Understanding structure-activity relationships in highly active La promoted Ni catalysts for CO2 methanation

Ni-based catalysts are selective in the hydrogenation of CO2 to CH4 but their activity and stability need improvement. Herein, we propose a hydrotalcite-derived high loaded Ni-Al2O3 catalyst promoted by La. The effect of La on the catalyst properties is investigated and compared with that of Y and Ce. The NiOx crystallite size and basic properties (rather than the nickel reducibility) as well as the catalytic activity depend on the rare-earth element. The La-catalyst achieves a more relevant activity enhancement at low temperature and high space velocity (480 L g(-1) h(-1), CO2/H-2/N-2 = 1/4/1 v/v), high CH4 productivity (101 LCH4 gNi(-1) h(-1)) and stability, even under undiluted feeds. In situ DRIFTS and the characterization of spent catalysts confirm that this enhanced performance is related to the combination of dissociative and associative CO2 activation on more reduced, highly dispersed and stable Ni nanoparticles and basic sites in the La2O3-Al2O3 matrix, respectively.