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Model System of Zirconium Oxide An First-principles based treatment of charged species equilibria at electrochemical interfaces: model system of zirconium oxide and titanium oxide by Jing Yang B.S., Physics, Peking University, China Submitted to the Department of Materials Science and Engineering in partial fulfillment of the requirements for the degree of Doctor of Philosophy at the MASSACHUSETTS INSTITUTE OF TECHONOLOGY February 2020 © Massachusetts Institute of Technology 2020. All rights reserved. Signature of Author: Jing Yang Department of Materials Science and Engineering January 10th, 2020 Certified by: Bilge Yildiz Professor of Materials Science and Engineering And Professor of Nuclear Science and Engineering Thesis Supervisor Accepted by: Donald R. Sadoway John F. Elliott Professor of Materials Chemistry Chair, Department Committee on Graduate Studies 2 First-principles based treatment of charged species equilibria at electrochemical interfaces: model system of zirconium oxide and titanium oxide by Jing Yang Submitted to the Department of Materials Science and Engineering on Jan. 10th, 2020 in partial fulfillment of the requirements for the degree of Doctor of Philosophy Abstract Ionic defects are known to influence the magnetic, electronic and transport properties of oxide materials. Understanding defect chemistry provides guidelines for defect engineering in various applications including energy storage and conversion, corrosion, and neuromorphic computing devices. While DFT calculations have been proven as a powerful tool for modeling point defects in bulk oxide materials, challenges remain for linking atomistic results with experimentally-measurable materials properties, where impurities and complicated microstructures exist and the materials deviate from ideal bulk behavior. This thesis aims to bridge this gap on two aspects. First, we study the coupled electro-chemo-mechanical effects of ionic impurities in bulk oxide materials. Second, we develop a modeling framework for describing point defect redistribution at extended defects, including grain boundaries, oxide/oxide interfaces, and oxide/water interfaces. The first part of this thesis deals with zirconium oxide in the context of corrosion of zirconium alloys used as nuclear cladding materials in light water reactors. We provide physically-deduced diffusion coefficients for higher-level modeling as well as better mechanistic understanding of zirconium alloy corrosion by studying defect equilibria in ZrO2 passive films. A first-principles based model for predicting charged species redistribution profiles at electrochemical interfaces is established and applied to ZrO2/Cr2O3 and ZrO2/water interfaces, and ZrO2 grain boundaries. Defect redistribution at these extended defects can lead to significant changes in transport properties of oxides. The second part applies similar methodology to TiO2 as a model system for studying field-assisted sintering (FAST). FAST has been demonstrated for multiple ceramic materials as a promising sintering technique for shortening consolidation times and lowering sintering temperatures. By studying the defect chemistry of acceptor- and donor-TiO2 and designing experiments accordingly, we show that while Joule heating is the dominant effect of the applied electric field, the shrinkage rate also correlates strongly with titanium diffusivity. Through donor doping, which increases the concentrations of fast-diffusing titanium interstitials, a higher shrinkage rate is achievable. These results prove that first-principles base calculations are capable of predicting the defect chemistry of oxide materials that quantitatively agree with measured values. Such understanding of defect chemistry gives insights into practical defect engineering strategies that are broadly applicable to electrochemical applications. Thesis Supervisor: Bilge Yildiz Professor of Materials Science and Engineering and Nuclear Science and Engineering 3 Acknowledgement I would like to express my sincere gratitude to Dr. Mostafa Youssef and my thesis advisor, Prof. Bilge Yildiz for their guidance and assistance throughout my thesis project. I would like to thank Dr. Clement Nicollet and Prof. Harry L. Tuller for collaboration on titanium oxide-related research. I am also grateful to Prof. Harry L. Tuller and Prof. Jeffrey Grossman for serving on my thesis committee and for providing constructive feedback throughout my thesis research. During my years in the Yildiz group, I have had the pleasure to interact with many diligent and supportive colleagues and I have learned a lot from them. They are: Dr. Mostafa Youssef, Dr. Dario Marrocchelli, Dr. Yan Chen, Dr. Kiran Adepalli, Dr. Aravind Krishnamoorthy, Dr. Jonathan M. Polfus, Dr. Kiran Adepalli, Dr. Gulin Vardar, Dr. Qiyang Lu, Dr. Lixin Sun, Dr. Roland Bliem, Dr. William Bowman, Dr. Franziska Hess, Dr. Cigdem Toparli, Dr. Konstantin Klyukin, Dr. Pjotrs Zguns, Minh A. Dinh, Jiayue Wang, Dongha Kim, Yen-ting Chi, Vrindaa Somjit, William Zhou, Younggyu Kim, Sara Sand, Hantao Zhang, Seungchan Ryu, and Huijun Chen. I would like to thank my friends, Yixiang Liu and Jinghui Miao, who kept me company. I deeply thank my parents, Chunxiao Wu and Zhongming Yang, who supported me with love and trust. This work is supported by the Consortium for Advanced Simulation of Light Water Reactors (CASL), an Energy Innovation Hub for Modeling and Simulation of Nuclear Reactors under U.S. Department of Energy Contract No. DE-AC05-00OR22725. Computational resources are provided by the Extreme Science and Engineering Discovery Environment (XSEDE) program for calculations performed under allocation No. TG-DMR120025 and National Energy Research Scientific Computing Center (NERSC) under allocation m2403. 4 Contents 1 Introduction ............................................................................................................ 7 1.1 Context: exploit the predictive power of first-principles calculation for designing functional oxides ........................................................................................ 8 1.2 Corrosion of zirconium alloy as nuclear cladding material .......................... 14 1.3 Flash sintering of oxide materials ................................................................. 17 1.4 Thesis outline ................................................................................................ 19 2 Oxygen self-diffusion mechanisms in monoclinic ZrO2 revealed and quantified by density functional theory, random walk and kinetic Monte Carlo calculations .......... 21 2.1 Introduction ................................................................................................... 21 2.2 Methods ......................................................................................................... 23 2.3 Results and discussion ................................................................................... 24 2.4 Conclusion ..................................................................................................... 35 3 First-principles prediction of hydrogen pickup and oxidation kinetics of zirconium alloy: dopant effects from the chemo-mechanical perspective .................................... 36 3.1 Introduction ................................................................................................... 36 3.2 Methods ......................................................................................................... 38 3.3 Results and Discussion .................................................................................. 39 3.4 Conclusion ..................................................................................................... 50 4 Electro-chemo-mechanical effects of lithium incorporation in zirconium oxide . 51 4.1 Introduction ................................................................................................... 51 4.2 Methods ......................................................................................................... 53 4.3 Results and Discussion .................................................................................. 54 4.4 Conclusion ..................................................................................................... 68 5 Predicting point defect equilibria across oxide hetero-interfaces: model system of ZrO2/Cr2O3 ................................................................................................................... 70 5.1 Introduction ................................................................................................... 70 5.2 Methods ......................................................................................................... 76 5.3 Results ........................................................................................................... 85 5.4 Conclusion ..................................................................................................... 99 6 Unravelling water structure, kinetics and thermodynamics at water/monoclinic-ZrO2 interface via ab initio molecular dynamics ................................................................ 101 6.1 Introduction ................................................................................................. 101 6.2 Methods ....................................................................................................... 103 6.3 Results and Discussion ................................................................................ 105 5 6.4 Conclusion ..................................................................................................
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