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Publié par | universitat_stuttgart |
Publié le | 01 janvier 2010 |
Nombre de lectures | 20 |
Poids de l'ouvrage | 11 Mo |
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In-situ X-ray Studies of Model Electrode Surfaces for Solid Oxide Fuel Cells
Navid Khorshidi
Max-Planck-Institut
für Metallforschung
Stuttgart
Institut für theoretische
und angewandte Physik
Universität Stuttgart
مردام یا� �
Für meine Mutter
For my mother
ب
In-situ X-ray Studies of Model Electrode Surfaces
for Solid Oxide Fuel Cells
Von der Fakultät Mathematik und Physik der Universität Stuttgart
zur Erlangung der Würde eines Doktors der
Naturwissenschaften (Dr. rer. nat.) genehmigte Abhandlung
Vorgelegt von
NAVID KHORSHIDI
aus Tehran (Iran)
Hauptberichter: Prof. Dr. H. Dosch Mitberichter: rof. Dr. P. Michler
Tag der mündlichen Prüfung: 17.12.2010
Max-Planck-Institut für Metallforschung Stuttgart
und
Institut für theoretische und angewandte Physik
der Universität Stuttgart
2010
Table of Contents
Acronyms ..................................................................................................................................... 7
Symbols ........ 8
Deutsche Zusammenfassung ................................................................................................ 9
Motivation ............................................. 9
Zielsetzung ......................................... 11
Ergebnisse .......................................................................... 12
Schlussfolgerungen ......................................................................................................................... 21
1 Introduction .................... 25
2 Yttria-Stabilized Zirconia and Nickel Nanoparticles ........................................ 31
2.1 Solid Oxide Fuel Cell ......................................................................... 32
2.2 Motivation ............................................................ 34
2.3 Pure Zirconia ...................................................................................... 36 2.3.1 Cubic ZrO ....................................................................................................................................... 36 22.3.2 Tetragonal ZrO ............................................................................................................................ 37 22.3.3 Monoclinic ZrO (Baddelyite) ................................................................................................. 37 2
2.4 Yttria-Stabilized zirconia ................................................................................................ 37 2.4.1 Partially-Stabilized Zirconia (PSZ) ....................................................................................... 39 2.4.2 Fully-Stabilized Zirconia (FSZ) .............................................................................................. 39
2.5 Fully Yttrium-Stabilized Zirconia Surface Structures .......................................... 46 2.5.1 The (111) Surface ........................................................................................................................ 47 2.5.2 The (110) Surface ........................................................................................................................ 48 2.5.3 The (100) Surface ........................................................................................................................ 49
2.6 Nickel Growth ..................................................................................................................... 51 2.6.1 Bulk Structure of Nickel and Nickel Oxide ........................................................................ 51 2.6.2 Equilibrium Shape....................................................................................................................... 53 2.6.3 Supported Nickel Growth ........................................................................................................ 54
3 Physics of Metal Oxides ............................................................................................... 57
3.1 Bulk Oxides .......................................................... 57 4 3.1.1 Defects.............................................................................................................................................. 58
3.2 Oxide Surfaces .................................................................................................................... 60 3.2.1 Tasker Model ................................................................................................................................. 61 3.2.2 Dangling-Bonds Model .............................................................................................................. 62 3.2.3 ZrO (111) and (100) Termination ....................................................................................... 63 23.2.4 Surface Reconstructions and Defects .................................................................................. 65
4 Experimental Techniques .......................................................................................... 67
4.1 Surface X-ray Diffraction (SXRD) ................................................. 67 4.1.1 X-ray Diffraction (XRD) ............................................................................................................. 67 4.1.2 Surface X-ray Diffraction .......................................................................................................... 71 4.1.3 Non-anomalous and Anomalous X-ray Diffraction ....................................................... 73 4.1.4 Experimental Setups .................................................................................................................. 75 4.1.5 Data Analysis ................................................................................................................................. 79
4.2 Complementary Characterization Techniques ....................................................... 86 4.2.1 X-ray Reflectivity ......................................................................................................................... 86 4.2.2 Atomic Force Microscopy (AFM) .......................................................................................... 89 4.2.3 Auger Electron Spectroscopy (AES) .................................................................................... 92
4.3 Physical Vapor Deposition (PVD) ................................................................................ 95
5 The YSZ(111) Surface .................................. 97
5.1 Surface Structure ............................................................................... 98 5.1.1 Sample Preparation .................................................................................................................... 98 5.1.2 Surface X-ray Diffraction Experiments ............................................................................ 102 5.1.3 Structure Refinement ............................................................................................................. 109 5.1.4 Summary ...................................................................................................................................... 130
5.2 Growth and Shape Change of Nickel Nanoparticles ............................................ 132 5.2.1 Growth .......................................................................................................................................... 132 5.2.2 Particle Shape ............................................................................................................................ 133 5.2.3 Shape Changes ........................................................................................................................... 148 5.2.4 Summary ...................................................................................................................................... 161
6 The YSZ(100) Surface ................................................................................................ 165
6.1 Surface Structure ............. 166 6.1.1 Sample Preparation ................................................................................................................. 166
5 6.1.2 Surface X-ray Diffraction Experiments ............................................................................ 166 6.1.3 Structure Refinements ........................................................................................................... 170 6.1.4 Summary ...................................................................................................................................... 182
6.2 Growth and Shape Change of Nickel Nanoparticles ............................................ 184 6.2.1 Growth .......................................................................................................................................... 184 6.2.2 Particle Shape ............................................................................................................................ 185 6.2.3 Shape Changes ........................................................................................................................... 197 6.2.4 Summary ......................................................