Two-Phase Flow Through the PTL of PEM Water Electrolyzer: MRI Experiments and Numerical Modeling Using Phase-Field Theory
Authors: Amoury Bilal , Le Tien Dung , Dillet Jérôme , Leclerc Sébastien , Maranzana Gael , Didierjean Sophie 
Published: February 2024

In 2021, estimation shows that the worldwide annual hydrogen production is around 94 Mt. Exploitation of native hydrogen being not mature, it is obtained by its separation from other elements by different methods such as steam methane reforming, and electrolysis of water. The latter supplied by a renewable power source will take part in the development of a green hydrogen economy [1]. In this context, Proton Exchange Membrane (PEM) Electrolyzer is a promising technology due to its flexibility and very quick adaptation to load variations. However, its current development still confronts some limitations at a large industrial scale. For instance, efficiency and durability are directly impacted by the mass transport and electrical transfer within the porous materials at the anode side. Limitation of the water supply to the catalyst layer happens once there is a poor oxygen evacuation which decreases the performance of the device by inducing high overpotential. Furthermore, the PTL has an important role as an electrical conductor for charge transfer from the catalyst layer [1]. The efficiency of all the transport phenomena through the PTL and porous electrode assembly depends on their transport properties which are related to their microstructure and operating conditions. For instance, PTL with a large pore size allows good water and gas transport, while produced electrons choose a long-distance path generating an electrical resistance higher than that in the case of PTL with a small pore size [1]. So, controlled and optimum porosity and pore size could contribute to efficient water, gas, and electron transport. To define the best porous layers morphologies, a deep and accurate understanding of the phenomena is developed in this work by combining modeling and experiments.
The magnetic resonance imaging (MRI) technique was used to quantify the water content within the porous layer during the two-phase flow. Instead of the real PTL made of titanium which is paramagnetic and cannot be used in the MRI, borosilicate filters with thickness, porosity, and pore size similar to the PTL were used. After positioning the sample in the 600 MHz vertical imager (Figure 1-A), a constant water flow rate is introduced while the gas flow rate is varied. The saturation profiles measured through the porous material depend on the gas flow rate and a semi-dryness of the sample occurs (Figure 1-B) with a residual quantity trapped between pores (minimum stable water content). The water flow rate variation in the channel does not affect saturation, but a higher gas flow rate is needed to reach a minimum stable water content for higher water flow rate.The gas pressure drop through the porous medium was measured and bubble formation in the channel was also analyzed. The results show that the pressure drops and types of flow (slug, annular, and bubble flow) depend on orientation of the water channel (horizontally and vertically) and flow direction (up or downward), and on the water and gas flow rates.
To reach a better understanding of the dynamic characteristics of water and oxygen transport over the PTL, the phase-field model based on the Cahn-Hilliard theory was used to simulate the two-phase flow through a porous medium [2]. In this model, the modified Navier-Stokes equations for two phases are coupled with a phase-field equation for describing the diffuse interface. Numerical simulations performed in the COMSOL® multiphysics software were carried on 2D geometries composed of spherical solid grains of different sizes, having properties similar to the PTL used in the MRI experiments. Gas is injected on one side of the sample and flows through the porous medium initially saturated and evacuated on another side in contact with the water channel (Figure 1-C). Gas flow in the porous medium and bubble formation in the water channel are studied while varying the gas and water flow rates. The simulation results give information about the gas pathways within the porous medium and the saturation profiles over time, depending on the gas/water flow rates, which will be compared with experimental results.
[1] J. Parra-Restrepo, “Caractérisation des hétérogénéités de fonctionnement et de dégradation au sein d’un électrolyseur à membrane échangeuse de protons (PEM),” Université de Lorraine, 2020.
[2] J. W. Cahn and J. E. Hilliard, “Free Energy of a Nonuniform System. I. Interfacial Free Energy,” The Journal of Chemical Physics, vol. 28, no. 2, pp. 258–267, Feb. 1958.

Figure 1