Carbon-supported Platinum Electrocatalysts probed in a Gas Diffusion Setup with Alkaline Environment: how Particle Size and Mesoscopic Environment influence the Degradation Mechanism

In this work, we investigate the stability of four different types of Pt/C fuel cell catalysts upon applying accelerated degradation tests (ADTs) in a gas diffusion electrode (GDE) setup equipped with an anion exchange membrane (AEM). In contrast to previous investigations exposing the catalysts to liquid electrolyte, the GDE setup provides a realistic three-phase boundary of the reactant gas, catalyst and ionomer which enables reactant transport rates close to real fuel cells. Therefore, the GDE setup mimics the degradation of the catalyst under more realistic reaction conditions as compared to conventional electrochemical cells. Combining the determination of the loss in electrochemically active surface area (ECSA) of the Pt/C catalysts via CO stripping measurements with the change in particle size distribution determined by small-angle X-ray scattering (SAXS) measurements, we demonstrate that i) the degradation mechanism depends on the investigated Pt/C catalyst and might indeed be different to the one observed in conventional electrochemical cells, ii) degradation is increased in an oxygen gas atmosphere (as compared to an inert atmosphere), and iii) the observed degradation mechanism depends on the mesoscopic environment of the active phase. The measurements indicate an increased particle growth if small and large particles are immobilized next to each other on the same carbon support flakes as compared to a simple mix of two catalysts with small and large particles, respectively.