硫化铋修饰沸石对高温氩气环境中碘的净化研究

Purification of Iodine from High-temperature Argon Environment by Bismuth Sulfide-modified Zeolite

  • 摘要: 乏燃料后处理过程中产生的放射性气体中含有129I,因其半衰期长、含量高且毒性大而备受关注。现阶段对干法后处理中129I高温氩气环境条件下的研究很少,为探究固体多孔吸附剂在干法高温氩气环境中对放射性碘的吸附性能,本文以Bi(NO3)3·5H2O为铋源、L-半胱氨酸为硫源、乙二醇为溶剂,采用水热法制备硫化铋修饰沸石复合材料(Bi2S3-MOR),并采用该复合材料进行静态吸附实验。结果表明:在130 ℃氩气环境中,硫化铋修饰沸石对单质碘的静态吸附容量可达180 mg/g,捕集形式既有化学吸附的BiI3,又有物理吸附的I2,而在50 ℃氩气环境中,对甲基碘的静态吸附容量为50 mg/g,仅存在BiI3形式的化学吸附。水热法Bi2S3修饰沸石表现出同Ag0修饰沸石一样优异的碘吸附性能。

     

    Abstract: Nowadays, fast breeder reactor (FBR) is one of the preferred reactor types for Generation Ⅳ advanced nuclear energy systems in the world. FBRs can improve the utilization rate of uranium resources, make the long-lived spent fuel generation much lower, and achieve the minimization of radioactive waste. The characteristics of high burnup, high irradiation, and high plutonium content of fast reactor spent fuel make it difficult for the traditional aqueous reprocessing process to meet the separation needs. Compared with the traditional liquid separation technology, dry technology has potential advantages and dry reprocessing is mainly under high temperature argon environment, for the treatment of radioactive gases in the spent fuel reprocessing process, as the 129I containing exhaust gas has attracted much attention due to its long half-life, high content and high toxicity. In this paper, Bi(NO3)3·5H2O was used as the source of bismuth, L-cysteine as the source of sulfur, and ethylene glycol as the solvent, two-step hydrothermal method was used to prepare bismuth sulfide modified zeolite composites (Bi2S3-MOR). The static adsorption experiments were carried out in a reactor with a valve, where the composites were first placed in a polytetrafluoroethylene liner together with iodine (methyl iodide), and the experiments were kept in an argon environment by closing the valve after 20 min of argon gas was passed through the valve. The physical phase of the composites was analyzed by XRD, the specific surface area and pore size by BET, the structure of functional groups by FT-IR, the morphology of the materials before and after modification and the distribution of the elements by SEM and EDS, the loading after modification by ICP-OES, and the content of C and H in the composites by elemental analyzer, and the valence change of the composites before and after the adsorption as well as the strength of the binding energy were analyzed by XPS, the thermal stability of the composites was analyzed by TGA. The experimental results show that the static adsorption capacity of bismuth sulfide modified zeolite for monosubstituted iodine is up to 180 mg/g at 130 ℃ under argon environment, and the trapping forms are both chemisorbed BiI3 and physisorbed I2, while the static adsorption capacity for CH3I is 50 mg/g at 50 ℃ under argon environment, and only the chemical adsorption in the form of BiI3 exists. The research results can provide new ideas and options for the purification and treatment of gaseous radioactive iodine in the dry reprocessing process.

     

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