Micromodel of a Gas Diffusion Electrode Tracks In‐Operando Pore‐Scale Wetting Phenomena

Abstract Utilizing carbon dioxide (CO₂) as a resource for carbon monoxide (CO) production using renewable energy requires electrochemical reactors with gas diffusion electrodes that maintain a stable and highly reactive gas/liquid/solid interface. Very little is known about the reasons why gas diffusion electrodes suffer from unstable long‐term operation. Often, this is associated with flooding of the gas diffusion electrode (GDE) within a few hours of operation. A better understanding of parameters influencing the phase behavior at the electrolyte/electrode/gas interface is necessary to increase the durability of GDEs. In this work, a microfluidic structure with multi‐scale porosity featuring heterogeneous surface wettability to realistically represent the behavior of conventional GDEs is presented. A gas/liquid/solid phase boundary was established within a conductive, highly porous structure comprising a silver catalyst and Nafion binder. Inoperando visualization of wetting phenomena was performed using confocal laser scanning microscopy (CLSM). Non‐reversible wetting, wetting of hierarchically porous structures and electrowetting were observed and analyzed. Fluorescence lifetime imaging microscopy (FLIM) enabled the observation of reactions on the model electrode surface. The presented methodology enables the systematic evaluation of spatio‐temporally evolving wetting phenomena as well as species characterization for novel catalyst materials under realistic GDE configurations and process parameters.