Development and Validation of Multi-Residue Method for Drugs Analysis in Human Feces by Liquid Chromatography-Tandem Mass Spectrometry

Abstract

The use of veterinary drugs in animal production is a common practice to secure animal and human health. However, residues of administrated drugs could be present in animal food products. Levels of drugs in food of animal origin are regulated within the European Union. In recent years, residues have been detected not only in food, but also in the environmental elements such as water or soil, meaning that humans are involuntarily exposed to these substances. This article presents a multiclass method for the analysis of various therapeutic groups of pharmaceuticals in human feces. Pharmaceuticals are extracted from feces with an acid extraction solvent, and after filtration the extract was analyzed by HPLC-MS/MS. A limit of detection of 10 ng/g was achieved for 9 pharmaceuticals, with linearity over 0.99 and repeatability and reproducibility lower than 20%. The method was satisfactorily applied in 25 feces samples of individuals that had declared not to be under medical treatment for the last two months. Results indicate the presence of six different compounds at concentration between 10 and 456 ng/g. This preliminary study showed the involuntary exposure of human gut microbiota to active substances such as pharmaceuticals.

Keywords: HPLC–MS/MS; antibiotic; feces; food; food of animal origin; water.

Figure 1

Total ion chromatograms of a blank sample and of a sample spiked with selected pharmaceuticals at 1000 ng/g.

Figure 2

MRM chromatograms of ciprofloxacin, diclofenac, doxycycline and sulfachloropiridazine in a blank sample, sample spiked at 1000 ng/g and in a negative sample.

Figure 3

MRM chromatograms of ciprofloxacin, diclofenac, doxycycline and sulfachloropiridazine in a blank, spiked with pharmaceuticals at 1000 ng/g and in positive samples.