Occurrence and Risk Assessment of Pyrrolizidine Alkaloids in Spices and Culinary Herbs from Various Geographical Origins

Abstract

Pyrrolizidine alkaloids (PA) and their N-oxides (PANO) are a group of toxic secondary plant metabolites occurring predominantly as contaminants in (herbal) teas, honeys and food supplements, as well as in spices and culinary herbs. Depending on the botanical origin of the contaminating plant, the pattern of PA/PANO can strongly vary within a sample. The current study aimed to broaden the existing data on the occurrence of PA/PANO in spices and culinary herbs. For this, 305 authentic samples covering 15 different matrices mainly harvested in 2016 or 2017 and originating from 36 countries were investigated for the presence of 44 PA/PANO. Fifty-eight percent of the samples contained at least one PA/PANO. The average sum content over all samples was 323 µg/kg (median of 0.9 µg/kg, 95% percentile of 665 µg/kg). The highest amount of 24.6 mg/kg was detected in an oregano sample. Additionally, conspicuous analyte patterns were discovered in samples from similar cultivation regions, indicating related botanical sources of PA/PANO contaminations. Particularly, oregano and cumin from Turkey often contained high amounts of PA/PANO. The results were used to assess the acute and chronic health risks related to PA/PANO intake via spices and culinary herbs, indicating a potential health risk in particular for adults and children with high consumption or when considering worst-case contamination scenarios of a sum content of 5500 µg/kg.

A Miniaturized QuEChERS Method Combined with Ultrahigh Liquid Chromatography Coupled to Tandem Mass Spectrometry for the Analysis of Pyrrolizidine Alkaloids in Oregano Samples

“…Particularly, europine, europine N -oxide, lasiocarpine and lasiocarpine N -oxide were found to a greater or lesser extent in all the samples analyzed. The average concentration of PAs/PANOs was 1254 µg/kg, which is a notably concerning value despite being lower than the ones reported in previous works (3140 and 6160 µg/kg) [ 12 , 36 ]. Although maximum levels for PAs in food have not yet been stablished, a maximum quantity of 1000 μg/kg for herbs such as oregano is currently under discussion by the EU Commission [ 36 ].…”

“…and Borago spp. coharvesting or adulteration [ 9 , 12 , 36 ]. Among the samples analyzed, C-S13, C-S14-A and O-S18 showed the highest values of heliotrine-type compounds—the N -oxides being more predominant than their corresponding PAs ( Figure 5 )—except C-S13, in which europine, lasiocarpine and heliotrine were more abundant than their N -oxides ( Table 3 ).…”

“…Nevertheless, despite the relatively high amounts of PAs recently identified in oregano, to the best of our knowledge, current works focusing on the detection of PAs and their PANOs in aromatic herbs and spices are very scarce in the literature [ 9 , 10 , 11 , 12 ], as research has mainly focused on other types of products such as honey, teas and food supplements [ 13 , 14 , 15 , 16 , 17 , 18 , 19 , 20 , 21 ]. In these few works, it is suggested that aromatic herbs and spices can be widely contaminated with PAs-producing plants during coharvesting or in an intentional way by adulteration.…”

Development and Validation of a UHPLC-ESI-MS/MS Method for Quantification of Oleandrin and Other Cardiac Glycosides and Evaluation of Their Levels in Herbs and Spices from the Belgian Market

“…Since more analytical methods became available for screening of organic molecules at low levels, several contaminants have surfaced as an issue of relevance in food safety. That was the case for other plant toxins, such as tropane alkaloids and pyrrolizidine alkaloids, which were found in herbal teas, herbs and spices, cereal-based food, and herbal food supplements [32][33][34][35], sometimes at levels that can represent risk for human health [36,37]. The current study aimed at developing a reliable analytical method for detection of CGs in plant-based food products.…”

Spread of Jacobaea vulgaris and Occurrence of Pyrrolizidine Alkaloids in Regionally Produced Honeys from Northern Germany: Inter- and Intra-Site Variations and Risk Assessment for Special Consumer Groups

“…In the light of food safety, (herbal) teas, culinary herbs and spices as well as food supplements can be contaminated with PA/PANO via co-harvesting parts or seeds of PA-containing plants and via horizontal transfer in the soil [12]. These food commodities are currently regarded as the main sources of human exposure to PA/PANO [4,13,14]. Food of animal origin, such as milk and meat, may also contribute to the consumers' exposure if animals are fed with PA/PANO-containing feed [4,15].…”