Shanaiah Narasimhamurthy, Desilva M Aruni, Nagana Gowda G A, Raftery Michael A, Hainline Bryan E, Raftery Daniel
Department of Chemistry, Purdue University, 560 Oval Drive, West Lafayette, IN 47907, USA.
Proc Natl Acad Sci U S A. 2007 Jul 10;104(28):11540-4. doi: 10.1073/pnas.0704449104. Epub 2007 Jul 2.
We report a chemical derivatization method that selects a class of metabolites from a complex mixture and enhances their detection by 13C NMR. Acetylation of amines directly in aqueous medium with 1,1'-13C(2) acetic anhydride is a simple method that creates a high sensitivity and quantitative label in complex biofluids with minimal sample pretreatment. Detection using either 1D or 2D 13C NMR experiments produces highly resolved spectra with improved sensitivity. Experiments to identify and compare amino acids and related metabolites in normal human urine and serum samples as well as in urine from patients with the inborn errors of metabolism tyrosinemia type II, argininosuccinic aciduria, homocystinuria, and phenylketonuria demonstrate the method. The use of metabolite derivatization and 13C NMR spectroscopy produces data suitable for metabolite profiling analysis of biofluids on a time scale that allows routine use. Extension of this approach to enhance the NMR detection of other classes of metabolites has also been accomplished. The improved detection of low-concentration metabolites shown here creates opportunities to improve the understanding of the biological processes and develop improved disease detection methodologies.
我们报告了一种化学衍生化方法,该方法可从复杂混合物中选择一类代谢物,并通过13C核磁共振增强其检测效果。在水介质中直接用1,1'-13C(2)乙酸酐对胺进行乙酰化是一种简单的方法,只需最少的样品预处理就能在复杂生物流体中产生高灵敏度和定量标记。使用一维或二维13C核磁共振实验进行检测可产生分辨率高且灵敏度提高的光谱。在正常人尿液和血清样本以及患有II型酪氨酸血症、精氨琥珀酸尿症、同型胱氨酸尿症和苯丙酮尿症等先天性代谢缺陷患者的尿液中鉴定和比较氨基酸及相关代谢物的实验证明了该方法。代谢物衍生化和13C核磁共振光谱的使用产生了适用于生物流体代谢物谱分析的数据,其时间尺度允许常规使用。这种方法扩展到增强对其他类代谢物的核磁共振检测也已实现。此处显示的对低浓度代谢物的改进检测为增进对生物过程的理解和开发改进的疾病检测方法创造了机会。