Journal of Power Sources, Vol.123, No.2, 182-189, 2003
Homogeneous kinetics and equilibrium predictions of coking propensity in the anode channels of direct oxidation solid-oxide fuel cells using dry natural gas
Direct electrochemical oxidation (DECO) solid-oxide fuel cells (SOFCs) offer the potential to generate electrical power from hydrocarbon fuels without the need for upstream fuel processing, such as reforming. However, with pure hydrocarbon fuel entering the flow channels at temperatures typically above 700degreesC, fuel pyrolysis can cause molecular-weight growth and the formation of deleterious carbonaceous deposits. This paper, which develops a plug-flow model for fuel (natural gas surrogate) within the anode channels, considers the elementary gas-phase chemical kinetics of fuel pyrolysis and oxidation. It also considers the limiting case of local chemical equilibrium. Formation of cyclic hydrocarbon species is used to indicate deposit propensity. Results show that the likelihood of deposit formation depends strongly on cell temperature, current density, and residence time. Generally speaking, equilibrium favors deposit formation early in the channel whereas, owing to limited residence time, the homogeneous finite-rate kinetics predicts relatively low levels of deposit precursors. In the downstream portions, because of electrochemical oxygen flux though the electrode-electrolyte membrane, chemical equilibrium shifts strongly away from deposit formation to volatile carbon-oxygen species. However, the homogeneous finite-rate kinetics predictions show a continuing increase in coking propensity. (C) 2003 Elsevier Science B.V. All rights reserved.