Several experimental studies have shown that, 1) the extent of the poisoning effect due to trace amounts of sulfur compounds in the fuel is lower if a SOFC is operated at a higher current density, and 2) the performance drop due to sulfur poisoning is much lower for Ni-GDC or Ni-ScSZ anodes when compared to Ni-YSZ anodes. This work presents a first principles numerical model that simulates experimental studies of sulfur poisoning on SOFC button cells. The exchange current densities for the electrodes are determined using sulfur-free polarization data for cells fueled by humidified mixtures of H 2 and N 2 . A detailed surface reaction model that predicts the fractional coverage of all adsorbed species at the three phase interface is coupled to the SOFC model and the sulfur coverage is used to alter the anode exchange current density. The resulting model predictions match experimental observations during both galvanostatic and potentiostatic operation. Our analysis shows that the observed lower performance drop at higher current density is due to the non-linear nature of the electrochemical rate equations, and that the lower impact of sulfur poisoning on Ni-GDC and Ni-ScSZ anodes (compared to Ni-YSZ anodes) is due to their higher electrochemical activity. Solid oxide fuel cell (SOFC) systems operating on natural gas or gasified coal can be significantly more energy efficient than today's combustion systems and can thus reduce CO 2 emissions. However, a major problem associated with the use of hydrocarbon fuels is the presence of sulfur containing compounds that are converted to H 2 S under SOFC operating conditions.1 The H 2 S present in the feed gas can readily deactivate conventional Ni cermet anodes. One can certainly have a desulfurization unit before the fuel cell stack to deal with the sulfur poisoning. However, this leads to increased system complexity and decrease in overall efficiency. Nevertheless, it is important to understand and quantify the sulfur tolerance of SOFC anodes in the event of sulfur breakthrough from the desulfurizer. Sulfur poisoning of Ni-YSZ anodes in SOFC is well studied experimentally for model fuel compositions consisting of ppm levels of H 2 S in mixtures of H 2 , H 2 O and an inert 2-4 as well as H 2 S in gas mixtures representative of natural gas or reformed natural gas.5-8 Most of the experimental literature deals with H 2 S concentrations well below 10 ppm and work that treats H 2 S concentrations higher than 20 ppm is rather limited. 2,5,8 On the other hand it is well known that natural gas and biogas can have substantially higher sulfur concentrations and that catalytic steam reforming of methane can be carried out on Ni even with 100 ppm H 2 S without losing all catalytic activity 9,10 e.g., a methane conversion (in model biogas) of ∼35% can be maintained using a supported Ni catalyst with 100 ppm H 2 S at 800• C.
10For an electrolyte supported cell Zha et al., 2 studied the cell performance for a wide range of H 2 S concentrations using DC polarization and electrochemical i...