Fuel cells with directly deposited membrane (DDM) reveal an ultra low membrane resistance and outperform conventional catalyst coated membranes (CCM).

The interface between the catalyst layer (CL) and the polymer electrolyte membrane (PEM) in a fuel cell has substantial impact on its electrochemical performance. In consequence, there have been growing research activities to engineer this interface to improve the performance of polymer electrolyte membrane fuel cells (PEMFCs). This review summarizes these novel approaches and compares the various techniques. Based on available fuel cell data in the literature, a quantitative comparison of relative improvements due to a micro‐ and nano‐engineered PEM|CL interface is provided. This allows several conclusions: First, regardless of the applied method, a re‐engineering of the PEM|CL interface leads to an improvement of power‐determining parameters, such as mass transport resistances. The latter has hitherto not been clearly connected to the PEM|CL interface and is an important piece of information for future fuel cell development. Second, for patterned membrane surfaces, feature sizes of about 1–10 µm on the membrane surface seem to result in the most significant power density improvement. Third, an engineered PEMCL interface can contribute to extend the fuel cell durability due to enhanced adhesion and contact between the two layers. With this, novel membrane electrode assemblies (MEAs) can be designed that enable significantly higher power densities compared conventional 2D‐layer MEAs.

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Direct membrane deposition was used to produce record platinum catalyst utilization efficiency polymer electrolyte membrane fuel cells. The novel membrane fabrication technique was applied to gas diffusion electrodes with low Pt-loadings of 0.102 and 0.029 mg/cm 2 . Under oxygen atmosphere and 300 kPa abs total pressure, 88 kW/g Pt cathodic catalyst utilization efficiency with a symmetrical Pt-loading of 0.029 mg/cm 2 on the anode and cathode side was achieved. This is 2.3 times higher than the Pt-utilization efficiency of a reference fuel cell prepared using a commercial Nafion N-211 membrane and identical catalyst layers, emphasizing that the improvement is purely attributable to the novel membrane fabrication technique. This value represents the highest Pt-utilization efficiency reported in literature. The results strongly motivate the application of employing direct membrane deposition techniques to prepare low resistance polymer electrolyte thin films in order to compensate for kinetic losses introduced when using low catalyst loadings.

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High‐power, durable composite fuel cell membranes are fabricated here by direct membrane deposition (DMD). Poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVDF‐HFP) nanofibers, decorated with CeO2 nanoparticles are directly electrospun onto gas diffusion electrodes. The nanofiber mesh is impregnated by inkjet‐printed Nafion ionomer dispersion. This results in 12 µm thin multicomponent composite membranes. The nanofibers provide membrane reinforcement, whereas the attached CeO2 nanoparticles promote improved chemical membrane durability due to their radical scavenging properties. In a 100 h accelerated stress test under hot and dry conditions, the reinforced DMD fuel cell shows a more than three times lower voltage decay rate (0.39 mV h−1) compared to a comparably thin Gore membrane (1.36 mV h−1). The maximum power density of the DMD fuel cell drops by 9%, compared to 54% measured for the reference. Impedance spectroscopy reveals that ionic and mass transport resistance of the DMD fuel cell are unaffected by the accelerated stress test. This is in contrast to the reference, where a 90% increase of the mass transport resistance is measured. Energy dispersive X‐ray spectroscopy reveals that no significant migration of cerium into the catalyst layers occurs during degradation. This proves that the PVDF‐HFP backbone provides strong anchoring of CeO2 in the membrane.

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