超声与微混合联用对过氧化铀连续沉淀增强作用研究

Study on Enhancing Effect of Ultrasonic Combined with Micro-mixing on Continuous Precipitation of Uranium Peroxide

  • 摘要: 为改进传统釜式沉淀方式,强化过氧化铀(UO4·4H2O)沉淀过程,本文将超声场与微通道技术耦合,利用管式沉淀装置和微混合装置研究了超声作用联合微通道技术对过氧化铀沉淀转化和杂质净化的影响。结果表明,超声强化技术与微混合技术共同作用于过氧化铀沉淀过程可加速沉淀反应,显著提高沉淀率,且无需陈化,可实现均一、规整、较大粒径过氧化铀沉淀的连续制备,同时实现沉淀过程杂质净化能力的极大提升。在60%超声功率下,微通道-超声耦合技术制备的过氧化铀晶体粒径主要分布在16 μm和22 μm附近,粒径均一,相较于无超声情况,两特征粒径占比分别提升了7.8倍和2.2倍。在298.14 g/h的通量条件下,微通道-超声耦合技术对过氧化铀中Fe、Cr、Ni、Cu、Al的净化系数分别为传统釜式沉淀过程的130.8、9.13、9.39、136.5、11.39倍。微通道-超声耦合技术可实现过氧化铀晶体连续化、高纯度制备,适用于核燃料规模化生产及核废料铀资源回收纯化。

     

    Abstract: In the uranium chemical process, the hydrogen peroxide precipitation method can be used for the purification of uranyl nitrate. The research on the overoxidized uranium crystallization process based on the batch-stirred reactor is relatively in-depth. However, due to the batch precipitation process being batchwise precipitation and using mechanical stirring for mixing, there are problems such as lack of process continuity, dependence on equipment volume, average mass transfer effect, large retention volume, and multiple moving components. To improve the traditional batch precipitation method and strengthen the overoxidized uranium precipitation process, the ultrasonic field and microchannel technology were coupled to study the influence of the combined effect of ultrasonic action and microchannel technology on the precipitation conversion and impurity purification of overoxidized uranium. Firstly, the influence of the coupling of ultrasonic and microchannel technology on the precipitation rate and the crystal size distribution of the precipitate was studied. Then, the influence of the coupling of ultrasonic and microchannel technology on impurity purification was investigated. Finally, the influence of the combined use of ultrasonic and microchannel technology on continuous impurity purification in the precipitation process was verified through a large-flux precipitation test. The results show that the combined action of ultrasonic strengthening technology and micro-mixing technology significantly improves the growth rate of precipitation crystals, thereby accelerating the formation rate of precipitation and significantly increasing the precipitation rate, without aging, ensuring the size of the crystal, achieving uniform, regular, and having a large particle size of overoxidized uranium precipitate crystals, and simultaneously achieving a significant improvement in the impurity purification ability of the precipitation process. Only under the microchannel reaction conditions, the amounts of the five impurities (Al, Fe, Ni, Cu, Cr) in the product UO4·4H2O decrease from 9178 μg/gU to below 4.89 μg/gU. This indicates that the continuous homogeneous mixing of the micro-mixing process reduces the entrainment of impurities and improves the impurity purification rate. For Zr4+, which has a larger ionic potential, the ultrasonic action accelerates the crystal growth rate, controls the particle size and distribution of the precipitation crystals, reduces the encapsulation of Zr, and the two technologies are combined to achieve a significant improvement in the impurity purification ability of the precipitation process. Under the optimal conditions of the test device with a flux of 298.14 g/h, the total amount of six impurities in the UO4·4H2O crystals is less than 136 μg/gU (while the original solution contains 9178 μg/gU). The purification coefficients of Fe, Cr, Ni, Zr, Cu, and Al are 969, 1528, 1427, 9, 1237, and 131 respectively, far exceeding the average impurity purification efficiency of the original batch precipitation process.

     

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