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通过物种特异性同位素稀释气相色谱-电感耦合等离子体质谱法测定硫柳汞给药后小鼠组织中的甲基汞、乙基汞和无机汞。

Determination of methylmercury, ethylmercury, and inorganic mercury in mouse tissues, following administration of thimerosal, by species-specific isotope dilution GC-inductively coupled plasma-MS.

作者信息

Qvarnström Johanna, Lambertsson Lars, Havarinasab Said, Hultman Per, Frech Wolfgang

机构信息

Analytical Chemistry, Department of Chemistry, Umeå University, S-901 87 Umeå, Sweden.

出版信息

Anal Chem. 2003 Aug 15;75(16):4120-4. doi: 10.1021/ac0342370.

Abstract

Isotopically enriched HgO standards were used to synthesize CH3(200)Hg+ and C2H5(199)Hg+ using Grignard reagents. These species were employed for isotope dilution GC-ICPMS to study uptake and biotransformation of ethylmercury in mice treated with thimerosal, (sodium ethylmercurithiosalicylate) 10 mg L(-1) in drinking water ad libitum for 1, 2.5, 6, or 14 days. Prior to analysis, samples were spiked with aqueous solutions of CH3(200)Hg+, C2H5(199)Hg+, and 201Hg2+ and then digested in 20% tetramethylammonium hydroxide and extracted at pH 9 with DDTC/toluene. Extracted mercury species were reacted with butylmagnesium chloride to form butylated derivatives. Absolute detection limits for CH3Hg+, C2H5Hg+, and Hg2+ were 0.4, 0.2, and 0.6 pg on the basis of 3sigma of five separate blanks. Up to 9% of the C2H5Hg+ was decomposed to Hg2+ during sample preparation, and it is therefore crucial to use a species-specific internal standard when determining ethylmercury. No demethylation, methylation, or ethylation during sample preparation was detected. The ethylmercury component of thimerosal was rapidly taken up in the organs of the mice (kidney, liver, and mesenterial lymph nodes), and concentrations of C2H5Hg+ as well as Hg2+ increased over the 14 days of thimerosal treatment. This shows that C2H5Hg+ in mice to a large degree is degraded to Hg2+. Increased concentrations of CH3Hg+ were also observed, which was found to be due to impurities in the thimerosal.

摘要

使用同位素富集的HgO标准品,通过格氏试剂合成CH3(200)Hg+和C2H5(199)Hg+。这些物质用于同位素稀释气相色谱 - 电感耦合等离子体质谱法,以研究硫柳汞(乙基汞硫代水杨酸钠,10 mg L(-1),自由饮水)处理1、2.5、6或14天的小鼠中乙基汞的摄取和生物转化。分析前,向样品中加入CH3(200)Hg+、C2H5(199)Hg+和201Hg2+的水溶液,然后在20%的四甲基氢氧化铵中消化,并在pH 9下用二乙基二硫代氨基甲酸钠/甲苯萃取。萃取的汞物种与丁基氯化镁反应形成丁基化衍生物。基于五个单独空白的3σ,CH3Hg+、C2H5Hg+和Hg2+的绝对检测限分别为0.4、0.2和0.6 pg。在样品制备过程中,高达9%的C2H5Hg+分解为Hg2+,因此在测定乙基汞时使用物种特异性内标至关重要。在样品制备过程中未检测到脱甲基、甲基化或乙基化。硫柳汞中的乙基汞成分在小鼠的器官(肾脏、肝脏和肠系膜淋巴结)中迅速被摄取,在硫柳汞处理的14天内,C2H5Hg+以及Hg2+的浓度增加。这表明小鼠体内的C2H5Hg+在很大程度上降解为Hg2+。还观察到CH3Hg+浓度增加,发现这是由于硫柳汞中的杂质所致。

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