Climate change has propelled the development of alternative power sources that minimize the emission of greenhouse effect gases. Widespread commercialization of polymer electrolyte membrane fuel cell (PEM-FC) technology for transportation and stationary applications requires
cost-competitiveness with improved durability and performance. Advantages compared to battery electric vehicles include fast refueling and long distance range. One way to improve performance and minimize costs of PEM-FC involves the optimization of the nanostructure of the catalyst layer. The rate limiting oxygen reduction reaction occurs at a triple-phase interface in the cathode catalyst layer (CL) between the proton conductor perfluorosulfonic acid, PFSA, the Pt catalyst particles decorating the electron conductor carbon support and gaseous O2 available through the porous framework of the carbon support. Visualization and quantitation of the distribution of
components in the CL requires microscopy techniques. Electron and X-ray microscopy have been used to characterize the distribution of the PFSA relative to the carbon support and porosity in CLs. Understanding and limiting the analytical impact of radiation damage, which occurs due to
the ionizing nature of electrons and X-rays, is needed to improve quantitation, particularly of PFSA. This thesis developed scanning transmission X-ray microscopy (STXM) methods for quantitation of damage due to electron and soft X-ray irradiation in PFSA materials. Chemical
damage to PFSA when irradiated by photons and electrons is dominated by fluorine loss and CF2-CF2 amorphization. The quantitative results are used to set maximum dose limits to help optimize characterization and quantitation of PFSA in fuel cell cathode catalyst layers using: analytical electron microscopy, X-ray microscopy, spectromicroscopy, spectrotomography, spectroptychography and spectro-ptycho-tomography. / Thesis / Doctor of Philosophy (PhD) / Polymer electrolyte membrane fuel cells are an alternative, environmentally friendly power
source for transportation and stationary applications. Major challenges for mass production
include cost competitiveness, improved durability and performance. A key component to enhance
the performance and lower costs involves understanding and improving the spatial distribution of
the perfluorosulfonic acid (PFSA) polymer in the catalyst layer. The ionizing nature of electrons
and X-rays used in microscopy characterization tools challenges PFSA characterization since this
material is radiation sensitive. This thesis developed measurement protocols and methods for
quantitative studies of radiation damage to PFSA and other polymers using scanning transmission
X-ray microscopy. The chemical changes to PFSA films irradiated with photons, electrons and
ultraviolet (UV) photons were studied. The quantitative results identify limits to analytical
electron and soft X-ray microscopy characterization of PFSA. The results are used to optimize
methods for soft X-ray microscopy characterization of PFSA in fuel cell applications.
| Identifer | oai:union.ndltd.org:mcmaster.ca/oai:macsphere.mcmaster.ca:11375/23904 |
| Date | January 2018 |
| Creators | Melo, Lis GA |
| Contributors | Hitchcock, Adam P., Chemistry |
| Source Sets | McMaster University |
| Language | English |
| Detected Language | English |
| Type | Thesis |
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