Following our two previous publications on material synthesis and on ex situ characterization, we present an experimental in situ study to evaluate the effects of using gas diffusion layers with patterned wettability at the cathode side of polymer electrolyte fuel cells. The operando performance was assessed using traditional electrochemical diagnostics (such as polarization curves) combined with the pulsed gas analysis (PGA) method, which allows measuring the mass transport losses. Neutron radiography was performed simultaneously in order to image the water distribution during operation. Using this methodology, the effects of changing the pattern, including a microporous layer (MPL), and varying the operation conditions (temperature and relative humidity of the cathode gas) have been systematically evaluated. It has been confirmed that water redistributes according to the engineered pattern and that the power density is significantly increased thanks to reduced mass transport losses under various conditions. © The Author Several attempts have been reported in the literature to develop porous materials for fuel cells with optimized liquid/gas transport characteristic.1,2 The variation of microstructure 3,4 and the optimization of hydrophobic coatings and their content permitted significant improvements in performance, 5-9 while the inclusion of microporous layers led to the state-of-the-art materials that we know today.
10-17However, these materials do not have dedicated pathways for liquid and gas transport, but randomly distributed transport paths defined by the pore size and coating distributions.The perforation of GDLs in specific locations showed improved performances under certain operating conditions. 18,19 The local application of hydrophobic coatings was reported to improve oxygen diffusivity using an ex situ test rig combined with X-ray tomography. [20][21][22] An in situ study by the same research group demonstrated clear improvements when combining these hybrid GDLs with micro-grooved gas channels, but the isolated effect of hybrids GDLs did not lead to significant performance improvements. 23 Recently, we reported a method to produce GDLs with patterned wettability 24,25 based on radiation induced chemical grafting, and were the first to publish operando data with such patterned materials, showing a significant improvement when using them on the cathode of a PEFC. 25 Here, we present a comprehensive study on the impact of GDLs having patterned wettability on the water distribution and performance of the cell. The varied parameters include the dimensions of the pattern, the presence or absence of an MPL, and operating parameters such as humidity and temperature, respectively. This work currently rounds up a series of three papers including a detailed study on the material synthesis parameters (Part I) 26 and the analysis of the impact of various material parameters (substrate, coating load, grafting chemistry, pattern dimensions) on the water distribution in capillary injection experiments (Part II...