Structure and Reactivity of S-Triazine-Based Compounds in C/N/H Chemistry

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Structure and Reactivity of S-Triazine-Based Compounds in C/N/H Chemistry Dissertation zur Erlangung des Doktorgrades der Fakultät für Chemie und Pharmazie der Ludwig-Maximilians-Universität München Structure and Reactivity of s-Triazine-Based Compounds in C/N/H Chemistry Fabian Karl Keßler aus Augsburg, Deutschland 2019 Erklärung Diese Dissertation wurde im Sinne von § 7 der Promotionsordnung vom 28. November 2011 von Herrn Prof. Dr. Wolfgang Schnick betreut. Eidesstattliche Versicherung Diese Dissertation wurde eigenständig und ohne unerlaubte Hilfe erarbeitet. München, 30.10.2019 ............................................... Fabian Karl Keßler Dissertation eingereicht am 05.08.2019 1. Gutachter: Prof. Dr. W. Schnick 2. Gutachter: Prof. Dr. B. V. Lotsch Mündliche Prüfung am 22.10.2019 Danksagung Eine Arbeit wie diese ist niemals das Werk eines Einzelnen, insofern möchte ich an dieser Stelle meinen Dank all jenen ausdrücken, die mich auf diesem Weg begleitet und unterstützt haben. Zuvordest möchte ich Herrn Prof. Dr. Wolfgang Schnick für die Möglichkeit danken, diese Arbeit in seiner Arbeitsgruppe anzufertigen, ebenso wie für die Betreuung und Anleitung die mir im Verlauf dieser Arbeit zuteil wurde. Insbesondere bedanke ich mich für die eingeräumte Gestaltungsfreiheit, sowie für beständige Ermutigung und Unterstützung. Frau Prof. Dr. Bettina Lotsch danke ich herzlichst für die Übernahme des Koreferats dieser Arbeit. Herrn PD Dr. Constantin Hoch, Herrn Prof Dr. Heinz Langhals, Herrn Prof. Dr. Thomas Klapötke und Herrn Prof. Dr. Hans-Christian Böttcher möchte ich meinen Dank für die Bereitschaft aussprechen, sich als weitere Prüfer meiner Doktorarbeit zur Verfügung gestellt zu haben. Ganz besonderen Dank möchte ich Herrn Sebastian Schmiechen, der mich in die Welt der Festkörperchemie eingeführt hat und Frau Nicole Braml, die mir die C/N/H-Chemie nahe gebracht und mir gerade zu Beginn meiner eigenen Arbeiten in diesem Themenbereich eine unverzichtbare Hilfe war, aussprechen. Ohne eure Anleitung wäre ich nicht dort, wo ich heute bin. Weiterhin möchte ich meinen Vorgängern im Bereich der C/N/H-Chemie, Dr. Nicole Braml, Dr. Eva Wirnhier, Dr. Sophia Makowski, Dr. Andreas Sattler und Prof. Dr. Bettina Lotsch für all die Vorarbeiten danken, auf denen ich aufbauen konnte, die mir Orientierung und Inspiration geboten haben und auf diesem Weg den Verlauf meiner Doktorarbeit ganz wesentlich geformt haben. Zahlreichen Personen bin ich darüber hinaus für ganz konkrete Hilfestellungen und Unterstützung bei diversesten Problemstellungen dankbar. Zuallererst sei hierbei Herr PD Dr. Constantin Hoch genannt, dem ich für seine Hilfe und Anleitung bei etlichen kristallographischen Problemen herzlichst danken möchte. Herrn Prof. Dr. Jürgen Senker, Frau Dr. Maria Mesch und Frau Beate Bojer möchte ich meinen Dank für die Hilfe bei der NMR-spektroskopischen Charakterisierung von C/N/H- Verbindungen und die Aufnahme diesbezüglicher Messungen aussprechen. Für weitere Hilfestellung hinsichtlich der Planung und Auswertung von NMR-Experimenten ergeht mein herzlicher Dank an Herrn Thomas Bräuniger. Ganz herzlich möchte ich mich außerdem bei Herrn Dr. Markus Döblinger für die gemeinsame Planung und Durchführung von TEM-Experimenten bedanken. Herrn Wolfgang Wünschheim und Herrn Thomas Miller bin ich außerordentlich dankbar für die Unterstützung in allerlei technischen Belangen. Meinen Kooperationspartnern in München und Leipzig möchte ich für die fruchtbare Zusammenarbeit danken: Herrn Prof. Dr. Christian Ochsenfeld, Herrn Dr. Asbjörn Burow und Herrn Gökcen Savasci für quantenchemische Berechnungen und Herrn Prof. Dr. Oliver Oeckler, Herrn. Dr. Tobias Rosenthal und Herrn Peter Schultz für die Aufnahme und Auswertung von Synchrotron- Beugungsdatensätzen. Ich danke außerdem der Schar fleißiger Praktikanten, welche mich im Laufe meiner Doktorarbeit unterstützt haben und an die ich mein Wissen weitergeben durfte: Lucie Thomas, Sebastian Häringer, Marie Däntl, Frank Schäfer, Thaddäus Koller und Alexander Schuhbeck. Für die Durchführung zahlloser Messungen und die Unterstützung bei der Auswertung und Interpretation der Ergebnisse ergeht mein verbindlichster Dank an: Dr. Peter Mayer und Arthur Haffner für Einkristall-Beugungsexperimente, Marion Sokoll für FT-IR-Aufnahmen, Christian Minke für Festkörper-NMR-Spektroskopie und Rasterelektronenmikroskopie, Susanne Ebert und Robert Eicher für CHNS-Elementaranalytik, Jaroslava Obel für ICP-AES-Messungen, Brigritte Breitenstein und Sonja Kosak für massenspektrometrische Untersuchungen, Sascha Harm für DSC/TG- Aufnahmen und Anna-Katharina Hatz für impedanzspektroskopische Messungen. Jenseits der reinen Wissenschaft möchte ich mich ganz besonders bei meinen Laborkollegen Sascha Harm, Jonny Sappl, Anna-Katharina Hatz und Christian Minke, sowie all den zahlreichen Bacheloranden, F-Praktikanten und Masteranden, mit denen ich im Verlauf der letzten fünf Jahre das Labor teilen durfte, für die angenehme und entspannte Arbeitsatmosphäre und zahllose amüsante Unterhaltungen im und außerhalb des Labors bedanken. Darüber hinaus danke ich an dieser Stelle allen gegenwärtigen und ehemaligen Mitgliedern der Arbeitskreise Schnick, Johrendt und Lotsch, die ich als ungemein herzliche, hilfsbereite und angenehme Kollegen kennen lernen durfte: Dr. Dominik Baumann, Dr. Eva-Maria Bertschler, Dr. Philipp Bielec, Jakob Blahusch, Dr. Nicole Braml, Dr. Thomas Bräuniger, Leo Diehl, Dr. Dajana Durach, Lucien Eisenburger, Eugenia Elzer, Florian Engelsberger, Dr. Erik Flügel, Dr. Gina Friederichs, Lisa Gamperl, Tobias Giftthaler, Kerstin Gottschling, Arthur Haffner, Sascha Harm, Anna-Katharina Hatz, Dr. Jonas Häusler, PD Dr. Constantin Hoch, Dr. Katrin Horky, Dr. Franziska Hummel, Dr. Simon Kloß, Dr. Claudia Lermer, Catrin Löhnert, Olga Lorenz, Dr. Christian Maak, Mathias Mallmann, Dr. Olaf Alberto von Mankowski, Dr. Alexej Marchuk, Christian Minke, Dr. Lukas Neudert, Robin Niklaus, Dr. Ursula Pachmayr, Dr. Simon Peschke, Dr. Christine Pösl, Reinhard Pritzl, Florian Pucher, Dr. Philipp Pust, Tobias Rackl, Dr. Annekathrin Ranft, Dr. Dieter Rau, Bettina Rendenbach, Jonathan Sappl, Hendrik Schlomberg, Dr. Sebastian Schmiechen, Stefanie Schneider, Dr. Katharina Schwinghammer, Juliane Stahl, Dr. Linus Stegbauer, Dr. Philipp Strobel, Dr. Christine Stürzer, Dr. Tobias Stürzer, Dr. Katalin Szendrei-Temesi, Dr. Frank Tambornino, Stefan Trenker, Sebastian Vogel, Peter Wagatha, Sophia Wandelt, Valentin Weippert, Sebastian Wendl, Dr. Erwin Wiesenmayer, Dr. Matthias Wörsching, Wolfgang Wünschheim und Otto Zeman. Ein ganz herzliches Dankeschön ergeht an meine Studienkollegen Philipp Angloher, Martin Reynders, Sabine Auras, Juliane Stahl, Patrick Jüstel, Leonhard Kick, Martin Grundei, Anselm Gruber, Anne Schultz, Patricia Liebhäuser, Thomas Rösener und Kerstin Sigl, die mich nicht nur während meiner Doktorarbeit, sondern bereits zuvor durchs Studium – alles in allem also ein volles Jahrzehnt – begleitet haben und die als meine Freunde zu zählen ich mich außerordentlich glücklich schätze. Schlussendlich möchte ich selbstverständlich auch meiner gesamten Familie danken – insbesondere meinen Eltern Marion und Wilhelm Keßler, sowie meiner Schwester Nina – die mich in all diesen Jahren immer vorbehaltslos und uneingeschränkt unterstützt und bekräftigt haben und mir so erst ermöglicht haben, mein Studium und meine Promotion zum Abschluss zu bringen. Inhalt 1. Introduction .............................................................................................................................................................. 1 2. Summary .................................................................................................................................................................. 33 2.1 Ionic Compounds—Melamium and Ammelinium Salts ......................................................................... 34 2.2 Molecular Adduct Compounds: Melam-Melem (1:1) ............................................................................. 36 2.3 Polymeric Compounds .................................................................................................................................. 37 3. Ionic Compounds—Melamium and Ammelinium Salts .............................................................................. 41 3.1 Melamium Bromide and Melamium Iodide .............................................................................................. 41 3.1.1 Introduction .............................................................................................................................................. 42 3.1.2 Results and Discussion .......................................................................................................................... 44 3.1.3 Conclusions .............................................................................................................................................. 52 3.1.4 Experimental Section ............................................................................................................................. 53 3.1.5 References ................................................................................................................................................. 54 3.2 Melamium Thiocyanate Melam ................................................................................................................... 57 3.2.1 Introduction .............................................................................................................................................. 58 3.2.2 Results and Discussion .........................................................................................................................
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