Accurate evaluation of hydrogen crossover in water electrolysis systems for wetted membranes

In fuel cell and electrolysis systems, hydrogen crossover is a phenomenon where hydrogen molecules (H₂) permeate through a membrane, lowering the overall process efficiency and generating a potential safety risk. Many works have been reported to mitigate this undesired phenomenon, but it is yet difficult to accurately measure the rate of hydrogen crossover, particularly when the membrane is fully wetted in water. In this work, we investigated the pressure decay method as a simple, convenient, and low-cost method to characterize hydrogen crossover through wetted membranes for water electrolysis systems. Three different ion exchange membranes were analyzed: Nafion 212, Nafion 115, and in-house sulfonated poly(arylene ether sulfone). We rigorously confirmed our method and data by comparing it to the ANSI dataset with the current state-of-the-art equations of state (EOS) to account for the nonideality of high pressure hydrogen systems. The error from the gas non-ideality was less than 0.03%. As expected, the rate of hydrogen crossover showed high dependency on the temperature; more importantly, hydrogen crossover increased significantly when the membrane was fully soaked in water. For dry membranes, the proposed pressure decay method corroborated well with the literature data measured using other known methods. Moreover, for wetted membranes, the obtained data showed high similarity compared to the GC method which is currently the most reliable method in the literature. We attempted to predict the hydrogen permeability of wetted membranes using the solution diffusion model. The model based on the given thermodynamic parameters overestimated the hydrogen permeability, which can be used to estimate the ion channel tortuosity.