/L，通过用磺化双三嗪基吡啶（BTP）配体和乙酰异羟肟酸（AHA）的组合进行反萃取，可以有效地将钚和镅与镧系元素分离。
For the homogeneous recycling of actinides from spent nuclear fuels, within the future nuclear fuel cycle based on a transition to fast neutron reactors, a new GANEX (Grouped Actinide Extraction) process is under development. This potentially provides a simpler, more proliferation resistant hydrometallurgical process for recycling actinides. The so-called EURO-GANEX process is based on liquid-liquid extraction into an organic phase comprising 0.2 mol/L TODGA and 0.5 mol/L DMODHEMA in an odourless kerosene diluent. Before testing the EURO-GANEX process with dissolved fast reactor spent fuel, data are required on the distribution ratios of likely problematic fission products (Fe, Sr, Zr, Mo, Tc, Ru, Pd) under typical extraction and scrubbing conditions. Also, suitable conditions must be defined for the selective backwashing of the transuranic actinides (specifically plutonium and americium) in the presence of extracted lanthanide elements.Distribution ratio data obtained indicate that conditions can be defined that prevent iron and strontium break through whilst maintaining actinide extraction across the extract-scrub contactors although some accumulation may occur. Zirconium and palladium extraction can be effectively inhibited by a polycarboxylate ligand: CDTA. However, technetium and molybdenum are likely to be extractable in the first contactor due to high distribution ratios and no significant suppression with CDTA. Ruthenium may be partially extracted but behaviour is complex in nitric acid. It was also shown that plutonium and americium can be efficiently separated from lanthanides by stripping with a combination of a sulphonated bis-triazinyl pyridine (BTP) ligand and acetohydroxamic acid (AHA) for plutonium concentrations ranging from