2017, Landstorfer, Manuel

Consistent boundary conditions for electrochemical interfaces, which cover double layer charging, pseudo-capacitive effects and transfer reactions, are of high demand in electrochemistry and adjacent disciplines. Mathematical modeling and optimization of electrochemical systems is a strongly emerging approach to reduce cost and increase efficiency of super-capacitors, batteries, fuel cells, and electro-catalysis. However, many mathematical models which are used to describe such systems lack a real predictive value. Origin of this shortcoming is the usage of oversimplified boundary conditions. In this work we derive the boundary conditions for some general electrode-electrolyte interface based on non-equilibrium thermodynamics for volumes and surfaces. The resulting equations are widely applicable and cover also tangential transport. The general framework is then applied to a specific material model which allows the deduction of a current-voltage relation and thus a comparison to experimental data. Some simplified 1D examples show the range of applicability of the new approach.

2019, Krause, Beate, Pötschke, Petra, Hickmann, Thorsten

Novel material solutions for polymer based bipolar plates in fuel cells require adapted ways to develop suitable material compositions. The common pathway to develop materials with at the same time high electrical as well as thermal conductivity is the use of conductive graphite as filler with contents up to 80-85 wt.%. However, there is a need to develop recipes with maximized conductive behavior at lowest possible content of conductive filler to enhance the mechanical properties and allow good processability. In this study, composites based on polypropylene (PP) and different filler systems were melt-mixed using a lab scale co-rotating twin-screw extruder and compression molded to bipolar type plates. As fillers synthetic (G) or expanded (EG) graphites were incorporated. At the overall filler content of 60 wt.% or 80 wt% part of the graphite was replaced by highly conductive carbon black (CB, 2.5 wt.%, 5.0 wt.%). It was found that the addition of CB significantly reduced the electrical volume as well as the surface resistivity up to values of 0.12 Ωcm or 4 mΩ/square, respectively. For the values of thermal conductivity the kind and particle size of the selected graphite was important. If expanded graphite was partially replaced by CB, the thermal conductivity of PP/EG+CB composites decreased significantly. Otherwise, the combination of synthetic graphite and CB changed the thermal conductivity of PP composites only marginal at the same overall filler content. For both graphite types the filler with larger particle size resulted in higher thermal conductivity.

2019, Naji, Ahmed, Krause, Beate, Pötschke, Petra, Ameli, Amir

Conductive polymer composites (CPCs) with high electrical and thermal conductivities are demanded for bipolar plates of fuel cells. In this work, CPCs of polycarbonate (PC) filled with carbon nanotube (CNT), carbon fiber (CF), graphite (G), and their double and triple hybrids were prepared using solution casting method followed by compression molding. The results showed that the electrical percolation thresholds for the PC-CNT and PC-CF were ~1 wt% and ~10 wt%, respectively, while no clear threshold was found for PC-G composites. Addition of 3–5 wt% CNT improved the electrical conductivity of PC-CF and PC-G systems up to 6 orders of magnitude and enhanced the thermal conductivity as much as 65%. The results of triple hybrid CPCs (with constant loading of 63 wt%) indicated that the combination of highest electrical and thermal conductivities is achieved when the CF and CNT loadings were near their percolation thresholds. Therefore, a triple filler system of 3 wt% CNT, 10 wt% CF, and 50 wt% G resulted in a composite with the through-plane and in-plane electrical conductivity, and thermal conductivity values of 12.8 S/cm, 8.3 S/cm, and 1.7 W/m•K, respectively. The results offer a combination of properties surpassing the existing values and suitable for high-conductivity applications such as bipolar plates. POLYM. COMPOS., 40:3189–3198, 2019. © 2018 Society of Plastics Engineers.

2019, Rzeczkowski, Piotr, Krause, Beate, Pötschke, Petra

In order to evaluate the suitability of graphite composite materials for use as bipolar plates in fuel cells, polypropylene (PP) was melt compounded with expanded graphite as conductive filler to form composites with different filler contents of 10–80 wt %. Electrical resistivity, thermal conductivity, and mechanical properties were measured and evaluated as a function of filler content. The electrical and thermal conductivities increased with filler content. Tensile and flexural strengths decreased with the incorporation of expanded graphite in PP. With higher graphite contents, however, both strength values remained more or less unchanged and were below the values of pure PP. Young’s-modulus and flexural modulus increased almost linearly with increasing filler content. The results of the thermogravimetric analysis confirmed the actual filler content in the composite materials. In order to evaluate the wettability and suitability for adhesive joining of graphite composites, contact angle measurements were conducted and surface tensions of composite surfaces were calculated. The results showed a significant increase in the surface tension of graphite composites with increasing filler content. Furthermore, graphite composites were adhesively joined and the strength of the joints was evaluated in the lap-shear test. Increasing filler content in the substrate material resulted in higher tensile lap-shear strength. Additionally, the influence of surface treatment (plasma and chemical) on surface tension and tensile lap-shear strength was investigated. The surface treatment led to a significant improvement of both properties.

2019, Rzeczkowski, P., Lucia, M., Müller, A., Facklam, M., Cohnen, A., Schäfer, P., Hopmann, C., Hickmann, T., Pötschke, Petra, Krause, Beate

Novel material solutions for bipolar plates in fuel cells require adapted ways of joining and sealing technologies. Safe and life time enduring leak-tight contacts must be achieved by automatic processes using reasonable joint forces. A proper sealing should manage such challenges as good ageing properties, excellent leaktightness, high thermal conductivity and low gas permeability. Hence in this work, adhesive bonding and welding are considered as suitable methods, which can fulfill the requirements mentioned above. Adhesive systems seem to be more easy to apply than conventional sealing (hand layed-up rubber gaskets), e.g. with automatic dispensers. Additionally, the properties of an adhesive joint can be enhanced by a process-specific surface pre-treatment. This work focuses on the characterization of adhesive systems and their joints with highly filled graphite composites. Mechanical properties of the joints were characterized through lap-shear tests. The influence of ageing caused by humidity or acidic solvent at increased temperature on the bond line properties as well as neat adhesive was examined. The thermal conductivities of neat adhesives and through the entire joint were examined. In order to improve above conductivities, roughening, substrate pre-heating, post-curing and various contact pressure weights were applied. Plasma treatment was chosen as surface pre-treatment method for improving substrate's surface energy. An alternative to bonding is plastic welding, which does not require the use of sealants and adhesives. Based on former study of influences of filler content on the welding process using ultrasonic, hot plate or infrared welding, a welding method for joining the graphite compounds was derived.