Reforming of hydrocarbon fuels is one of the most important heterogeneous catalytic processes. Particularly appealing is potential development of catalysts that could be used as direct, reforming anodes in solid oxide fuel cells (SOFCs). Current reforming catalysts such as Ni, however, suffer from two major problems: (i) carbon-induced deactivation and (ii) sulfur poisoning of the catalyst. We have utilized Density Functional Theory (DFT) calculations to study the surface chemistry of carbon atoms and carbon fragments on Ni. These studies demonstrated that there is a strong thermodynamic driving force to form sp2-bonded carbon networks. These extended carbon networks diminish the reforming activity of Ni. We have further utilized DFT to search for Ni-containing alloys that are more carbon-tolerant than monometallic Ni, i.e., that have a lower propensity to form the carbon networks. These studies have yielded a few promising alloy formulations. Subsequent steady-state reactor studies validated the predictions of the DFT calculations. Aside from the steady-state reactor tests, the catalysts were characterized with multiple spectroscopic and microscopic tools.

1. E.Nikolla, A. Holewinski, J. Schwank, S. Linic; “Controlling Carbon Surface Chemistry by Alloying: Carbon Tolerant Reforming Catalyst”, Journal of the American Chemical Society, 2006; 128(35); 11354-11355.