Radiation-grafted membranes can be considered an alternative to perfluorosulfonic acid (PFSA) membranes, such as Nafion, in a solid polymer electrolyte electrolyzer. Styrene, acrylonitrile, and 1,3-diisopropenylbenzene monomers are cografted into preirradiated 50 μm ethylene tetrafluoroethylene (ETFE) base film, followed by sulfonation to introduce proton exchange sites to the obtained grafted films. The incorporation of grafts throughout the thickness is demonstrated by scanning electron microscopy/energy-dispersive X-ray spectroscopy (SEM/EDX) analysis of the membrane cross-sections. The membranes are analyzed in terms of grafting kinetics, ion-exchange capacity (IEC), and water uptake. The key properties of radiation-grafted membranes and Nafion, such as gas crossover, area resistance, and mechanical properties, are evaluated and compared. The plot of hydrogen crossover versus area resistance of the membranes results in a property map that indicates the target areas for membrane development for electrolyzer applications. Tensile tests are performed to assess the mechanical properties of the membranes. Finally, these three properties are combined to establish a figure of merit, which indicates that radiation-grafted membranes obtained in the present study are promising candidates with properties superior to those of Nafion membranes. A water electrolysis cell test is performed as proof of principle, including a comparison to a commercial membrane electrode assembly (MEA).

The stability of different types of platinum surfaces in the presence of chloride was evaluated by applying a potential of 1.2 V vs reversible hydrogen electrode while the associated mass change in the Pt electrode was monitored with an electrochemical quartz crystal microbalance. The platinum metal surfaces based on the particles and films show a large difference toward dissolution when exposed to small amounts of chloride. While an electrodeposited platinum metal film showed no degradation in a sulfuric acid solution containing 10 ppm of chloride, an electrode made from a fuel cell catalyst (50 wt % Pt/C) lost 10% of its platinum content over a 24 h period when exposed to a sulfuric acid solution containing 10 ppm of chloride. At a chloride concentration of 20 ppm, the onset potential of the Pt oxide formation increased ∼200mV compared to an electrode in a chloride-free solution. The degradation of nanoparticles thus appears to be much more significant than for the electrodeposited platinum electrodes.

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h i g h l i g h t s g r a p h i c a l a b s t r a c t A new technique, that introduces micrometer sized pores in the nanoporous catalyst layer, is tested. The technique uses monodisperse polystyrene particles as pore formers. Macropores in the nanoporous layer improves the polymer electrolyte fuel cell performance. Results are obtained for catalyst loading which are twice the US DOE target for 2020. a b s t r a c tWe show experimentally for the first time that the introduction of macro-pores in the nanoporous catalyst layer of a polymer electrolyte membrane fuel cell can improve its performance. We have achieved a Pt utilization of about 0.23 mg W À1 at 0.6 V which is twice the value of the DOE target for 2020, and three times (0.60 mg W À1 ) smaller than the value of a fully nanoporous reference layer at a catalyst loading of 0.11 mg cm À2 . In this work, monodispersed polystyrene particles with diameters of 0.5 and 1 mm were used as pore formers. Cathode catalyst layers with macroporous volume fractions between 0 and 0.58 were investigated. Maximum performance was observed for fuel cells with a macroporous volume fraction of about 0.52 for a 1 mm thick catalyst layer. The results, which were obtained for the cathode layer, support earlier theoretical predictions that gas access to and water escape from the catalyst can be facilitated by introduction of macropores in the nanoporous layer.

Three different concepts for H 2 -Cl 2 fuel cells have been evaluated. An ordinary PEM fuel cell based on a Nafion membrane, a fuel cell based on a combination of circulating hydrochloric acid and a Nafion membrane and a system based on a phosphoric acid doped Polybenzimidazole (PBI) membrane. None of the investigated systems were able to demonstrate stable operation under the conditions used in this study, due to electrocatalyst corrosion, membrane dehydration and/or electrode flooding. All systems studied achieved open circuit voltages close to the reversible thermodynamic value for production of aqueous hydrochloric acid, suggesting formation of dissolved HCl in the electrolyte and fast electrode kinetics.