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

doi:10.3390/molecules27144444

Thorough Investigation of the Phenolic Profile of Reputable Greek Honey Varieties: Varietal Discrimination and Floral Markers Identification Using Liquid Chromatography-High-Resolution Mass Spectrometry

Molecules. 2022 Jul 11;27(14):4444. doi: 10.3390/molecules27144444.

Authors

Georgios A Koulis^{1

2}, Aristeidis S Tsagkaris³, Panagiota A Katsianou¹, Panagiotis-Loukas P Gialouris^{1

2}, Ioannis Martakos^{1

2}, Fotis Stergiou^{1

4}, Alberto Fiore⁴, Eleni I Panagopoulou¹, Sofia Karabournioti⁵, Carsten Baessmann⁶, Noud van der Borg⁶, Marilena E Dasenaki², Charalampos Proestos², Nikolaos S Thomaidis¹

Affiliations

¹ Analytical Chemistry Laboratory, Chemistry Department, National and Kapodistrian University of Athens, Panepistimiopolis Zographou, 15771 Athens, Greece.
² Food Chemistry Laboratory, Department of Chemistry, National and Kapodistrian University of Athens, Panepistimiopolis Zographou, 15771 Athens, Greece.
³ Department of Food Analysis and Nutrition, Faculty of Food and Biochemical Technology, University of Chemistry and Technology Prague, Technická 5, 16628 Prague, Czech Republic.
⁴ Division of Engineering and Food Science, School of Applied Science, Abertay University, Bell Street, Dundee DD1 1HG, UK.
⁵ Attiki Honey SA, Kryoneri Attikis, 14568 Athens, Greece.
⁶ Bruker Daltonik GmbH, Fahrenheitstraße 4, 28359 Bremen, Germany.

Abstract

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.

Keywords: Greek honey; authenticity; botanical origin; chemometrics; discrimination; high-resolution mass spectrometry; honey; metabolomics; phenolic compounds.

MeSH terms

Biomarkers
Chromatography, High Pressure Liquid / methods
Chromatography, Liquid
Greece
Honey* / analysis
Mass Spectrometry / methods
Phenols / analysis
Thymus Plant* / chemistry

Substances

Biomarkers
Phenols

Grants and funding

The authors acknowledge support of this work by the project “FoodOmicsGR – National Research Infrastructure for the Comprehensive Characterization of Foods” (MIS 5029057), which is implemented under the Action “Reinforcement of the Research and Innovation Infrastructure”, funded by the Operational Programme “Competitiveness, Entrepreneurship and Innovation” (NSRF 2014–2020) and co-financed by Greece and the European Union (European Regional Development Fund).