A new type of fuel cell architecture, the fuel cell ribbon, is presented. The fuel cell ribbon architecture relies on the gas diffusion layer (GDL) to conduct electrical current in-plane to adjacent cells or collector terminals. The potential advantages of the fuel cell ribbon architecture with respect to conventional fuel cell stacks include reduced manufacturing costs, reduced weight, reduced volume, and reduced component cost. The critical component of fuel cell ribbon assemblies, the gas diffusion media, is investigated herein. Analytical models which focus on the electrical loses within the gas diffusion media of the novel architecture are developed. The materials and treatments necessary to fabricate novel gas diffusion media for fuel cell ribbon assemblies are presented. Experimental results for the novel gas diffusion media of are also presented. One dimensional and two dimensional analytical models were developed for the fuel cell ribbon. The models presented in this work focus on the losses associated with the transport of the electrons in fuel cell ribbon assemblies, rather than the complex system of equations that governs the rate of electron production. The 1-D model indicated that the GDL used in ribbon cells must exhibit an in-plane resistance which is approximately an order of magnitude lower than the resistance of gas diffusion media typically used in conventional fuel cells. A 2-D model was developed with which a parametric study of GDL properties and ribbon cell dimensions was performed. The parametric study indicated that ribbon cells of useful size can be constructed using novel diffusion media that offer reduced resistivity, and that the ribbon cells can produce as much as 80-85% of the power density produced in a conventional fuel cell. Novel gas diffusion media for fuel cell ribbons that have the necessary characteristics suggested by the analytical study were developed.. Properties and performance for a commercially available gas diffusion media, ELAT, were measured as a reference for the novel media developed. The increased thickness PAN (ITPN) series diffusion media was constructed of PAN based fibers exhibiting similar resistive properties to the fibers used in ELAT. The ITPN series of materials were woven in a manner which made them approximately twice the thickness of ELAT, effectively reducing their in-plane resistance to half the resistance exhibited by ELAT. The coarsely woven pitch (CWPT) series of materials were constructed in a manner which yielded a similar number of fibers in the plane of the material to ELAT and a similar material thickness to ELAT, but the fibers used were mesophase pitch based fibers which exhibit a resistivity of approximately one-tenth the resistivity of the fibers used to make the ELAT and ITPN materials. The reduction in fiber resistivity led to the CWPT material having an in-plane resistance an order of magnitude lower than ELAT. The widely used ELAT material exhibited an in-plane resistance of 0.39 Ω/sq., a through-plane area specific resistance of 0.007 Ω-cm2, and a Darcy permeability coefficient of 8.1 Darcys. The novel diffusion materials exhibited in-plane resistances in the range of 0.18-0.036 Ω/sq., through-plane area specific resistances in the range of 0.017-0.013 Ω-cm2, and Darcy permeability coefficients in the range of 30-150 Darcys. Experiments were performed to validate the analytical model and to prove the feasibility of fuel cell ribbon concept. When the novel gas diffusers were adhered to a catalyzed membrane and tested in a ribbon test assembly utilizing serpentine flow channels and in-plane current collection, a range of performance was achieved between 0.28-0.4 A/cm2 at a cell output potential of 0.5 V. In contrast, when ELAT was adhered to a catalyzed membrane and tested in the fixture requiring in-plane conduction, a current density of 0.21 A/cm2 was achieved at 0.5 V. Additionally, the 2-D finite element model was used to predict the performance of a ribbon cell based on the cells performance when a conventional method of through-plane conduction was utilized. The agreement between the experimental data and the model predictions was very good for the ELAT and ITPN materials, whereas the predictions for the CWPT materials showed more significant deviation which was likely due to mass transport and contact resistance effects. / Master of Science

Non-woven carbon paper is a porous material composed of carbon composite and is the preferred material for use as the gas diffusion layer (GDL) of polymer electrolyte membrane (PEM) fuel cells. This material is both chemically and mechanically stable and provides a free path for diffusion of reactants and removal of products and is electrically conductive for transport of electrons. The transport of species in the GDL has a direct effect on the overall reaction rate in the catalyst layer. Numerical simulation of these transport phenomena is dependent on the transport properties associated with each phenomenon. Most of the available correlations in literature for these properties have been formulated for spherical shell porous media, sand and rock, which are not representative of the structure of the GDL. Hence, the objective of this research work is to investigate the transport properties (diffusion coefficient, thermal conductivity, electrical conductivity, intrinsic and relative permeability and the capillary pressure) of the GDL using experimental and numerical techniques. In this thesis, a three-dimensional reconstruction of the complex, anisotropic structure of the GDL based on stochastic models is used to estimate its transport properties. To establish the validity of the numerical results, an extensive comparison is carried out against published and measured experimental data. It was found that the existing theoretical models result in inaccurate estimation of the transport properties, especially in neglecting the anisotropic nature of the layer. Due to the structure of the carbon paper GDL, it was found that the value of the transport properties in the in-plane direction are much higher than that in the through-plane direction. In the in-plane direction, the fibers are aligned in a more structured manner; hence, the resistance to mass transport is reduced. Based on the numerical results presented in this thesis, correlations of the transport properties are developed. Further, the structure of the carbon paper GDL is investigated using the method of standard porosimetry. The addition of Teflon was found have little effect on the overall pore volume at a pore radius of less than 3 micro meters. A transition region where the pore volume increased with the increase in pore radius was found to occur for a pore radius in the range 3<5.5 micro meters regardless of the PTFE content. Finally, the reduction of the overall pore volume was found to be proportional to the PTFE content. The diffusion coefficient is also measured in this thesis using a Loschmidt cell. The effect of temperature and PTFE loading on the overall diffusibility is examined. It was found that the temperature does not have an effect on the overall diffusibility of the GDL. This implies that the structure of the GDL is the main contributor to the resistance to gas diffusion in the GDL. A comparison between the measured diffusibility and that predicted by the existing available models in literature indicate that these models overpredict the diffusion coefficient of the GDL significantly. Finally, both the in-plane and through-plane thermal conductivity were measured using the method of monotonous heating. This method is a quasi-steady method; hence, it allows the measurement to be carried out for a wide range of temperatures. With this method, the phase transformation due to the presence of PTFE in the samples was investigated. Further, it was found that the through-plane thermal conductivity is much lower than its in-plane counterpart and has a different dependency on the temperature. Detailed investigation of the dependency of the thermal conductivity on the temperature suggests that the thermal expansion in the through-plane direction is positive while it is negative in the in-plane direction. This is an important finding in that it assists in further understanding of the structure of the carbon paper GDL. Finally, the thermal resistance in the through-plane direction due to fiber stacking was investigated and was shown to be dependent on both the temperature and compression pressure.

Non-woven carbon paper is a porous material composed of carbon composite and is the preferred material for use as the gas diffusion layer (GDL) of polymer electrolyte membrane (PEM) fuel cells. This material is both chemically and mechanically stable and provides a free path for diffusion of reactants and removal of products and is electrically conductive for transport of electrons. The transport of species in the GDL has a direct effect on the overall reaction rate in the catalyst layer. Numerical simulation of these transport phenomena is dependent on the transport properties associated with each phenomenon. Most of the available correlations in literature for these properties have been formulated for spherical shell porous media, sand and rock, which are not representative of the structure of the GDL. Hence, the objective of this research work is to investigate the transport properties (diffusion coefficient, thermal conductivity, electrical conductivity, intrinsic and relative permeability and the capillary pressure) of the GDL using experimental and numerical techniques. In this thesis, a three-dimensional reconstruction of the complex, anisotropic structure of the GDL based on stochastic models is used to estimate its transport properties. To establish the validity of the numerical results, an extensive comparison is carried out against published and measured experimental data. It was found that the existing theoretical models result in inaccurate estimation of the transport properties, especially in neglecting the anisotropic nature of the layer. Due to the structure of the carbon paper GDL, it was found that the value of the transport properties in the in-plane direction are much higher than that in the through-plane direction. In the in-plane direction, the fibers are aligned in a more structured manner; hence, the resistance to mass transport is reduced. Based on the numerical results presented in this thesis, correlations of the transport properties are developed. Further, the structure of the carbon paper GDL is investigated using the method of standard porosimetry. The addition of Teflon was found have little effect on the overall pore volume at a pore radius of less than 3 micro meters. A transition region where the pore volume increased with the increase in pore radius was found to occur for a pore radius in the range 3<5.5 micro meters regardless of the PTFE content. Finally, the reduction of the overall pore volume was found to be proportional to the PTFE content. The diffusion coefficient is also measured in this thesis using a Loschmidt cell. The effect of temperature and PTFE loading on the overall diffusibility is examined. It was found that the temperature does not have an effect on the overall diffusibility of the GDL. This implies that the structure of the GDL is the main contributor to the resistance to gas diffusion in the GDL. A comparison between the measured diffusibility and that predicted by the existing available models in literature indicate that these models overpredict the diffusion coefficient of the GDL significantly. Finally, both the in-plane and through-plane thermal conductivity were measured using the method of monotonous heating. This method is a quasi-steady method; hence, it allows the measurement to be carried out for a wide range of temperatures. With this method, the phase transformation due to the presence of PTFE in the samples was investigated. Further, it was found that the through-plane thermal conductivity is much lower than its in-plane counterpart and has a different dependency on the temperature. Detailed investigation of the dependency of the thermal conductivity on the temperature suggests that the thermal expansion in the through-plane direction is positive while it is negative in the in-plane direction. This is an important finding in that it assists in further understanding of the structure of the carbon paper GDL. Finally, the thermal resistance in the through-plane direction due to fiber stacking was investigated and was shown to be dependent on both the temperature and compression pressure.

Three testing methods are proposed to characterize properties of fuel cell materials that affect the mechanical durability of proton exchange membranes (PEMs). The first two methods involved measuring the in-plane biaxial strength of PEMs and the biaxial hygrothermal stresses that occur in PEMs during hygrothermal cycles. The third method investigated the nonuniform thickness and compressibility of gas diffusion media which can lead to concentrated compressive stresses in the PEM in the through-plane direction. Fatigue and creep to leak tests using multi-cell pressure-loaded blister fixtures were conducted to obtain the lifetimes of PEMs before reaching a threshold value of gas leakage. These tests are believed to be more relevant than quasi-static uniaxial tensile to rupture tests because of the introduction of biaxial cyclic and sustained loading and the use of gas leakage as the failure criterion. They also have advantages over relative humidity cycling test because of the controllable mechanical loading. Nafion® NRE-211 membrane was tested at three different temperatures and the time-temperature superposition principle was used to construct a stress-lifetime master curve. Tested at 90°C, extruded Ion Power® N111-IP membrane was found to have longer lifetime than Gore™-Select® 57 and Nafion NRE-211 membranes under the same blister pressure profiles. Bimaterial specimens fabricated by bonding a piece of PEM to a substrate material were used to measure the hygral stresses, compressive and tensile, in the PEM during relative humidity cycles. The substrate material and its thickness were carefully chosen so that stresses in the PEM could be obtained directly from the curvature of the bimaterial specimen without knowing the constitutive properties of the PEM. Three commercial PEMs were tested at 80°C by cycling the relative humidity between 90% and 0% and by drying the membrane to 0%RH after submersion in liquid water. Stress histories for all three membranes show strong time-dependencies and Nafion® NRE-211 exhibited the largest tensile stress upon drying. Besides in-plane stresses, hard spots in gas diffusion media (GDM) can locally overcompress PEMs in the out-of-plane direction and cause electrical shorting. In this study, GDM samples sealed with an impermeable Kapton® film on the surface were compressed with uniform air pressure and the nonuniform displacement field was measured with a three-dimensional digital image correlation technique. Hard spots as a result of the nonuniform thickness and compressibility of the GDM were found and their severities as stress risers are evident. Locally, a nominal platen compression (similar to bipolar plate land compression) of 0.68 MPa can lead to compressive stress as large as 2.30 MPa in various hard spots that are in the order of 100s µm to 1 mm in size. / Ph. D.