Revealing adulterated olive oils by triacylglycerol screening methods: Beyond the official method

•The official method is unable to detect high oleic oils at 5–10% in olive oil.•Screening methods are highly sensitive for low levels of high oleic and linoleic oils.•Fingerprinting by HT-GC–MS method has the highest sensitivity and specificity.•TAG fingerprint is a suitable screening tool to detect olive oil adulteration. Official control methods to detect olive oil (OO) adulteration fail to provide satisfactory consumer protection. Thus, faster and more sensitive screening tools are needed to increase their effectiveness. Here, the official method for adulterant detection in OO was compared with three untargeted screening methods based on triacylglycerol analysis using high-throughput (FIA-HESI-HRMS; HT-GC–MS; HPLC-RID) and pattern recognition techniques (PLS-DA). They were assayed on a set of genuine and adulterated samples with a high natural variability (n = 143). The sensitivity of the official method was 1 for high linoleic (HL) blends at ≥2 % but only 0.39 for high oleic (HO) blends at ≥5 %, while specificity was 0.96. The sensitivity of the screening methods in external validation was 0.90–0.99 for the detection of HL and 0.82–0.88 for HO blends. Among them, HT-GC–MS offered the highest sensitivity (0.94) and specificity (0.76), proving to be the most suitable screening tool for OO authentication.