Choi Man Sik, Lee Dong-Soo, Choi Jae-Cheon, Cha Hyun-Ju, Yi Hee-Il
Division of Earth and Environmental Sciences, Chungnam National University, 220 Gungdong, Yuseongku, Daejeon, 305-764, Korea.
Sci Total Environ. 2006 Oct 15;370(1):262-70. doi: 10.1016/j.scitotenv.2006.07.036. Epub 2006 Sep 7.
Concentration and isotope ratio of Pu were analyzed for aerosols collected at Anmyeondo located in the western coast of Korea using multiple collector inductively coupled plasma mass spectrometer equipped with desolvated micro-concentric nebulizer. Aerosols were collected from June 2001 to April 2002 using high volume air sampler. The samples consist of high dust samples (Yellow Sand), and also low dust samples; maximum Al concentration was 74.2 microg/m(3) and minimum was 0.17 microg/m(3). Pu was concentrated using 0.1 ml TEVA resin columns after conc. HNO(3) extraction. Isotope dilution using (242)Pu spike and mass bias correction using (233)U and (236)U mixed solution enabled the quantification of Pu and measurement of isotope ratio simultaneously. The contribution of (238)U from both spikes and samples was minimized by careful chemical separation and optimization of spike concentration. The (238)U(1)H and tail contribution on (239)Pu peak were about 0.75 x 10(-5) and 1 x 10(-5) of (238)U intensity, respectively, and they were corrected from (239)Pu using externally determined ((238)U(1)H + tailing)/(238)U ratio and (238)U measurement during acquisition. The detection limits of this analytical procedure were 0.61 fg/ml and 0.56 fg/ml for (239)Pu and (240)Pu, respectively (4 nBq/m(3) and 12 nBq/m(3) for (239)Pu and (240)Pu, respectively). The precision of isotope ratio measurement was better than 2% for larger quantity than 20 fg of (239)Pu. In spring, maximum concentration of 0.580 microBq/m(3) for (239)Pu and 0.404 microBq/m(3) for (240)Pu was observed when Al concentration was maximum, so called as Yellow Sand event. Pu concentrations in aerosols are well correlated with Al, a tracer of soil dust. The ratios of Pu/Al were 0.0082 (microBq/microg) and 0.0055 (microBq/microg) for (239)Pu/Al and (240)Pu/Al, respectively. Isotope ratios of Pu ((240)Pu/(239)Pu) in Yellow Sand samples show 0.191+/-0.014 close to those of global fallout. These facts indicate that Yellow Sand plays an important role in the behavior of Pu in the environment like other concomitant metals such as Al, Fe etc.
使用配备去溶剂化微同心雾化器的多接收电感耦合等离子体质谱仪,对在韩国西海岸安眠岛采集的气溶胶中的钚浓度和同位素比率进行了分析。2001年6月至2002年4月期间,使用大容量空气采样器收集气溶胶。样本包括高沙尘样本(黄沙)以及低沙尘样本;铝的最大浓度为74.2微克/立方米,最小浓度为0.17微克/立方米。经浓硝酸萃取后,使用0.1毫升TEVA树脂柱对钚进行浓缩。使用242Pu尖峰进行同位素稀释,并使用233U和236U混合溶液进行质量偏倚校正,从而能够同时对钚进行定量分析并测量同位素比率。通过仔细的化学分离和优化尖峰浓度,使来自尖峰和样本的238U的贡献降至最低。238U1H和239Pu峰上的拖尾贡献分别约为238U强度的0.75×10−5和1×10−5,并在采集过程中使用外部测定的(238U1H + 拖尾)/238U比率和238U测量值从239Pu中进行校正。该分析程序对239Pu和240Pu的检测限分别为0.61飞克/毫升和0.56飞克/毫升(239Pu和240Pu分别为4纳贝克勒尔/立方米和12纳贝克勒尔/立方米)。对于数量大于20飞克的239Pu,同位素比率测量的精度优于2%。在春季,当铝浓度达到最大值(即所谓的黄沙事件)时,观测到239Pu的最大浓度为0.580微贝克勒尔/立方米,240Pu的最大浓度为0.404微贝克勒尔/立方米。气溶胶中的钚浓度与作为土壤尘埃示踪剂的铝密切相关。239Pu/Al和240Pu/Al的比率分别为0.0082(微贝克勒尔/微克)和0.0055(微贝克勒尔/微克)。黄沙样本中钚的同位素比率(240Pu/(239)Pu)显示为0.191±0.014,接近全球沉降物的比率。这些事实表明,黄沙与铝、铁等其他伴随金属一样,在环境中钚的行为中起着重要作用。