Thermodynamics of Materials in Extreme Environments: Thermodynamics and Stabilities of Alloys and Ceramics
Sponsored by: ACerS Basic Science Division, ACerS Energy Materials and Systems Division
Program Organizers: Xiaofeng Guo, Washington State University; Kristina Lilova, Arizona State University; Kyle Brinkman, Clemson University; Alexandra Navrotsky, Arizona State University; Jake Amoroso, Savannah River National Laboratory; Xingbo Liu, West Virginia University; Gustavo Costa, NASA Glenn Research Center
Tuesday 8:00 AM
October 11, 2022
Room: 310
Location: David L. Lawrence Convention Center
Session Chair: Kyle Brinkman, Clemson University
8:00 AM Invited
Persistence of Materials Under Extreme Conditions: Alexandra Navrotsky1; 1Arizona State University
The term “extreme conditions” implies conditions far from those we normally encounter. But the effect of a given condition on different materials may range from minor to catastrophic. A more useful definition is that for a given material, a condition is extreme if it causes substantial changes in physical and chemical properties. Thus 4 K is extreme for helium, while 2000 K has little effect, on alumina. Alumna shows only normal compressibility over a wide range of pressure, while complex oxides show structural and electronic transformations. Alumina is stable under electron irradiation, while silica and many silicates readily amorphize. Radiation damage is a balance between initial damage and relaxation and annealing, with complex intermediate states. Survival under harsh chemical conditions is controlled long-term by thermodynamics and short-term by kinetics, often involving surface passivation. Several examples are presented to better define “extreme”.
8:30 AM
Design of High Melting Point Materials via Deep Learning and First Principles: Qijun Hong1; 1Arizona State University
I build a deep learning model that predicts melting temperature from chemical composition in milliseconds. The model, along with its database that contains approximately 10K melting points, also serves as a handbook for experimental melting temperatures. The model is deployed and publicly available at my group’s webpage. We utilize this model to design refractory materials with extremely high melting temperatures. We also employ this model to study melting temperatures of 4,700 naturally formed minerals, which correlates reasonably well with two major events in Earth's history. This extremely rapid model complements the SLUSCHI method we previously built for accurate, robust, and automated density functional theory melting point calculations. We are integrating the deep learning model and the first principles method to build a framework for rapid and accurate melting temperature prediction.
8:50 AM
Thermo-mechanical Property Prediction of Materials Using a Python Based Interface with Quantum Espresso: Joseph Derrick1; Tejesh Dube1; Jing Zhang1; 1IUPUI MEE Department
The aim of this work is to provide engineers a framework and tool for evaluating thermo-mechanical properties of high temperature materials through a python-based interface that harnesses Quantum Espresso, an open-source simulation package for materials simulation. Quantum Espresso is a predictive material properties code that is based on density-functional theory, planes waves, and pseudopotentials. Several open-source python packages were used to achieve the framework and perform calculations. As this work is to establish a baseline framework upon which further improvements and modifications will be integrated, only materials with well-established testing from external sources, such as silicon carbide and titanium carbide, were used to validate results generated.
9:10 AM Invited
There is More to Heat Capacity Measurements than Calculating Entropy: Brian Woodfield1; 1Brigham Young University
The heat capacity of a material is a concept taught in all general chemistry classes and is explored in only slightly more depth in the typical physical chemistry course. True, accurate low-temperature heat capacity data is used to calculate enthalpy increments and the absolute entropy, vital for determining the complete thermodynamic landscape for materials, but heat capacity data can also provide valuable insight into the fundamental properties of a wide range of geologic and technically important materials. In this talk we will provide a brief survey and introduction to modern heat capacity measurements and how the data is analyzed to extract information about the lattice, electronic, magnetic, nuclear, and defects of the material. Several examples will be provided to demonstrate the breadth of materials that can be studied. The goal is to remind the materials community that heat capacity data can be an important tool in our toolbox of methods.
9:40 AM
High Temperature Boron, Lithium, Iron, and Nickel Aqueous Thermochemistry for Pressurized Water Nuclear Reactors: Jason Rizk1; Brian Wirth2; 1Los Alamos National Laboratory; 2University of Tennessee, Knoxville
Chalk River Unidentified Deposits (CRUD) occur in the core of pressurized water nuclear reactors (PWRs) and cause several phenomena impacting the reactor’s efficiency, lifetime, and reliability. The primary of these phenomena is Axial Offset Anomaly (AOA) which is caused by nonuniform trapping of boron within the core. To aid in the modeling of these deposits, the high temperature aqueous thermochemistry of boron, lithium, nickel, and iron is described using the Helgeson-Kirkham-Flowers (HKF) formalism, which calculates the thermodynamic properties of individual aqueous species for temperatures up to 350 C. Non-ideality is treated using the Pitzer equations. The stability of compounds thought to constitute CRUD is mapped out for a range of possible conditions. The database contains new correlation parameters based on available experimental data and first-principles calculations. The thermodynamic system considered is vital for the power industry and has broader applications such as lithium production from natural brines containing boron.
10:00 AM Break
10:10 AM Invited
The Thermochemical Stability of Rare Earth Oxides and Silicates for Thermal/Environmental Barrier Coating Applications: Mackenzie Ridley1; Kristyn Ardrey2; Cameron Miller2; Kate Tomko2; Mahboobe Jassas2; Kang Wang2; Mukil Ayyasamy2; Prasanna Balachandran2; Bi-Cheng Zhou2; Patrick Hopkins2; Elizabeth Opila2; 1Oak Ridge National Laboratory; 2University of Virginia
Rare earth oxides are among the most thermochemically stable oxides making them desirable as thermal/environmental barrier coating materials in high temperature reactive environments such as turbine engines. Rare earth silicates can be visualized as assemblages of rare earth oxides and silicon-oxygen tetrahedra. The rare earth oxides and silicates exhibit a large number of polymorphs due to the variation in rare earth cation sizes existing for the seventeen rare earths. In this presentation, the many crystal structures for the rare earth oxides and silicates will be described in terms of the rare earth – oxygen coordination polyhedral. Trends for thermal properties as well as the phase stability of monosilicates, disilicates, apatite phases and rare earth oxides in high temperature steam and molten calcium magnesium aluminosilicates present in combustion environments will be related to periodic trends. Possibilities for optimizing properties via synthesis of multicomponent rare earth oxides and silicates are described.
10:40 AM
Measuring Interfacial Thermodynamics from High Temperature In situ TEM Based Bicrystals Tested under Mechanical Load: Shen Dillon1; 1University of California, Irvine
grain boundary and solid-solid interfacial thermodynamics are challenging to probe at individual interfaces. Force balances with applied load and the stress dependence of kinetic response enables the measurement of interfacial energy and the properties of transport mediating defects. Such experiments ideally require the use of small scale samples due to the importance of length scale in the diffusional response. We have developed in situ TEM based mechanical loading experiments coupled with localized laser heating that enable such experiments to be performed over a broad range of temperatures. The talk will discuss how zero creep, Coble creep type experiments, and sintering can be utilized to probe interfacial properties.
11:00 AM
Phase Diagrams of Metal-Nitrogen Compounds at High Pressure and High Temperature: Peter Kroll1; 1University of Texas at Arlington
The quest for hard materials and compounds with high energy density drives high-pressure research of nitrogen-rich compounds, with implications for planetary science. Predicting the formation of nitrogen-rich compounds at high pressure and high temperature requires knowledge of the chemical potential of nitrogen under extreme conditions. We have developed models and provided intelligible data for the chemical potential of nitrogen at temperature and pressure conditions relevant for experiments in Laser–heated diamond anvil cells. In combination with first-principles calculations, we derive pressure−temperature phase diagrams readily accessible to guide experimental efforts. We demonstrate the validity of our approach for characteristic systems, including pure nitrogen and already discovered nitrogen-rich metal-nitrogen phases. We then provide predictions for new metal-nitrogen compounds – binary and ternary – awaiting their synthesis at high pressure and high temperature.