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Atom Dynamics of Amorphous Materials by X-Ray Photon Correlation Spectroscopy (Xpcs) & Neutron Spectroscopy

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Atom Dynamics of Amorphous Materials by X-Ray Photon Correlation Spectroscopy (Xpcs) & Neutron Spectroscopy University of Nevada, Reno ATOM DYNAMICS OF AMORPHOUS MATERIALS BY X-RAY PHOTON CORRELATION SPECTROSCOPY (XPCS) & NEUTRON SPECTROSCOPY A Dissertation Submitted in Partial Fulfillment of the Requirements for the degree of Doctor of Philosophy in Materials Science and Engineering By Suchismita Sarker Dr. Dhanesh Chandra, Dissertation Advisor August 2017 i ABSTRACT The mitigation of greenhouse gas emissions on the environment led to the development of non-polluting hydrogen fuel cell use in automobiles. Syngas produced from coal gasification is converted to H2 and CO2 gasses by the water shift reaction. Metallic membranes are used to separate H2 from CO2 and other gasses obtained from the water shift reaction of coal-derived syngas. Commercial crystalline Pd-Ag membranes are widely used for this purpose; however, Pd is an expensive strategic metal. Thus, inexpensive Ni- Nb-Zr alloys are studied. The permeation property of amorphous membranes are known, however, the mechanism of permeation and the nature of the local atomic order of the amorphous membranes was not fully understood. In this study, atom dynamics studied by synchrotron x-ray photon correlation spectroscopy (XPCS) showed the movement of heavier elements such as Ni, Nb, and Zr, at room temperature and 373K. The addition of hydrogen significantly accentuates the motion of atoms as the hydrogen occupies the tetrahedral sites within the icosahedra leading to expansion and short-range diffusion, and no long-range diffusion is observed estimated to be ~10-22 m2/s. Vacuum removal of hydrogen from these membranes showed a contraction of the icosahedra and approached to its original position. This suggests that the process reversible due to the pressure gradient. The XPCS results did not reveal the specific position of hydrogen atoms in the icosahedra; hydrogen goes into the tetrahedral sites of Zr4 and distorted Nb4 sites as determined by neutron vibrational spectroscopy. Total neutron scattering and DFT-MD simulation determine the short-range order of up to 1.8 nm and the nearest neighbor bond distances. Determination of cluster formation was first ii attempted by using small neutron scattering, but it did not have appropriate “Q” range. Thus atom probe tomography (APT) was attempted. This APT study revealed Nb-rich and Zr-rich clusters embedded in Ni-rich matrix, whose compositions are reported. DFT-MD simulation reveals interconnected icosahedra in the metal matrix. The atom dynamics (NVS and XPCS), atom probe tomography, total neutron scattering studies are discussed which have implication in the mechanisms of hydrogen permeation in amorphous metallic membranes. iii To my loving husband & family iv Acknowledgement I hereby would like to express my gratitude to those people who supported me on the way to the completion of this Ph.D. work, which is a truly life-changing experience for me. First and foremost, I would like to thank my advisor, Prof. Dhanesh Chandra, for his inspiring advice and ideas throughout my research work. Ever since, Dr. Chandra has supported me not only by providing a research assistantship, but also constant encouragement. Thanks to him, I had the opportunity to work with several national laboratories. It would not have been possible for me to complete this thesis without his support. I would also like to thank Dr. Yanyao Jiang, Dr. Bin Li, Dr. Wen-Ming Chien, and Dr. Jaak Daemen as my advisory committee members for sparing their precious time and suggestions towards finalizing dissertation. I will be forever thankful to Dr. Beatrice Ruta, at European Synchrotron Radiation Facility for her guidance in x-ray photon correlation spectroscopy work and Dr. Terrence J. Udovic for his immense support for neutron work. I am also indebted to Dr. Maddury Somayazulu, Dr. Dieter Isheim and Dr. Graham King for high pressure, atom tomography and neutron work. I would also like to thank Dr. Qi An and S. I. Morozov for DFT-MD simulation work. I would like to give my special thanks to my friends Madhura for giving me a pleasant and memorable time at school. Finally, I want to express thanks to my parents, in-laws and family. Their unconditional love and support has been all these years throughout my study, specially, my best friend and husband Unmagna for always believing in me and encouraging me. I would not have made it this far without him. His love and limitless emotional support helped me make my way to success. v TABLE OF CONTENTS ABSTRACT ......................................................................................................................... i Acknowledgement ............................................................................................................. iv List of Table ...................................................................................................................... vii List of Figure.................................................................................................................... viii 1 Introduction ................................................................................................................. 1 1.1 Organization of the Thesis ................................................................................... 4 1.2 Amorphous material for Hydrogen permeability ................................................. 6 1.3 Development of Ni-based membranes for Hydrogen permeation ....................... 7 1.4 Metallic glasses .................................................................................................. 10 1.5 Glass transition ................................................................................................... 11 2 Dynamical X-ray Studies of Disordered Materials: X-ray Photon Correlation Spectroscopy (XPCS) ....................................................................................................... 18 2.1 Synchrotron Technique ...................................................................................... 23 2.2 Theory of XPCS ................................................................................................. 30 2.3 Historical Perspective of XPCS ......................................................................... 37 2.4 Experimental Details .......................................................................................... 48 2.5 Results and Discussions ..................................................................................... 49 2.5.1 XPCS Results .............................................................................................. 49 2.5.2 Extended X-ray Absorption Spectroscopy Results ..................................... 62 3 Neutron Characterization Studies of Disordered Materials ....................................... 68 3.1 Introduction to Neutron scattering studies ......................................................... 68 3.2 Inelastic neutron scattering Studies .................................................................... 76 3.3 Neutron Vibrational Spectroscopy ..................................................................... 79 3.3.1 Theory ......................................................................................................... 79 3.3.2 Experimental Details ................................................................................... 99 3.3.3 NVS Result and Discussions .................................................................... 103 3.4 Neutron Total Scattering experiment (HIPD) .................................................. 131 3.4.1 Theory of Total Neutron Scattering .......................................................... 131 3.4.2 Result and Discussions ............................................................................. 134 vi 3.5 Small angle neutron scattering (SANS) ........................................................... 137 3.5.1 Brief Theory .............................................................................................. 138 3.5.2 Result and Discussions ............................................................................. 143 4 Atom Probe Tomography ........................................................................................ 145 4.1 Introduction: ..................................................................................................... 145 4.2 Theory .............................................................................................................. 148 4.3 Experimental details ......................................................................................... 152 4.3.1 Sample preparation by Focused Ion Beam ............................................... 152 4.3.2 Local Electrode Atom Probe (LEAP) ....................................................... 154 4.4 Results and Discussions ................................................................................... 156 5 High-Pressure Studies on Disordered Materials: Diamond Anvil Cell (DAC) ....... 173 5.1 Introduction ...................................................................................................... 173 5.2 Diamond Anvil Cell and Raman Spectroscopy................................................ 173 5.3 Experimental Details ........................................................................................ 177 5.4 Result and Discussions ..................................................................................... 179 6 Summary & Future Study ........................................................................................ 187 7 References
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