Heterogeneously Catalyzed Oxidation Reactions Using ... - CHEC

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CHAPTER 3 however, seems not preferable as it would refer to 400 mg of catalyst material compared to 150 mg for a 2:1 (Ag/SiO2 – CeO2) ratio. A reason for the increased catalytic activity with a higher CeO2 amount might be that water and benzaldehyde are partly adsorbed thereby preventing catalyst deactivation caused by the reaction products (vide infra). Intensive mixing of Ag/SiO2 and CeO2 by e.g. grinding was not required prior to reaction so both compounds were added separately to the reaction mixture. Nevertheless, a close proximity of Ag/SiO2 and CeO2 was necessary. This is indicated by the observation that when CeO2 and Ag/SiO2 were packed in separated filter paper containers the catalytic activity was not higher than Ag/SiO2 packed in a filter container alone. Additionally, the reaction did not proceed significantly after filtering the hot reaction mixture Conversion (%) 100 80 60 40 20 0 0 5 10 15 20 Silver loading (%) Figure 3‐2: Conversion (■) and selectivity (●) obtained from Ag/SiO2 (calcined in air at 500 °C for 2 h) with different silver loadings. Reaction conditions: 40.0 mL xylene, 19.3 mmol benzyl alcohol, 0.20 g biphenyl, 100 mg Ag/SiO2, 50 mg CeO2, reflux, O2 atmosphere, 3 h reaction time. The lines are for the guide of the eye. 84 100 80 60 40 20 0 Selectivity (%)
Conversion (%) 100 90 80 70 60 50 40 30 20 10 0 3.3 Results 0.1 1 Ratio CeO 2 / 10%Ag/SiO 2 Figure 3‐3: Conversion (■) and selectivity (●) obtained from Ag/SiO2 with different CeO2 to 10%Ag/SiO2 ratios. Reaction conditions: 40.0 mL xylene, 19.3 mmol benzyl alcohol, 0.20 g biphenyl, 100 mg 10%Ag/SiO2 (calcined in air at 500 °C for 2 h) with the indicated CeO2 content, reflux, O2 atmosphere, 3 h reaction time. Note that the abscissa is logarithmic. The lines are for the guide of the eye. Figure 3‐4: TEM images of catalyst mixtures of 10%Ag/SiO2 and CeO2 after 15 min (a) and 300 min (b) reaction time. Arrows indicate CeO2 nanoparticles. Dark circles are silver particles on the silica support (verified with EDX). 85 100 90 80 70 60 50 40 30 20 10 0 Selectivity (%)
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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
Page 47 and 48: 2.3 Selective liquid‐phase oxidat
Page 51 and 52: Table 2-4: Side-chain oxidation of
Page 53 and 54: 2.3.4 Oxidation of cyclohexane 2.3
Page 55 and 56: Table 2-5: Oxidatin of cyclohexane.
Page 59 and 60: Table 2-6: Ring hydroxylation of ar
Page 63 and 64: Table 2-7: Aerobic oxidation of ami
Page 65 and 66: Table 2-8: Oxidation of hydroquinon
Page 69 and 70: Table 2-9: Oxidation of silanes wit
Page 71 and 72: Table 2-10: Oxidation reactions cat
Page 73 and 74: 2.4 Strengths and opportunities of
Page 81 and 82: 2.6 References 2.6 References [1] M
Page 83 and 84: 2.6 References [56] H. Tumma, N. Na
Page 85 and 86: 2.6 References [113] C. Keresszegi,
Page 87 and 88: 2.6 References [169] Q. Zhu, Y. Lia
Page 89 and 90: 2.6 References [223] M. Fetizon, M.
Page 91 and 92: Chapter 3 Selective Liquid-Phase Ox
Page 93 and 94: 3.2 Experimental 3.2.1 Catalyst pre
Page 95 and 96: 3.3 Results Scattering amplitudes a
Page 97: Absorption (a.u.) 1.2 1.0 0.8 0.6 0
Page 101 and 102: 3.3 Results Figure 3‐5: In situ X
Page 103 and 104: 3.3 Results Table 3‐2: Conversion
Page 105 and 106: 3.3 Results In order to gain insigh
Page 107 and 108: 3.3 Results the cost of selectivity
Page 109 and 110: 3.4 Discussion synergetic interacti
Page 111 and 112: 3.5 Conclusions to corroborate the
Page 113 and 114: 3.6 References [29] T. Mitsudome, Y
Page 115 and 116: Chapter 4 Selective Side-Chain Oxid
Page 117 and 118: 4.2 Experimental single‐step flam
Page 119 and 120: 4.2 Experimental alcohol (Aldrich,
Page 121 and 122: 4.3 Results Scheme 4‐1: Oxidation
Page 123 and 124: 4.3 Results Figure 4‐2: Formation
Page 125 and 126: 4.3 Results oxidation by either 2,6
Page 127 and 128: Absorption (a.u.) Absorption (a.u.)
Page 129 and 130: 4.3 Results atomic mixing of Ag and
Page 131 and 132: 4.3 Results Figure 4‐7: Influence
Page 133 and 134: 4.4 Discussion and mechanistic cons
Page 135 and 136: 4.5 Conclusions heterogeneous radic
Page 137 and 138: 4.6 References [29] S.I. Zabinsky,
Page 139 and 140: Chapter 5 Experimental Determinatio
Page 141 and 142: 5.2 Experimental The most important
Page 143 and 144: 5.2 Experimental Eurotherm 2216e te
Page 145 and 146: Figure 5-1: Schematic view of the e
Page 147 and 148: (Eq. 5‐5) AB i j ε AB i j β 5.2
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(a) (b) (c) (d) (e) (f) (g) (h) (i)
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5.3 Results two association sites o
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Pressure (bar) 150 145 140 135 5.3
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5.3 Results Figure 5‐7: Oxidation
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Weight (g) 5.3 Results Figure 5‐8
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5.4 Discussion catalytic reactions
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5.4 Discussion corresponding CO2‐
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5.5 Conclusions 5.5 Conclusions The
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5.6 References [29] I. Tsivintzelis
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6.1 Introduction 6.1 Introduction A
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6.2 Experimental [38]. In a typical
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6.3 Results out in 1 mm quartz tube
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6.3 Results Figure 6‐2: Structure
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6.3 Results Figure 6‐4: Epoxidati
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6.3 Results Figure 6‐6: Compariso
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6.3 Results Figure 6‐8: Influence
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6.3 Results investigated the epoxid
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6.3 Results Figure 6‐10: Co‐epo
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6.3 Results Figure 6‐11: EXAFS an
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6.4 Discussion would need to be for
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6.5 Conclusions Formation of the ep
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6.6 References [28] J. Perles, N. S
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Chapter 7 Concluding Remarks 7.1 Co
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7.2 Final remarks and outlook speci
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Acknowledgements Acknowledgements T
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Curriculum Vitae Matthias Josef Bei
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