使用高碘酸铜（III）回收六价A,Inorganic Chemistry

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使用高碘酸铜（III）回收六价A
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2016-10-31 00:00:00 , DOI: 10.1021/acs.inorgchem.6b02120
Kevin McCann ₁ , Derek M. Brigham ₂ , Samuel Morrison ₃ , Jenifer C. Braley ₁

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从镧系元素中分离a被认为是关闭核燃料循环中最困难的分离步骤之一。这种分离的一种方法可能涉及将a氧化为六价态以形成线性二氧阳离子，而镧系元素则保留为三价离子。这项工作认为在硝酸溶解摩尔条件下，水溶性的Cu ³⁺高碘酸盐作为氧化剂可将正十二烷中的六价Am与戊基戊酸二戊酯（DAAP）分离。初步研究评估了酸性介质中Cu ³⁺高碘酸盐自动还原的动力学，以帮助开发溶剂萃取系统。表征Cu ³⁺高碘酸盐氧化剂，溶剂萃取研究优化了从各种硝酸介质中以及在存在其他裂变产物或裂变产物替代物物种下的Am的回收率。短的水/有机接触时间促进了在没有氧化还原活性裂变产物的情况下从硝酸介质中成功回收Am（分布值高达2）。在-后铀氧化还原萃取（后PUREX）模拟水质进料的存在下，发生了四价物种（Ce，Ru，Zr）的沉淀，并且抑制了²⁴¹ Am的分布值，表明Cu ^3的某些氧化能力⁺高碘酸盐被模拟物中的其他氧化还原活性金属大量消耗。手稿显示了Cu ³⁺ 高碘酸盐作为Am氧化和回收的潜在可行氧化剂，并指出在寻求将Am氧化以进行与核燃料循环相关的分离的任何方法中，都需要解决在存在PUREX模拟饲料后观察到的氧化能力的消耗问题。

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Hexavalent Americium Recovery Using Copper(III) Periodate

Separation of americium from the lanthanides is considered one of the most difficult separation steps in closing the nuclear fuel cycle. One approach to this separation could involve oxidizing americium to the hexavalent state to form a linear dioxo cation while the lanthanides remain as trivalent ions. This work considers aqueous soluble Cu³⁺ periodate as an oxidant under molar nitric acid conditions to separate hexavalent Am with diamyl amylphosphonate (DAAP) in n-dodecane. Initial studies assessed the kinetics of Cu³⁺ periodate autoreduction in acidic media to aid in development of the solvent extraction system. Following characterization of the Cu³⁺ periodate oxidant, solvent extraction studies optimized the recovery of Am from varied nitric acid media and in the presence of other fission product, or fission product surrogate, species. Short aqueous/organic contact times encouraged successful recovery of Am (distribution values as high as 2) from nitric acid media in the absence of redox active fission products. In the presence of a post-plutonium uranium redox extraction (post-PUREX) simulant aqueous feed, precipitation of tetravalent species (Ce, Ru, Zr) occurred and the distribution values of ²⁴¹Am were suppressed, suggesting some oxidizing capacity of the Cu³⁺ periodate is significantly consumed by other redox active metals in the simulant. The manuscript demonstrates Cu³⁺ periodate as a potentially viable oxidant for Am oxidation and recovery and notes the consumption of oxidizing capacity observed in the presence of the post-PUREX simulant feed will need to be addressed for any approach seeking to oxidize Am for separations relevant to the nuclear fuel cycle.

更新日期：2016-10-31

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