Heterogeneously Catalyzed Oxidation Reactions Using ... - CHEC

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Acknowledgements the MOF project), Björn Schimmöller and Sotiris E. Pratsinis (for FSP synthesis and very fruitful discussion in the side‐chain oxidation project), Samira Telschow (for determining BET surfaces), Ioannis Tsivintzelis (for phase behavior modeling and advice) and finally Michael T. Wharmby and Paul A. Wright (for MOF synthesis and characterization). Furthermore I would like to thank Alexander Gese and Søren Mikkelsen for performing experiments for me as part of their studies. I would like to acknowledge my colleagues from ETH Zürich and DTU for integrating me so quickly and for the frequent Friday afternoon “meetings”. I enjoyed being a part of both groups! I would like to especially highlight Bertram Kimmerle, Jean‐Michel Andason, Stefan Marx, Fabian Jutz (all ETH), Jacob Brix, Jakob Munkholdt, Nikolaj Musko, Anne Juul Pedersen and Martin Høj (all DTU). Special thanks to Tobias Dokkedal Elmøe and Jacob Brix for translating the summary and the abstract to Danish. I was very much supported by the technicians at DTU especially by Mette Larsen and Anders Tiedje. Mette ordered chemicals and therefore received more than 100 APVs from me. Anders was always at hand when I had technical problems, supported me with ordering equipment and last but not least encouraged me strongly in using the Danish language. The tool shop helped out swiftly when repairs where necessary. Charly Pickel supported me with details and tricks for the “supercritical” setup. A Ph.D. study is nothing without social life. Sincere thanks to my departmental colleagues for fun spare time activities, the members of the Staff Club and to my friends, especially Per and Jacob who were there for me when life was tough. I would like to thank my family, Petra, my mother, Manfred, my father, my grandparents, my girlfriend Samira and my brother Manuel for supporting me during these three years. Without you my life would be so dull! I would like to highlight my mother who was always there for me during the past 28 years of my life and brought me to where I am now! I did my best not to forget anyone and apologize if I should have done so. 184
Curriculum Vitae Matthias Josef Beier Date of Birth June, 26 th , 1982 Place of Birth Braunschweig, Germany Nationality German Parents Petra Schellhorn‐Beier, Social pedagogue Dr. Manfred Beier, Physicist Academic Education B. Sc. (Chemistry), University of Leipzig, Germany, 2005 M. Sc. (Chemistry), University of Leipzig, Germany, 2007 Present Employment 02/2008 – 02/2011: Ph.D. student, Department of Chemical and Biochemical Engineering, Technical University of Denmark 185
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TECHNICAL UNIVERSITY OF DENMARK (DT
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Preface The present dissertation su
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the carboxylic acid, ceria inhibite
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Resume Denne afhandling giver indle
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hvorimod mængden af katalysator ku
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2.3.8 Oxidation of sulfides .......
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5.3.5 Macroscopic mass transport in
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Chapter 1 Introduction With its gre
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1. Introduction Scheme 1‐1: High
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1. Introduction Figure 1‐2: Phase
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1. Introduction [28] S. Bawaked, N.
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2.1 Introduction 2.1 Introduction E
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2.2.1 Synthesis of gold catalysts 2
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2.2 Catalyst synthesis for oxidatio
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2.2 Catalyst synthesis for oxidatio
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2.3 Selective liquid‐phase oxidat
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Table 2-1: Overview over alcohol ox
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Ph O O Ph (4) (5) 2.3 Selective liq
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Table 2-4: Side-chain oxidation of
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2.3.4 Oxidation of cyclohexane 2.3
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Table 2-5: Oxidatin of cyclohexane.
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Table 2-6: Ring hydroxylation of ar
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Table 2-7: Aerobic oxidation of ami
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Table 2-8: Oxidation of hydroquinon
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Table 2-9: Oxidation of silanes wit
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Table 2-10: Oxidation reactions cat
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2.4 Strengths and opportunities of
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2.6 References 2.6 References [1] M
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2.6 References [56] H. Tumma, N. Na
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2.6 References [113] C. Keresszegi,
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2.6 References [169] Q. Zhu, Y. Lia
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2.6 References [223] M. Fetizon, M.
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Chapter 3 Selective Liquid-Phase Ox
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3.2 Experimental 3.2.1 Catalyst pre
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3.3 Results Scattering amplitudes a
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Absorption (a.u.) 1.2 1.0 0.8 0.6 0
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Conversion (%) 100 90 80 70 60 50 4
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3.3 Results Figure 3‐5: In situ X
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3.3 Results Table 3‐2: Conversion
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3.3 Results In order to gain insigh
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3.3 Results the cost of selectivity
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3.4 Discussion synergetic interacti
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3.5 Conclusions to corroborate the
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3.6 References [29] T. Mitsudome, Y
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Chapter 4 Selective Side-Chain Oxid
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4.2 Experimental single‐step flam
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4.2 Experimental alcohol (Aldrich,
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4.3 Results Scheme 4‐1: Oxidation
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4.3 Results Figure 4‐2: Formation
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4.3 Results oxidation by either 2,6
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Absorption (a.u.) Absorption (a.u.)
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4.3 Results atomic mixing of Ag and
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4.3 Results Figure 4‐7: Influence
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4.4 Discussion and mechanistic cons
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4.5 Conclusions heterogeneous radic
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4.6 References [29] S.I. Zabinsky,
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Chapter 5 Experimental Determinatio
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5.2 Experimental The most important
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5.2 Experimental Eurotherm 2216e te
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Figure 5-1: Schematic view of the e
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Page 163 and 164: 5.5 Conclusions 5.5 Conclusions The
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Page 167 and 168: 6.1 Introduction 6.1 Introduction A
Page 169 and 170: 6.2 Experimental [38]. In a typical
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Page 181 and 182: 6.3 Results investigated the epoxid
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Page 187 and 188: 6.4 Discussion would need to be for
Page 189 and 190: 6.5 Conclusions Formation of the ep
Page 191 and 192: 6.6 References [28] J. Perles, N. S
Page 193 and 194: Chapter 7 Concluding Remarks 7.1 Co
Page 195 and 196: 7.2 Final remarks and outlook speci
Page 197: Acknowledgements Acknowledgements T
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