多接收电感耦合等离子体质谱法精确测量铀中痕量钚同位素方法研究

Studies on the Precise Measurement of Isotope of Trace Plutonium in Uranium by MC-ICP-MS

经过核燃料后处理得到的铀产品中含有极微量钚杂质,对其同位素组成进行分析有利于对应铀材料的溯源。本工作在铀钚化学分离的基础上,对影响MC-ICP-MS法精确测量痕量钚同位素丰度比值的仪器条件进行了优化,研究了仪器分辨率、离子提取模式的选择、"背景和干扰"等参数的影响,探索研究了MC-ICP-MS上质量偏倚的校正方法。对选择的两个后处理铀产品中痕量钚同位素比进行了测量,当铀钚比例达1010时,测得的239Pu/240Pu相对不确定度优于5%。并且建立了在MC-ICP-MS上测量ng.L-1量级钚同位素丰度比值的方法。

The infinitesimal plutonium impurity was contained in the uranium product obtained by reproeessing. The precise measurement of the isotope ratio of plutonium was beneficial to the identification of the corresponding source of uranium product. Basing on the separation of trace plutonium from uranium matrix, the operating parameters of MC-ICP-MS were studied and optimized for determining the isotope ratio of trace plutonium, such as the adjustment of resolution, selection of mode of ion extraction, elimination of background and interference, etc. The correction method of the mass discrimination was explored for MCICP-MS measuring isotope ratio. The isotope ratio of 239pu/240 Pu in two selected uranium products obtained by reprocessing, which was measured and corrected by measuring plutonium reference material. The ratio of uranium and plutonium is more than 10^10, and the sum of relative uncertainty for plutonium measurement is better than 5%. The measuring method of isotope ratiois establishes for ng ·L^-1 level of plutonium.