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FUNDAMENTAL STUDY OF MECHANICAL AND CHEMICAL DEGRADATION MECHANISMS OF PEM FUEL CELL MEMBRANES
Title
FUNDAMENTAL STUDY OF MECHANICAL AND CHEMICAL DEGRADATION MECHANISMS OF PEM FUEL CELL MEMBRANES.
Creator
Yoon, Wonseok, Huang, Xinyu, University of Central Florida
Abstract / Description
One of the important factors determining the lifetime of polymer electrolyte membrane fuel cells (PEMFCs) is membrane degradation and failure. The lack of effective mitigation methods is largely due to the currently very limited understanding of the underlying mechanisms for mechanical and chemical degradations of fuel cell membranes. In order to understand degradation of membranes in fuel cells, two different experimental approaches were developed; one is fuel cell testing under open circuit...
Show moreOne of the important factors determining the lifetime of polymer electrolyte membrane fuel cells (PEMFCs) is membrane degradation and failure. The lack of effective mitigation methods is largely due to the currently very limited understanding of the underlying mechanisms for mechanical and chemical degradations of fuel cell membranes. In order to understand degradation of membranes in fuel cells, two different experimental approaches were developed; one is fuel cell testing under open circuit voltage (OCV) with bi-layer configuration of the membrane electrode assemblies (MEAs) and the other is a modified gas phase FentonÂÂ's test. Accelerated degradation tests for polymer electrolyte membrane (PEM) fuel cells are frequently conducted under open circuit voltage (OCV) conditions at low relative humidity (RH) and high temperature. With the bi-layer MEA technique, it was found that membrane degradation is highly localized across thickness direction of the membrane and qualitatively correlated with location of platinum (Pt) band through mechanical testing, Infrared (IR) spectroscopy, fluoride emission, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and energy dispersive spectroscopy (EDS) measurement. One of the critical experimental observations is that mechanical behavior of membranes subjected to degradation via FentonÂÂ's reaction exhibit completely different behavior with that of membranes from the OCV testing. This result led us to believe that other critical factors such as mechanical stress may affect on membrane degradation and therefore, a modified gas phase FentonÂÂ's test setup was developed to test the hypothesis. Interestingly, the results showed that mechanical stress directly accelerates the degradation rate of ionomer membranes, implying that the rate constant for the degradation reaction is a function of mechanical stress in addition to commonly known factors such as temperature and humidity. Membrane degradation induced by mechanical stress necessitates the prediction of the stress distribution in the membrane under various conditions. One of research focuses was on the developing micromechanism-inspired continuum model for ionomer membranes. The model is the basis for stress analysis, and is based on a hyperelastic model with reptation-inspired viscous flow rule and multiplicative decomposition of viscoelastic and plastic deformation gradient. Finally, evaluation of the membrane degradation requires a fuel cell model since the degradation occurs under fuel cell operating conditions. The fuel cell model included structural mechanics models and multiphysics models which represents other phenomena such as gas and water transport, charge conservation, electrochemical reactions, and energy conservation. The combined model was developed to investigate the compression effect on fuel cell performance and membrane stress distribution.
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Date Issued
2010
Identifier
CFE0003006, ucf:48359
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0003006
Scandia and ceria stabilized zirconia based electrolytes and anodes for intermediate temperature solid oxide fuel cells: Manufacturing and properties
Title
Scandia and ceria stabilized zirconia based electrolytes and anodes for intermediate temperature solid oxide fuel cells: Manufacturing and properties.
Creator
Chen, Yan, Orlovskaya, Nina, An, Linan, Chen, Quanfang, Sohn, Yongho, Raghavan, Seetha, Huang, Xinyu, University of Central Florida
Abstract / Description
Scandia and ceria stabilized zirconia (10 mol% Sc2O3 (-) 1 mol% CeO2 (-) ZrO2, SCSZ) has superior ionic conductivity in the intermediate temperature range for the operation of solid oxide fuel cells, but it does not exhibit good phase stability in comparison with yttria stabilized zirconia (8 mol% Y2O3 (-) ZrO2, YSZ). To maintain high ionic conductivity and improve the stability of the electrolyte, layered structures with YSZ outer layers and SCSZ inner layers were designed, along with the...
Show moreScandia and ceria stabilized zirconia (10 mol% Sc2O3 (-) 1 mol% CeO2 (-) ZrO2, SCSZ) has superior ionic conductivity in the intermediate temperature range for the operation of solid oxide fuel cells, but it does not exhibit good phase stability in comparison with yttria stabilized zirconia (8 mol% Y2O3 (-) ZrO2, YSZ). To maintain high ionic conductivity and improve the stability of the electrolyte, layered structures with YSZ outer layers and SCSZ inner layers were designed, along with the referential electrolytes containing pure SCSZ or YSZ. The electrolytes were manufactured by tape casting, laminating, and pressureless sintering techniques. After sintering, while the thickness of YSZ outer layers remained constant at ~30 ?m, the thickness of inner layers of SCSZ for the 3-, 4- and 6-layer designs varied at ~30, ~60 and ~120 ?m, respectively. Selected characterizations were employed to study the structure, morphology, impurity content and the density of the electrolytes. Furthermore, in situ X-ray diffraction, neutron diffraction and Raman scattering were carried out to study the phase transition and lattice distortion during long-term annealing at 350 (&)deg;C and 275 (&)deg;C for SCSZ and YSZ, respectively, where the dynamic damping occurred when Young's modulus was measured.In YSZ/SCSZ electrolytes, thermal residual stresses and strains were generated due to the mismatch of coefficients of thermal expansion from each layer of different compositions. They could be adjusted by varying the thickness ratios of each layer in different designs of laminates. The theoretical residual stresses have been calculated for different thickness ratios. The effect of thermal residual stress on the biaxial flexural strength was studied in layered electrolytes. The biaxial flexure tests of electrolytes with various layered designs were performed using a ring-on-ring method at both room temperature and 800 (&)deg;C. The maximum principal stress during fracture indicated an increase of flexural strength in the electrolytes with layered structure at both temperatures in comparison with the electrolytes without compositional gradient. Such an increase of strength is the result of the existence of residual compressive stresses in the outer YSZ layer. In addition, Weibull statistics of the strength values were built for the layered electrolytes tested at room temperature, and the effect of thermal residual stresses on Weibull distribution was established. The calculation of residual stress present at the outer layers was verified. The high ionic conductivity was maintained with layered electrolyte designs in the intermediate temperature range. It was also established that the ionic conductivity of layered electrolytes exhibited 7% (-) 11% improvement at 800 (&)deg;C due to the stress/strain effects, and the largest improvements in a certain electrolyte was found to nearly coincide with the largest residual compressive strain in the outer YSZ layer.In addition to the study of layered electrolytes, mechanical properties of porous Ni/SCSZ cermet were studied. The anode materials were reduced by 65 wt% NiO (-) 35 wt% SCSZ (N65) and 50 wt% NiO (-) 50 wt% SCSZ (N50) porous ceramics in the forming gas. Young's modulus as well as strength and fracture toughness of non-reduced and reduced anodes has been measured, both at room and high temperatures. High temperature experiments were performed in the reducing environment of forming gas. It was shown that while at 700 (&)deg;C and 800 (&)deg;C the anode specimens exhibited purely brittle deformation, a brittle-to-ductile transition occurred at 800 (-) 900 (&)deg;C, and the anode deformed plastically at 900 (&)deg;C. Fractography of the anode specimens were studied to identify the fracture modes of the anodes tested at different temperatures.
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Date Issued
2013
Identifier
CFE0005090, ucf:50750
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0005090