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Investigations on Behaviour, Occurrence and Risk Assessment of Toxic Pyrrolizidine Alkaloids in Various Food and Feed Matrices

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Investigations on Behaviour, Occurrence and Risk Assessment of Toxic Pyrrolizidine Alkaloids in Various Food and Feed Matrices TECHNISCHE UNIVERSITÄT MÜNCHEN Fakultät Wissenschaftszentrum Weihenstephan für Ernährung, Landnutzung und Umwelt Investigations on Behaviour, Occurrence and Risk Assessment of Toxic Pyrrolizidine Alkaloids in Various Food and Feed Matrices Florian Kaltner Vollständiger Abdruck der von der Fakultät Wissenschaftszentrum Weihenstephan für Ernährung, Landnutzung und Umwelt der Technischen Universität München zur Erlangung des akademischen Grades des Doktors der Naturwissenschaften (Dr. rer. nat.) genehmigten Dissertation. Vorsitzender: Prof. Dr. Wilfried Schwab Prüfer der Dissertation: 1. Prof. Dr. Michael Rychlik 2. Prof. Dr. Karl-Heinz Engel Die Dissertation wurde am 30.01.2020 bei der Technischen Universität München eingereicht und durch die Fakultät Wissenschaftszentrum Weihenstephan für Ernährung, Landnutzung und Umwelt am 13.04.2020 angenommen. Danksagung Eine wissenschaftliche Arbeit ist niemals ausschließlich das Werk einer einzelnen Person. An dieser Stelle möchte ich mich gerne bei einer ganzen Reihe an Menschen bedanken, ohne die die vorliegende Arbeit in dieser Form nicht möglich gewesen wäre. Ungeachtet der folgenden namentlichen Nennung sei hiermit insgesamt auch allen mehr oder weniger am Gelingen der Doktorarbeit Beteiligten mein Dank ausgesprochen. Zunächst bedanke ich mich bei Prof. Dr. Manfred Gareis für die Überlassung des interessanten und ergiebigen Themas und der Möglichkeit, die Arbeit an seinem Lehrstuhl anzufertigen. Prof. Dr. Karl-Heinz Engel möchte ich für seine Tätigkeiten als Zweitgutachter der vorliegenden Arbeit ebenfalls meinen Dank aussprechen, ebenso Prof. Dr. Wilfried Schwab als Prüfungsvorsitzendem. Auch bedanke ich mich bei Prof. Dr. Michael Rychlik als mein Doktorvater für die unkomplizierte Betreuung während der gesamten Promotionszeit. Bei Dr. Patrick Mulder vom Wageningen Food Safety Research Institute und allen bei diesem Prozess involvierten Kollegen bedanke ich mich sehr herzlich für die Möglichkeit, meine Doktorandenzeit unkompliziert um einen Auslandsaufenthalt zu bereichern. Weiter gilt mein Dank den Fachkollegen und Doktoranden der Technischen Universität München und des Leibniz-Instituts aus Freising vor allem für den fachlichen Austausch. Auch diese Kontakte trugen dazu bei, die Promotionszeit erfolgreich zu meistern. Bei all meinen in Oberschleißheim ansässigen Kollegen möchte ich sehr herzlich für die schöne und erlebnisreiche Zeit bedanken, vor allem auch für alle nichtfachlichen Tätigkeiten von Grillabenden über Feierabendbiere zu Billardturnieren, die unbestreitbar ebenso zu einer Doktorarbeit gehören (müssen) wie Laborarbeit, Vorträge und das Verfassen der Dissertation selbst. Danke, dass Ihr mich als Exoten so gut unter Euch Tierärzten aufgenommen habt! Namentlich bedanken möchte ich mich hiermit besonders bei meinem Kollegen, aber auch Mentor und Freund Dr. Christoph Gottschalk. Ihm gilt mein herzlicher Dank für die unzähligen Gespräche, Hilfestellungen, Tipps, Denkanstöße und vor allem Freiheiten während der Bearbeitung des Dissertationsprojekts und allen weiteren gemeinsamen Forschungsvorhaben. Danke Dir vielmals hierfür! Ebenso bedanke ich mich besonders bei meinen anfänglichen Bürogenossen Dr. Mathias Zimmermann und Dr. Ulrike Friedlein, die mir den Einstieg in den Kollegenkreis des Lehrstuhls sehr leicht gemacht haben und bei Bedarf jederzeit für Schabernack, Kaffeepausen oder mehr oder weniger tiefgründige Gespräche zu haben waren. Dem Honigtyp danke ich dabei für die überaus prägenden Probenahmefahrten nach nördlich des Polarkreises und in die hessische Provinz. Die gemeinsame Zeit werde ich immer mindestens mit einem Schmunzeln in Erinnerung behalten. Bei Sarah Eichhorn möchte ich mich sehr herzlich bedanken für viele Stunden Korrekturen, Korrespondenz und Kaffeeklatsch. Ihr alle habt meine Doktorandenzeit sehr bereichert, und dafür gebührt Euch mein herzliches und aufrichtiges Dankeschön! Bei meinen Freunden seit Schul- und Studientagen Andrea Skironi, Sabine von Hochmeister, Julia Groß, Benedikt Bächler und Katharina Bindl möchte ich mich sehr herzlich dafür bedanken, den Weg bis zum heutigen Tag mehr oder weniger aktiv mit mir gegangen zu sein – rückblickend betrachtet wäre ich ohne Euch mit Sicherheit in vielerlei Hinsicht heute nicht der Mensch, zu dem ich geworden bin, und das ist gut so. Dafür meinen aufrichtigen Dank und ich hoffe sehr, dass bei aller räumlichen und zeitlichen Distanz unsere Freundschaften noch lange Bestand haben. Außerdem danke ich meinen Eltern und Stiefeltern Susanne und Georg Maier, Helmut und Kerstin Kaltner, meinen Geschwistern Andreas Kaltner und Sebastian Maier sowie meinen Großeltern für die Unterstützung während der Promotion, das Interesse an dieser Arbeit und einfach dafür, dass es sie gibt. Zuletzt gilt mein wichtigster Dank meiner Partnerin Dr. Sabrina Geißlitz für ihre stetige und uneingeschränkte Unterstützung in allen Belangen, für den intellektuellen Austausch und insbesondere den emotionalen Rückhalt, für ihre Inspiration, Treue, Geduld und Warmherzigkeit, aber auch für ihre Direktheit, nötige Tritte in den Allerwertesten und die Unterstützung beim Kampf gegen innere Schweinehunde. Ohne Dich stünde ich heute sowohl beruflich als auch privat nicht da, wo ich gerade bin. Dafür, liebe Sabrina, gebührt Dir an dieser Stelle mein ehrfürchtigster und immerwährender Dank. Vorbemerkung Der praktische Teil dieser Arbeit wurde in der Zeit von März 2016 bis September 2019 unter der externen Betreuung von Dr. Christoph Gottschalk und Prof. Dr. Dr. habil. Manfred Gareis am Lehrstuhl für Lebensmittelsicherheit, Ludwig-Maximilians-Universität München, in Oberschleißheim durchgeführt. Die Arbeit wurde seitens der Technischen Universität München von Prof. Dr. Michael Rychlik, Lehrstuhl für Analytische Lebensmittelchemie, als Doktorvater betreut. Vorveröffentlichungen PUBLIKATIONEN IN WISSENSCHAFTLICHEN FACHJOURNALEN Kaltner F, Gottschalk C, Gareis M. Pflanzeninhaltsstoffe als Kontaminanten in der Lebensmittelkette. Nachrichten aus der Chemie 2018;66(2):109-113 Kaltner F, Rychlik M, Gareis M, Gottschalk C. Influence of Storage on the Stability of Toxic Pyrrolizidine Alkaloids and Their N-Oxides in Peppermint Tea, Hay and Honey. Journal of Agricultural and Food Chemistry 2018;66(20):5221-5228 Gottschalk C, Huckauf A, Dübecke A, Kaltner F, Zimmermann M, Rahaus I, Beuerle T. Uncertainties in the determination of pyrrolizidine alkaloid levels in naturally contaminated honeys and comparison of results obtained by different analytical approaches. Food Additives and Contaminants - Part A Chemistry, Analysis, Control, Exposure and Risk Assessment 2018;35(7):1366-1383 Kaltner F, Stiglbauer B, Rychlik M, Gareis M, Gottschalk C. Development of a Sensitive Analytical Method for Determining 44 Pyrrolizidine Alkaloids in Teas and Herbal Teas via LC- ESI-MS/MS. Analytical and Bioanalytical Chemistry 2019;411(27):7233-7249 Kaltner F, Rychlik M, Gareis M, Gottschalk C. Occurrence and Risk Assessment of Pyrrolizidine Alkaloids in Spices and Culinary Herbs from Various Geographical Origins. Toxins 2020;12(3):155 KONGRESSBEITRÄGE Kaltner F, Rychlik M, Gareis M, Gottschalk C. Lagerstabilität toxischer Pyrrolizidinalkaloide in Lebens- und Futtermitteln (Vortrag). 46. Deutscher Lebensmittelchemikertag, Würzburg 2017; ISBN 978-3-947197-03-3 Kaltner F, Rychlik M, Gareis M, Gottschalk C. Lagerstabilität toxischer Pyrrolizidinalkaloide in Lebens- und Futtermitteln (Poster). 58. Arbeitstagung des Arbeitsgebietes Lebensmittel- hygiene der Deutschen Veterinärmedizinischen Gesellschaft, Garmisch-Partenkirchen 2017 Kaltner F, Rychlik M, Gareis M, Gottschalk C. Sensitive determination of 44 toxic pyrrolizidine alkaloids in spices and culinary herbs using liquid chromatography tandem - mass spectrometry (Poster). XXII International Mass Spectrometry Conference, Florenz (Italien) 2018; ISBN 978-8-890738-85-2 Kaltner F, Rychlik M, Gareis M, Gottschalk C. Entwicklung einer Analysenmethode zur Bestimmung von 44 Pyrrolizidinalkaloiden in Kräutern und Gewürzen mittels LC-MS/MS (Poster). 47. Deutscher Lebensmittelchemikertag, Berlin 2018; ISBN 978-3-947197-08-8 Kaltner F, Rychlik M, Gareis M, Gottschalk C. Entwicklung einer LC-MS/MS-Methode zur Analyse von 44 Pyrrolizidinalkaloiden in Kräutern und Gewürzen (Poster). 59. Arbeits-tagung des Arbeitsgebietes Lebensmittelhygiene der Deutschen Veterinärmedizinischen Gesellschaft, Garmisch-Partenkirchen 2018 Kaltner F, Kukula V, Rychlik M, Gareis M, Gottschalk C. Screening von Nahrungs- ergänzungsmitteln auf toxische Pyrrolizidinalkaloide (Poster). 48. Deutscher Lebensmittel- chemikertag, Dresden 2019; ISBN 978-3-947197-15-6 Kaltner F, Kukula V, Rychlik M, Gareis M, Gottschalk C. Screening von Nahrungs- ergänzungsmitteln auf toxische Pyrrolizidinalkaloide (Poster). 60. Arbeitstagung des Arbeits- gebietes Lebensmittelsicherheit und Verbraucherschutz der Deutschen Veterinärmedizinischen Gesellschaft, Garmisch-Partenkirchen 2019 Kaltner F, Rychlik M, Gareis M, Gottschalk C. Vorkommen und Risikobewertung von Pyrrolizidinalkaloiden in Kräutern und Gewürzen (Vortrag). 71. Arbeitstagung des Regionalverbands Bayern der Lebensmittelchemischen Gesellschaft, Würzburg 2020 Table of contents Table of contents 1 Introduction ......................................................................................................................... 1 1.1 Structural characterisation and diversity of pyrrolizidine alkaloids ............................ 2 1.2 Occurrence in plants ...................................................................................................
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