基于半导体制冷的活性炭冷阱设计

Design of Activated Charcoal Trap Based on Semiconductor Refrigeration

  • 摘要: Xe气体浓度和同位素比值的分析测试在核工业、核保障监督、前沿科学等领域具有重要意义,但Xe在空气中的含量极低,特别是在大气颗粒物和大气放射性氙样品中,极微量Xe的高效捕集成为非常大的难点和挑战。本文基于半导体制冷技术设计了一种紧凑型活性炭冷阱装置,并通过降低冷阱温度吸附混合气体中的Xe,再升温至180 ℃释放Xe,纯化后利用Helix MC Plus静态气体质谱仪测量Xe的浓度和同位素比值。实验结果显示:利用活性炭冷阱吸附分离的方法,最低温度可达−37 ℃,制冷时间只需180 s,Xe的回收率达到81%,Kr、Xe分离系数为188。在进样量约1×10−13 mol条件下,除124Xe/132Xe、126Xe/132Xe和128Xe/132Xe外,利用法拉第筒测量Xe同位素比值的精密度为0.06%~0.12%,与参考值的相对偏差为−0.14%~0.22%,其中129Xe/132Xe、130Xe/132Xe和134Xe/132Xe测量值与参考值的相对偏差为−0.03%~0.07%。结果表明,紧凑型活性炭冷阱装置制冷迅速且稳定,样品处理流程耗时约0.5 h,联合静态气体质谱可实现高精度Xe同位素比值分析,可为核保障监督和核环境监测中大气颗粒物和大气放射性氙的监测提供技术支撑。

     

    Abstract: Xenon (Xe) concentration and isotope ratios measurements are crucial in the nuclear industry, nuclear safeguards supervision, frontier science and other fields. However, due to its minimal presence in atmospheric composition, especially in atmospheric particulate matter and atmospheric radioactive xenon samples, efficient separation of minuscule xenon presents a significant challenge. One of the most commonly used methods is to separate xenon gases by using the principle of adsorption temperature difference between noble gases on activated charcoal. Activated charcoal can selectively adsorb Xe at low temperatures, making it an efficient adsorbent. Thermoelectric refrigeration technology based on semiconductors has the advantages of low noise, run steadily, low material consumption, and long service life, and is widely used in spaceflight, medical care, and biopharmaceutical industries. A compact activated charcoal trap based on technology of semiconductor refrigeration was designed. The activated charcoal trap device is mainly composed of four parts: adsorption module, heat conduction module, refrigeration module and heat dissipation module. In order to improve the cooling effect of activated charcoal particles, the elasticity of copper mesh was used to support activated charcoal particles on the stainless steel pipe wall. Xe in the mixed gas was adsorbed by reducing the temperature of the trap, subsequently released by heating to 180 ℃. After purification, the concentration and isotope ratio of Xe were measured by Helix MC Plus static gas mass spectrometer. Experimental results demonstrate that the lowest achieved temperature of activated charcoal trap is −37 ℃ with a refrigeration time of just 180 seconds. The recovery of Xe reaches 81% and the separation coefficient of Kr from Xe is above 188. For a sample injection of approximately 1×10−13 mol, the relative standard deviation (RSD) of Xe isotope ratio analysis is 0.06%-0.12% by Faraday tube, and the relative deviation between the measured value and certified value is −0.14%-0.22%, excluding 124Xe/132Xe, 126Xe/132Xe, and 128Xe/132Xe. Among them, the relative deviation between the measured value and the reference value of 129Xe/132Xe, 130Xe/132Xe and 134Xe/132Xe is −0.03%-0.07%. The measured results are stable and accurate, the reproducibility of the test process is good, and no obvious isotopic fractionation is observed during sample processing and measurement. The compact activated charcoal trap designed in this paper can be cooled swiftly and stably, with a processing time of sample preparation about 0.5 hours. Combined with static gas mass spectrometry, it enables high precision analysis of Xe isotope ratios, offering technical support for the monitoring of atmospheric particulate matter and atmospheric radioactive xenon gases in nuclear safeguards and nuclear environmental monitoring.

     

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