Thorough Investigation of the Phenolic Profile of Reputable Greek Honey Varieties: Varietal Discrimination and Floral Markers Identification Using Liquid Chromatography–High-Resolution Mass Spectrometry
Georgios A. Koulis,
Aristeidis S. Tsagkaris,
Panagiota A. Katsianou,
Panagiotis-Loukas P. Gialouris,
Ioannis Martakos,
Fotis Stergiou,
Alberto Fiore,
Eleni I. Panagopoulou,
Sofia Karabournioti,
Carsten Baessmann,
Noud van der Borg,
Marilena E. Dasenaki,
Charalampos Proestos,
Nikolaos S. Thomaidis
Affiliations
Georgios A. Koulis
Analytical Chemistry Laboratory, Chemistry Department, National and Kapodistrian University of Athens, Panepistimiopolis Zographou, 15771 Athens, Greece
Aristeidis S. Tsagkaris
Department of Food Analysis and Nutrition, Faculty of Food and Biochemical Technology, University of Chemistry and Technology Prague, Technická 5, 16628 Prague, Czech Republic
Panagiota A. Katsianou
Analytical Chemistry Laboratory, Chemistry Department, National and Kapodistrian University of Athens, Panepistimiopolis Zographou, 15771 Athens, Greece
Panagiotis-Loukas P. Gialouris
Analytical Chemistry Laboratory, Chemistry Department, National and Kapodistrian University of Athens, Panepistimiopolis Zographou, 15771 Athens, Greece
Ioannis Martakos
Analytical Chemistry Laboratory, Chemistry Department, National and Kapodistrian University of Athens, Panepistimiopolis Zographou, 15771 Athens, Greece
Fotis Stergiou
Analytical Chemistry Laboratory, Chemistry Department, National and Kapodistrian University of Athens, Panepistimiopolis Zographou, 15771 Athens, Greece
Alberto Fiore
Division of Engineering and Food Science, School of Applied Science, Abertay University, Bell Street, Dundee DD1 1HG, UK
Eleni I. Panagopoulou
Analytical Chemistry Laboratory, Chemistry Department, National and Kapodistrian University of Athens, Panepistimiopolis Zographou, 15771 Athens, Greece
Sofia Karabournioti
Attiki Honey SA, Kryoneri Attikis, 14568 Athens, Greece
Carsten Baessmann
Bruker Daltonik GmbH, Fahrenheitstraße 4, 28359 Bremen, Germany
Noud van der Borg
Bruker Daltonik GmbH, Fahrenheitstraße 4, 28359 Bremen, Germany
Marilena E. Dasenaki
Food Chemistry Laboratory, Department of Chemistry, National and Kapodistrian University of Athens, Panepistimiopolis Zographou, 15771 Athens, Greece
Charalampos Proestos
Food Chemistry Laboratory, Department of Chemistry, National and Kapodistrian University of Athens, Panepistimiopolis Zographou, 15771 Athens, Greece
Nikolaos S. Thomaidis
Analytical Chemistry Laboratory, Chemistry Department, National and Kapodistrian University of Athens, Panepistimiopolis Zographou, 15771 Athens, Greece
Honey is a highly consumed commodity due to its potential health benefits upon certain consumption, resulting in a high market price. This fact indicates the need to protect honey from fraudulent acts by delivering comprehensive analytical methodologies. In this study, targeted, suspect and non-targeted metabolomic workflows were applied to identify botanical origin markers of Greek honey. Blossom honey samples (n = 62) and the unifloral fir (n = 10), oak (n = 24), pine (n = 39) and thyme (n = 34) honeys were analyzed using an ultra-high-performance liquid chromatography hybrid quadrupole time-of-flight mass spectrometry (UHPLC-q-TOF-MS) system. Several potential authenticity markers were revealed from the application of different metabolomic workflows. In detail, based on quantitative targeted analysis, three blossom honey markers were found, namely, galangin, pinocembrin and chrysin, while gallic acid concentration was found to be significantly higher in oak honey. Using suspect screening workflow, 12 additional bioactive compounds were identified and semi-quantified, achieving comprehensive metabolomic honey characterization. Lastly, by combining non-targeted screening with advanced chemometrics, it was possible to discriminate thyme from blossom honey and develop binary discriminatory models with high predictive power. In conclusion, a holistic approach to assessing the botanical origin of Greek honey is presented, highlighting the complementarity of the three applied metabolomic approaches.
