超临界水氧化处理放射性废TBP/煤油技术研究

Study on Radioactive TBP/kerosene Treatment by Super Critical Water Oxidation

  • 摘要: 针对乏燃料后处理常用的有机溶剂TBP/煤油,采用以质量分数为30%的双氧水为氧化剂的超临界水氧化(SCWO)处理装置进行了模拟实验。结果显示,反应温度(550±50) ℃、停留时间(9±1) min、氧化剂与有机物流量比16.5±0.5条件下,有机物无机化率可达到99.9%以上。在此基础上开展了SCWO处理工艺放射性实验研究。结果表明,在气相产物中,放射性低于检测下限;在液相产物中,α活度浓度为2.37×103 Bq/L,β活度浓度为8.94×102 Bq/L,γ活度浓度为96 Bq/L;在固相产物中,α比活度为2 750.2 Bq/g,β比活度为5 863.3 Bq/g,γ比活度为5 840.2 Bq/g,根据放射性活度衡算,放射性核素大部分进入固体残渣中。SEM/EDS表征结果表明,反应过程产生的固体产物中,主要以U元素为主,产物中主要含U、Ni、Cr、Fe、Al的磷酸盐及氧化物。

     

    Abstract: A supercritical water oxidation (SCWO) treatment device, with 30% hydrogen peroxide as oxidant, was used to dispose TBP/kerosene in reprocessing, and the simulation experiments were carried out. The results show that under the condition of reaction temperature (550±50) ℃, residence time (9±1) min and the ratio of oxidant to organic flow 16.5±0.5, the inorganic rate of organic waste can reach over 99.9%. On this basis, the experimental study of radioactivity was carried out. The results show that no radioactivity is detected in the gas-phase products and the α, β and γ activity concentrations in liquid are 2.37×103, 8.94×102 and 96 Bq/L respectively, and specific activities in solid products are 2 750.2, 5 863.3 and 5 840.2 Bq/g respectively. The radionuclide is concentrated in the solid products. SEM/EDS analysis shows that the main component of the solid products is U, other components are phosphates and oxides composed of U, Ni, Cr, Fe and Al.

     

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