Balancing free and confined metallic Ni for an active and stable catalyst—A case study of CO methanation over Ni/Ni–Al2O3

Abstract

We propose a new strategy to make an active and stable Ni-based catalyst which can be operated in a wide range of reaction temperatures. The ordered mesoporous alumina (OMA) with confined Ni in the pore wall (Ni-OMA) was prepared via the one-pot evaporation induced self-assembly method. By using the incipient impregnation method, different amounts of free Ni were loaded over Ni-OMA (Ni/Ni-OMA) at a fixed total NiO content of 15 wt%. Characterization results confirmed the formation of well-structured Ni-OMA, and the ordered structure was still well preserved even after impregnating NiO at a content of as high as 12 wt%. The catalysts were evaluated for the CO methanation as a model reaction under varied conditions. Importantly, the activity and stability of Ni/Ni-OMA for the titled reaction were significantly regulated by simply changing the ratio of the confined to free Ni. Over the optimum catalyst of NiO (2 wt%)/NiO (13 wt%)-OMA, the high activity at a temperature of as low as 300 °C was achieved with the space-time yield of methane over 7.6 g gcat−1 h−1 while a long-term stability for a time-on-stream of 400 h was confirmed without an observable deactivation under the conditions of 600 °C and an extremely high gas hourly space velocity of 120,000 mL g−1 h−1. The results were well explained as the integrated merits of the free Ni for a high dispersion and the confined Ni in OMA for the anti-sintering property.