The influence of hydrophobicity and porosity of the catalyst layer (CL) and cathode microporous layer (MPLC) on water distribution and performance of polymer electrolyte membrane fuel cell (PEMFC) is investigated. Hydrophobicity of the layers is altered with the addition of PTFE (polytetrafluoroethylene) and mono‐dispersed polymer particles are utilized to introduce the macro‐pores with a diameter of 0.5 µm and 30 µm within the CL and MPLC, respectively. The treated materials are implemented in a specially designed fuel cell with an active area of 8 cm2 to perform operando high‐resolution neutron tomography measurements. At high current density and humid operating conditions, MPLs with higher PTFE content increase the overall water content of the cell. The more hydrophobic MPL (40 wt.% PTFE) performs below the corresponding reference MPL (20 wt.% PTFE), whereas the performance result of double layer MPLC gives hint for further potential improvements of such design. The local water saturation beneath the land regions with the presence of perforated CL and MPLC is increased which is explained by lower capillary pressure barriers of bigger pores. Despite a higher water content, the perforated layers enhance the performance of the cell at both dry (RH 70%) and humid conditions (RH 120%), indicating that the parallel two‐phase flow is facilitated where the oxygen is transported through small pores and the water is preferentially transported through the bigger pores.

This work describes the effects of catalyst layers (CLs) consisting of hydrophobic PTFE on the performance and water management of PEM fuel cells. Catalyst inks with various PTFE contents were coated on Nafion membranes and characterized using contact angle measurements, SEX-EDX, and mercury porosimetry. Fuel cell tests and electrochemical impedance spectroscopy (EIS) were conducted under varying operating conditions for the prepared materials. At dry conditions, CLs with 5 wt.% PTFE were advantageous for cell performance due to improved membrane hydration, whereas under humid conditions and high air flow rates CLs with 10 wt.% PTFE improved the performance in high current density region. Higher PTFE contents (≥20 wt.%) increased the mass transport resistance due to reduced porosity of the CLs structure. Operando neutron radiography was utilized to study the effects of hydrophobicity gradients within CLs and cathode microporous layer (MPLC) on liquid water distribution. More hydrophobic CLs increased the water content in adjacent layers and improved performance, especially at dry conditions. MPLC with higher PTFE contents increased the overall liquid water within the CLs and GDLs and escalated the water transfer to the anode side. Furthermore, the role of back-diffusion transport mechanism on water distribution was identified for the investigated cells.

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