Dokument: Metal-nanoparticles: synthesis and application in catalysis.
| Titel: | Metal-nanoparticles: synthesis and application in catalysis. | |||||||
| URL für Lesezeichen: | https://docserv.uni-duesseldorf.de/servlets/DocumentServlet?id=36521 | |||||||
| URN (NBN): | urn:nbn:de:hbz:061-20151208-104703-3 | |||||||
| Kollektion: | Dissertationen | |||||||
| Sprache: | Englisch | |||||||
| Dokumententyp: | Wissenschaftliche Abschlussarbeiten » Dissertation | |||||||
| Medientyp: | Text | |||||||
| Autor: | Marcos Esteban, Raquel [Autor] | |||||||
| Dateien: |
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| Dewey Dezimal-Klassifikation: | 500 Naturwissenschaften und Mathematik » 540 Chemie | |||||||
| Beschreibung: | Metal-nanoparticles (M-NPs) are of significant interest due to their novel and characteristic properties. Their high volume area and number of active centers in comparison with bulk materials, transform the metal-nanoparticles and nanomaterials into attractive materials, in particular, in the field of catalysis. Ionic liquids (ILs) are a good alternative for the stabilization of M-NPs in contrast to the synthesis in organic solvents because their ionic nature, high polarity, high viscosity and electrostatic-steric supramolecular network help to the stabilization of M-NPs without the use of stabilizers.
In this work, we were focused on the deposition of iridium and ruthenium nanoparticles on thermally reduced graphite oxide (also named graphene or abbreviated as TRGO) using the ionic liquid 1-butyl-3-methyltetrafluoroborate ([BMIm][BF4]) and propylene carbonate (PC). The deposition of Ir-NPs on TRGO could be achieved by the thermal decomposition of tetrairidium dodecacarbonyl, Ir4(CO)12, through microwave (MWI) or e-beam (IBA Rhodotron accelerator) irradiation in [BMIm][BF4], achieving small and narrow size distributions of 1.0 ± 0.4 and 2.7 ± 0.7 nm and of 3.6 ± 1.0 nm respectively. The Ir@TRGO nanomaterials were used for the hydrogenation of benzene or cyclohexene to cyclohexane, an important intermediate in the synthesis of Nylon. The microwave obtained Ir@TRGO nanomaterials achieved a turn over frequency (TOF) up to 10000 h–1 after ten consecutive hydrogenation runs, meanwhile the nanomaterials from the e-beam irradiation showed a lower TOF of 4582 h–1 after five runs. Ir@TRGO nanomaterials from the MWI experiments were also used for the hydrogenations of cyclohexene to cyclohexane (TOF 68000 h–1) and of levulinic acid to -valerolactone (GVL) (TOF = 1430 h–1). A similar method was used for the synthesis of Ru@TRGO nanomaterials, which could be obtained from the microwave decomposition of Ru3(CO)12 in PC, to achieve a size distribution of 4.3 ± 1.4 nm for Ru-NPs. The hydrogenation of benzene to cyclohexane achieved a TOF of ca. 34000 h–1 after ten consecutives hydrogenation runs. In parallel, we were focused on the synthesis of copper-nanoparticles (Cu-NPs) and cuprite-nanocubes (Cu2O-NCs) in [BMIm][BF4] and PC. The reduction through microwave irradiation led to the formation of Cu-NPs with sizes distributions of 45 nm from Cu(BF4)2 in PC and of 3.3 ± 0.9 nm from Cu(acac)2 in [BMIm][BF4]. The organometallic compound copper(II) bis(1 (dimethylamino)propan-2-olate), Cu(OCH(Me)CH2NMe2)2, achieved size distributions of 3.1 ± 0.7 nm (in PC) and 3.7 ± 1.4 nm (in [BMIm][BF4]). The Cu2O-NCs could be achieved by selecting the water content metal salt Cu(AcO)2 monohydrate as starting material in [BMIm][BF4], which led to the formation of Cu2O-NCs with size distributions of 43 ± 15 nm. | |||||||
| Lizenz: |  Urheberrechtsschutz | |||||||
| Fachbereich / Einrichtung: | Mathematisch- Naturwissenschaftliche Fakultät » WE Chemie » Anorganische Chemie und Strukturchemie | |||||||
| Dokument erstellt am: | 08.12.2015 | |||||||
| Dateien geändert am: | 08.12.2015 | |||||||
| Promotionsantrag am: | 05.10.2015 | |||||||
| Datum der Promotion: | 20.11.2015 |
