Enhanced carbon tolerance on Ni-based reforming catalyst with Ir alloying: A DFT study

Abstract

Carbon deposition is a major cause of performance degradation for the Ni-based catalyst used in steam reforming of hydrocarbons. In this work, we perform first principle calculations to show that carbon tolerance behavior can be significantly enhanced by alloying Ni with Ir. The most stable atomic structure predicted by the surface phased diagram shows that Ir atoms prefer to stay on the surface of the alloy ensuring their exposure to the incoming gas. We find that the presence of Ir atoms suppress the surface migration of carbon atoms and weaken the stability of the adsorbed carbon agglomerates. Finally, we elucidate that the local reactivity change caused by the shift in the d-band structure is responsible for such good carbon tolerance behavior.