Abstract
In the present work a physically based model of direct methanol fuel cell anode impedance has been developed and validated at different operating current densities. The proposed model includes the two-phase mass transport of both methanol and water through diffusion and catalyst layers and the methanol oxidation reaction involving CO adsorbed intermediate. Model simulations are in good quantitative agreement with experimental observations and permit to evaluate the origin of anode impedance features. Model results confirm that the high frequency 45° linear branch is caused by proton transport limitations within the catalyst layer and that the low frequency inductive behavior is due to surface coverage by CO reaction intermediate. Moreover model predictions elucidate the contribution to the impedance of mass transport phenomena through diffusion layer, that is relevant even at low current density and increases along the channel length. In particular liquid convective fluxes are considered as a process of pressure buildup and breakthrough at diffusion layer intersecting fibers, resulting in a discontinuous phenomenon. By means of this intermittent description it is possible to correctly reproduce mass transport limitations through diffusion layers, that manifest themselves as a second arch superimposed to the first one, peculiar of kinetic losses.
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