The role of metal-support interaction for CO-free hydrogen from low temperature ethanol steam reforming on Rh-Fe catalysts

Abstract

Rh-Fe catalysts supported on Ca-Al2O3, MgO and ZrO2 were evaluated in ethanol steam reforming at 623 K and compared to Rh catalysts on the same supports without iron promotion. The metal-support interaction among the three entities, i.e. Rh ↔ Fe2O3 ← support (ZrO2, MgO and Ca-Al2O3) was investigated using H2-chemisorption, TEM, XPS and in situ techniques such as DRIFTS, temperature-resolved XRD and XAS. As compared to the unpromoted Rh catalysts on the same supports, the CO selectivity is depressed in the presence of iron on Rh/MgO and Rh/Ca-Al2O3, the latter being significantly superior. The role of metal-support interaction for CO-free hydrogen generation was unravelled using a combination of techniques. It was found that the reducibility of iron oxide determines the extent of the strong metal support interaction between Rh and Fe2O3 and the reducibility of iron oxide was affected by the support. On Rh-Fe/Ca-Al2O3, a good balance of the interaction between Rh, Fe2O3 and Ca-Al2O3 prevents strong metal support interaction between Rh and Fe2O3 and thus promotes CO elimination via water-gas-shift reaction on Rh-FexOy sites.