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中放α泥浆中总Pu分析方法研究

Analytical method study of Pu in intermediate-level radioactive α-nuclide slurry

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中放α泥浆是中放废液长期贮存过程中沉积于贮罐底部的放射性泥浆,高放射性泥浆严重制约老罐区的退役进程,亟需处理处置,但目前国内没有工程化应用的处理处置方式.为后续大规模工业处理和处置,某厂拟定中放α泥浆酸溶去超铀核素的技术路线,而中放α泥浆酸溶样品中总Pu分析作为重要数据之一.中放α泥浆组分复杂,盐份高.目前还没有针对中放α泥浆中总Pu的分析标准和成熟分析方法.本研究基于中放α泥浆处理与处置研究中的酸溶液样品,并根据Pu4+阳离子与有机物的络合性能进行泥浆酸溶样品中Pu的分离、纯化后,采用液闪计数器测量进行研究.使用TiOA-二甲苯有机体系萃取酸溶液体样品中的Pu,采用液闪测量酸溶样品中Pu活度浓度,最终形成成熟、可靠的中放α泥浆酸溶样品中总Pu的分析方法.研究结果表明,TiOA-二甲苯对Pu有很强萃取能力,对U萃取性能很差,不能萃取Am;萃取中样品酸度对萃取效能微弱影响,萃取的理想酸度为4.0 mol·L-1左右,Pu萃取回收率达99.23%;Pu的阳离子在水溶液中Pu4+最为稳定;Fe2+的还原性能将Pu的高价态调整至四价态;NaNO2的氧化性将Pu(Ⅲ)氧化成Pu(Ⅳ).样品中Pu分离、纯化后采用液闪计数器测量,准确性高、稳定性好.该方法为中放α泥浆处理中准确快速分析建立基础条件.
The α nuclide slurry is the radioactive slurry deposited at the bottom of the storage tank during the long-term storage of the waste liquid in the reprocessing process of uranium-plutonium fuel cycle.The α nuclide slurry seriously restricts the decommissioning process of the old tank farm which urgently needs to be treated and disposed of but there is no treatment and disposal method for engineering application in China at present.For the follow-up large-scale industrial treatment and disposal,a plant has formulated a technical route for the acid dissolution of transuranic nuclides in α nuclide slurry,and the analysis of total Pu in the acid-soluble samples of the α nuclide slurry is one of the important data.Due to the complex chemical composition and high salt content of the α nuclide slurry,there is no standard and mature analytical method for the total Pu in the α nuclide slurry.In this study,the acid solution samples in the treatment and disposal of the α nuclide slurry were studied,the separation,purification and liquid scintillation measurement of Pu in the mud acid-soluble samples were studied according to the complexing properties of Pu4+cations and organic matter,the Pu in the acid solution samples was extracted by TiOA-xylene organic system,and the Pu activity concentration in the acid-soluble samples was measured by liquid scintillation,finally a mature and reliable method for the analysis of total Pu in the acid-soluble samples of the α mud was formed.The results showed that TiOA-xylene had strong extraction ability for Pu,but poor extraction performance for U,and could not extract Am.The acidity of the sample had limited effect on the extraction efficiency,and the ideal acidity of the extraction was about 4.0 mol·L-1,and the recovery rate of Pu extraction was 99.23%.The cation of Pu was the most stable in aqueous solution with Pu4+.The reduction performance of Fe2+adjusted the high valence state of Pu to the tetravalent state.The oxidation of NaNO2 oxidized Pu(III)to Pu(IV).After the separation and purification of Pu in the sample,the liquid scintillation counter was used to measure it,which was of high accuracy and good stability.Therefore,the basic conditions of this method has been established for accurate and rapid analysis in the treatment of intermediate α nuclide slurry.

intermediate-level radioactive α-nuclide slurrytotal Pudistribution ratioextraction

张明东、李小平、阳帆、张玉清、谢伟婷、冯润松

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中核四川环保工程有限责任公司,四川 广元 628000

中放α泥浆 分配比 调价 萃取

中核集团青年英才项目

[2023]384号

2024

世界核地质科学
核工业北京地质研究院

世界核地质科学

CSTPCD
影响因子:0.463
ISSN:1672-0636
年,卷(期):2024.41(5)