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Hydrogen produced in a polymer electrolyte membrane (PEM) electrolyzer must be stored under high pressure. It is discussed whether the gas should be compressed in subsequent gas compressors or by the electrolyzer. While gas compressor stages can be reduced in the case of electrochemical compression, safety problems arise for thin membranes due to the undesired permeation of hydrogen across the membrane to the oxygen side, forming an explosive gas. In this study, a PEM system is modeled to evaluate the membrane-specific total system efficiency. The optimum efficiency is given depending on the external heat requirement, permeation, cell pressure, current density, and membrane thickness. It shows that the heat requirement and hydrogen permeation dominate the maximum efficiency below 1.6 V, while, above, the cell polarization is decisive. In addition, a pressure-optimized cell operation is introduced by which the optimum cathode pressure is set as a function of current density and membrane thickness. This approach indicates that thin membranes do not provide increased safety issues compared to thick membranes. However, operating an N212-based system instead of an N117-based one can generate twice the amount of hydrogen at the same system efficiency while only one compressor stage must be added.

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Hydrogen crossover poses a crucial issue for polymer electrolyte membrane (PEM) water electrolysers in terms of safe operation and efficiency losses, especially at increased hydrogen pressures. Besides the impact of external operating conditions, the structural properties of the materials also influence the mass transport within the cell. In this study, we provide an analysis of the effect of elevated cathode pressures (up to 15 bar) in addition to increased compression of the membrane electrode assembly on hydrogen crossover and the cell performance, using thin Nafion 212 membranes and current densities up to 3.6 A cm-2. It is shown that a higher compression leads to increased mass transport overpotentials, although the overall cell performance is improved due to the decreased ohmic losses. The mass transport limitations also become visible in enhanced anodic hydrogen contents with increasing compression at high current densities. Moreover, increases in cathode pressure are amplifying the compression effect on hydrogen crossover and mass transport losses. The results indicate that the cell voltage should not be the only criterion for optimizing the system design, but that the material design has to be considered for the reduction of hydrogen crossover in PEM water electrolysis.