Density functional theory study for the enhanced sulfur tolerance of Ni catalysts by surface alloying

Sulfur compounds in fuels deactivate the surface of anode materials in solid oxide fuel cells (SOFCs), which adversely affect the long-term durability. To solve this issue, it is important to design new SOFC anode materials with high sulfur tolerance. Unfortunately, it is difficult to completely replace the traditional Ni anode owing to its outstanding reactivity with low cost. As an alternative, alloying Ni with transition metals is a practical strategy to enhance the sulfur resistance while taking advantage of Ni metal. Therefore, in this study, we examined the effects of transition metal (Cu, Rh, Pd, Ag, Pt, and Au) doping into a Ni catalyst on not only the adsorption of H ₂ S, HS, S, and H but also H ₂ S decomposition using density functional theory (DFT) calculations. The dopant metals were selected rationally by considering the stability of the Ni-based binary alloys. The interactions between sulfur atoms produced by H ₂ S dissociation and the surface are weakened by the dopant metals at the topmost layer. In addition, the findings show that H ₂ S dissociation can be suppressed by doping transition metals. It turns out that these effects are maximized in the Au-doped Ni catalyst. Our DFT results will provide useful insights into the design of sulfur-tolerant SOFC anode materials.