"Processing, Stability and High-Temperature Properties of Transition Me" by Gunes Alp Yakaboylu

Date of Graduation

2018

Document Type

Dissertation

Degree Type

PhD

College

Statler College of Engineering and Mineral Resources

Department

Industrial and Managements Systems Engineering

Committee Chair

Edward M Sabolsky

Committee Co-Chair

Xingbo Liu

Committee Member

Konstantinos A Sierros

Committee Member

Charter D Stinespring

Committee Member

Nianqiang Wu

Abstract

Many common electrical materials used in the current sensing applications suffer from structural and functional issues related to high operating temperatures (750°-1600°C), alternating reducing/oxidizing atmospheres, high pressures and corrosive environments. Therefore, there is a need for development of new materials, which are capable to operate under high-temperature and harsh-environments to provide real-time, accurate sensing during industrial processes such as coal gasification and power generation. In this study, electroconductive ceramic composites were fabricated by incorporating the 20-90 vol% of transition metal silicides (MoSi2, WSi2, NbSi2, TaSi 2, CrSi2) within refractory oxides (Al2O 3, ZrO2, Cr2O3), followed by sintering at 1370°-1600°C in argon. The densification, microstructural evolution, phase development and thermal stability of the composites were studied after sintering and further annealing by Archimedes, Scanning electron microscopy (SEM) and X-ray diffraction/Rietveld (XRD) techniques. Their non-isothermal and isothermal oxidation behavior was studied under ambient air using a thermogravimetric analyzer (TGA) at 50°-870°C to understand the key parameters influencing their high-temperature oxidation. The selected composites were also preoxidized at 1000°-1200°C for 10-120 minutes to better understand their high-temperature oxidation kinetics and surface layer formation, and hence, to enhance their oxidation resistance by forming a protective surface layer. XRD, Raman spectroscopy and X-ray photoelectron spectroscopy (XPS) were used for structural and surface characterization. In addition, their 4-point DC electrical conductivities were measured up to 800°-1000°C to study their electrical performance as a function of the composition and processing. A microstructural image analysis method was also developed for quantitatively characterizing the degree of distribution (homogeneity) within the composites. Lastly, thick-film embedded thermocouples (e.g. MoSi2-Al2O3//WSi 2-Al2O3) were fabricated using selected composites by a screen printing technique. Their thermoelectric properties were measured in argon by a typical hot-cold junction temperature measurements, while their structural and microstructural analyses were performed by XPS, XRD and SEM.

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