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<i>Allium ursinum</i> and poisonous adulterants <i>Convallaria majalis</i> and <i>Arum maculatum</i> were used as a model for detection of adulterants in edible plant. <i>A. ursinum</i> samples were spiked with <i>C. majalis</i> and <i>A. maculatum</i> to mimic adulteration. Metabolomic fingerprinting of all samples was performed using ¹H NMR spectroscopy, and the resulting data sets were subjected to multivariate data analysis. As a result of this analysis, signals of adulterants were extracted from the data, and the structures of biomarkers of adulteration from partially purified samples were elucidated using 2D NMR and LC-MS techniques. Thus, isovitexin and vicenin II, azetidine-2-carboxylic acid, and trigonelline indicated adulteration of <i>A. ursinum</i> samples with <i>C. majalis</i>. Isovitexin was also recognized to be an indicator of adulteration of <i>A. ursinum</i> with <i>A. maculatum</i>. In conclusion, the case study of <i>A. ursinum</i> suggested that plant metabolomics approach could be utilized for identification of low molecular weight biomarkers of adulteration in edible plants.