Theses and dissertations

This collection includes both ASU Theses and Dissertations, submitted by graduate students, and the Barrett, Honors College theses submitted by undergraduate students. 

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Investigating the Solid Oxide Fuel Cell Anode Degradation under Siloxane Contamination

Description
Siloxane, a common contaminant present in biogas, is known for adverse effects on cogeneration prime movers. In this work, the solid oxide fuel cell (SOFC) nickel-yttria stabilized zirconia (Ni-YSZ) anode degradation due to poisoning by siloxane was investigated. For this purpose, experiments with different fuels, different deposition substrate materials, different…

Siloxane, a common contaminant present in biogas, is known for adverse effects on cogeneration prime movers. In this work, the solid oxide fuel cell (SOFC) nickel-yttria stabilized zirconia (Ni-YSZ) anode degradation due to poisoning by siloxane was investigated. For this purpose, experiments with different fuels, different deposition substrate materials, different structure of contamination siloxane (cyclic and linear) and entire failure process are conducted in this study. The electrochemical and material characterization methods, such as Electrochemical Impedance Spectroscopy (EIS), Scanning Electron Microscope- Wavelength Dispersive Spectrometers (SEM-WDS), X-ray Photoelectron Spectroscopy (XPS), X-ray Diffraction (XRD), and Raman spectroscopy, were applied to investigate the anode degradation behavior. The electrochemical characterization results show that the SOFCs performance degradation caused by siloxane contamination is irreversible under bio-syngas condition. An equivalent circuit model (ECM) is developed based on electrochemical characterization results. Based on the Distribution of Relaxation Time (DRT) method, the detailed microstructure parameter changes are evaluated corresponding to the ECM results. The results contradict the previously proposed siloxane degradation mechanism as the experimental results show that water can inhibit anode deactivation. For anode materials, Ni is considered a major factor in siloxane deposition reactions in Ni-YSZ anode. Based on the results of XPS, XRD and WDS analysis, an initial layer of carbon deposition develops and is considered a critical process for the siloxane deposition reaction. Based on the experimental results in this study and previous studies about siloxane deposition on metal oxides, the proposed siloxane deposition process occurs in stages consisting of the siloxane adsorption, initial carbon deposition, siloxane polymerization and amorphous silicon dioxide deposition.
ContributorsTian, Jiashen (Author) / Milcarek, Ryan J. (Thesis advisor) / Muhich, Christopher (Committee member) / Wang, Liping (Committee member) / Phelan, Patrick (Committee member) / Nian, Qiong (Committee member) / Arizona State University (Publisher)
Created2022
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Development of the Gas Diffusion Layers to Improve the Lower and Higher Relative Humidity Performance of the Proton Exchange Membrane Fuel Cells

Description
Gas Diffusion Layers (GDL) based on PUREBLACK® carbon and VULCAN® (XC72R) carbon along with catalyst coated membranes were used to fabricate the membrane electrode assemblies for use in proton exchange membrane fuel cells (PEMFCs). Polyethylene glycol was used as the pore-forming agent on the microporous layer to improve the lower…

Gas Diffusion Layers (GDL) based on PUREBLACK® carbon and VULCAN® (XC72R) carbon along with catalyst coated membranes were used to fabricate the membrane electrode assemblies for use in proton exchange membrane fuel cells (PEMFCs). Polyethylene glycol was used as the pore-forming agent on the microporous layer to improve the lower and higher relative humidity performance of the fuel cells. Accelerated stress tests based on the dissolution effect of GDLs were conducted and the long-term performance of the GDLs was evaluated. A single-cell fuel cell was used to evaluate the effect of porosity of the micro-porous layer and the effect of different types of carbon powder on the performance of the fuel cell at different operating relative humidity conditions and compared with commercial GDLs.Both PUREBLACK® and VULCAN® (XC72R) based GDLs show crack-free surface morphology in the Scanning electron microscopy and hydrophobic characteristics in the contact angle measurements. The fuel cell performance is evaluated under relative humidity conditions of 60 and 100 % using H2/O2 and H2/Air at 70 ℃ and the durability is also evaluated for the sample with and without 30% PEG for both carbons. The pristine PUREBLACK® based GDL sample with 30% pore-forming agent (total pore volume of 1.72 cc.g-1) demonstrated the highest performance (peak power densities of 432 and 444 mW.cm-2 at 100 and 60 % RH respectively, using H2/Air). There was a significant increase in the macropores when GDLs are aged in H2O2 and the contact angle dropped to about 14 and 95° for PUREBLACK® and VULCAN® carbon, respectively. Overall PUREBLACK® based GDLs performed the best after ageing both in H2O2 and H2O (average performance degradation of 8% in H2O2 and 8.25% in H2O).
ContributorsChauhan, Nitin (Author) / Kannan, Arunachala Mada (Thesis advisor) / Phelan, Patrick (Committee member) / Nian, Qiong (Committee member) / Arizona State University (Publisher)
Created2021