Unveiling the Role of PTFE Surface Coverage on Controlling Gas Diffusion Layer Water Content.

Gas diffusion layers (GDLs) are usually coated with a hydrophobic agent to achieve a delicate balance between liquid and gas phases to maximize mass transport. Yet, most GDL numerical models to date have assumed an average contact angle for all materials, thereby eliminating the possibility of studying the role of the polytetrafluoroethylene (PTFE) content. This study introduces two mixed wettability algorithms to predict the mixed wetting behavior of GDLs composed of multiple materials. The algorithms employ contact angle and distance to solid materials to determine the critical capillary pressure for each pore voxel. The application of the algorithms to the estimation of capillary pressure vs saturation curves for two GDLs, namely, a micro-computed tomography (µ-CT) reconstructed SGL 39BA GDL and a stochastically reconstructed Toray 120C GDL, showed that, in agreement with experimental data, the addition of PTFE resulted in a decrease in saturation at a given capillary pressure. For Toray-120C, the mixed wettability model was capable of reproducing experimentally observed features in the intrusion curve at low saturation that could not be reproduced with a single wettability model, providing a clear link between PTFE coverage and intrusion at low saturation. Numerical results also predicted an increased breakthrough pressure and a decrease in saturation with increasing PTFE, in agreement with experimental observations. The decreased saturation at breakthrough improves gas transport through the layer while maintaining the layer's ability to remove water. Diffusivity simulations confirm the increase in diffusivity at breakthrough with increasing PTFE, thereby providing a rationale for the addition of PTFE, as well as for the optimal amount. This study emphasizes the importance of multimaterial wetting models and calls for more detailed investigations into PTFE and ionomer distributions in GDLs and catalyst layers, respectively.

Spatio-Temporal Electrowetting and Reaction Monitoring in Microfluidic Gas Diffusion Electrode Elucidates Mass Transport Limitations.

The use of gas diffusion electrodes (GDEs) enables efficient electrochemical CO2 reduction and may be a viable technology in CO2 utilization after carbon capture. Understanding the spatio-temporal phenomena at the triple-phase boundary formed inside GDEs remains a challenge; yet it is critical to design and optimize industrial electrodes for gas-fed electrolyzers. Thus far, transport and reaction phenomena are not yet fully understood at the microscale, among other factors, due to a lack of experimental analysis methods for porous electrodes under operating conditions. In this work, a realistic microfluidic GDE surrogate is presented. Combined with fluorescence lifetime imaging microscopy (FLIM), the methodology allows monitoring of wetting and local pH, representing the dynamic (in)stability of the triple phase boundary in operando. Upon charging the electrode, immediate wetting leads to an initial flooding of the catalyst layer, followed by spatially oscillating pH changes. The micromodel presented gives an experimental insight into transport phenomena within porous electrodes, which is so far difficult to achieve. The methodology and proof of the spatio-temporal pH and wetting oscillations open new opportunities to further comprehend the relationship between gas diffusion electrode properties and electrical currents originating at a given surface potential.