Li Yan, Yu Hua, Zheng Siqian, Miao Yang, Yin Shi, Li Peng, Bian Ying
State Key Laboratory of Quality Research in Chinese Medicine, Institute of Chinese Medical Sciences, University of Macau, Av. Padre Tomás Pereira Taipa, Macau 999078, China.
Shanghai Institute of Occupational Safety and Health (SIOSH), 369 North Chengdu Road, Shanghai 200041, China.
Int J Environ Res Public Health. 2016 Mar 22;13(3):350. doi: 10.3390/ijerph13030350.
Rare earth elements (REEs) have undergone a steady spread in several industrial, agriculture and medical applications. With the aim of exploring a sensitive and reliable indicator of estimating exposure level to REEs, a simple, accurate and specific ICP-MS method for simultaneous direct quantification of 15 REEs ((89)Y, (139)La, (140)Ce, (141)Pr, (146)Nd, (147)Sm, (153)Eu, (157)Gd, (159)Tb, (163)Dy, (165)Ho, (166)Er, (169)Tm, (172)Yb and (175)Lu) in human urine has been developed and validated. The method showed good linearity for all REEs in human urine in the concentrations ranging from 0.001-1.000 μg ∙ L(-1) with r² > 0.997. The limits of detection and quantification for this method were in the range of 0.009-0.010 μg ∙ L(-1) and 0.029-0.037 μg ∙ L(-1), the recoveries on spiked samples of the 15 REEs ranged from 93.3% to 103.0% and the relative percentage differences were less than 6.2% in duplicate samples, and the intra- and inter-day variations of the analysis were less than 1.28% and less than 0.85% for all REEs, respectively. The developed method was successfully applied to the determination of 15 REEs in 31 urine samples obtained from the control subjects and the workers engaged in work with manufacturing of ultrafine and nanoparticles containing cerium and lanthanum oxide. The results suggested that only the urinary levels of La (1.234 ± 0.626 μg ∙ L(-1)), Ce (1.492 ± 0.995 μg ∙ L(-1)), Nd (0.014 ± 0.009 μg ∙ L(-1)) and Gd (0.023 ± 0.010 μg ∙ L(-1)) among the exposed workers were significantly higher (p < 0.05) than the levels measured in the control subjects. From these, La and Ce were the primary components, and accounted for 88% of the total REEs. Lanthanum comprised 27% of the total REEs while Ce made up the majority of REE content at 61%. The remaining elements only made up 1% each, with the exception of Dy which was not detected. Comparison with the previously published data, the levels of urinary La and Ce in workers and the control subjects show a higher trend than previous reports.
稀土元素（REEs）已在多个工业、农业和医学应用领域中稳步推广。为了探索一种灵敏且可靠的评估REEs暴露水平的指标，已开发并验证了一种简单、准确且特异的电感耦合等离子体质谱（ICP-MS）方法，用于同时直接定量测定人尿中的15种稀土元素（（89）Y、（139）La、（140）Ce、（141）Pr、（146）Nd、（147）Sm、（153）Eu、（157）Gd、（159）Tb、（163）Dy、（165）Ho、（166）Er、（169）Tm、（172）Yb和（175）Lu）。该方法在0.001 - 1.000 μg ∙ L⁻¹浓度范围内对人尿中所有稀土元素均显示出良好的线性，r² > 0.997。此方法的检测限和定量限分别在0.009 - 0.010 μg ∙ L⁻¹和0.029 - 0.037 μg ∙ L⁻¹范围内，15种稀土元素加标样品的回收率在93.3%至103.0%之间，重复样品中的相对百分比差异小于6.2%，所有稀土元素分析的日内和日间变化分别小于1.28%和小于0.85%。所开发的方法成功应用于测定从对照组受试者以及从事含铈和氧化镧的超细和纳米颗粒制造工作的工人中获取的31份尿样中的15种稀土元素。结果表明，仅暴露工人尿中La（1.234 ± 0.626 μg ∙ L⁻¹）、Ce（1.492 ± 0.995 μg ∙ L⁻¹）、Nd（0.014 ± 0.009 μg ∙ L⁻¹）和Gd（0.023 ± 0.010 μg ∙ L⁻¹）的水平显著高于（p < 0.05）对照组受试者中测得的水平。由此可知，La和Ce是主要成分，占总稀土元素的88%。镧占总稀土元素的27%，而Ce占稀土元素含量的大部分，为61%。其余元素各自仅占1%，未检测到Dy除外。与先前发表的数据相比，工人和对照组受试者尿中La和Ce的水平显示出比先前报告更高的趋势。
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